TY - JOUR A1 - Abad Andrade, Carlos Enrique A1 - Jegielka, Dennis A1 - Aloysius, Allen A1 - Recknagel, Sebastian T1 - SI-traceable total analysis of nitrate and nitrite by isotope dilution optical spectroscopy and its application to Berlin surface waters N2 - Accurate nitrate and nitrite data support water-quality regulation, yet routine methods rely on external calibration and rarely achieve SI traceability. We report a calibration-free determination of nitrate and nitrite by combining isotope dilution with high-resolution continuum-source graphite furnace molecular absorption spectrometry (ID-HR-CS-GF-MAS). A 15N-enriched nitrate spike (its concentration verified by reverse isotope dilution against the standard reference material NIST 3185) provides the SI link, and it is gravimetrically added to samples; nitrate and residual nitrite are converted in situ to nitric oxide (NO), whose 215 nm band is recorded at a pixel resolution of λ/Δλ ≈ 140 000. The 0.2127 nm shift between 14NO and 15NO electronic spectra is resolved, and a three-latent-variable partial least squares regression model yields the 15N/14N ratio with 0.3% precision. Instrumental LoD values of 4.8 ng (14N) and 3.2 ng (15N) translate to a method LoD of 4.8 ng of nitrogen (equivalent to 1.05 mg L−1 NO3− for a 20 μL aliquot). The furnace program allows for successive drying/pyrolysis loops, so additional 20 μL aliquots can be layered onto the graphite platform. Alternatively, a 10 mL anion-exchange solid-phase extraction step concentrates nitrate and nitrite fivefold, allowing for the analysis of even lower sample concentrations. Results for four certified reference materials (2.9 to 1000 mg L−1 NO3−) agreed with certified values, giving relative expanded uncertainties of 2 to 4%. Analysis of twenty Berlin surface-water samples revealed concentrations ranging from 0.10 to 7.3 mg L−1 NO3−, indicating that the Panke River and Teltow Canal are the primary sources of nitrogen. ID-HR-CS-GF-MAS thus delivers ID-MS-level accuracy in a few minutes per run with bench-top optics, and, with optional on-platform or SPE pre-concentration, extends SI-traceable nitrate/nitrite monitoring into the low-ng regime. KW - Isotope dilution KW - Nitrate and nitrite determination KW - SI-traceable quantification KW - Calibration-free analysis KW - Water quality KW - Berlin surface waters KW - NO molecular absorption bands PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-643785 DO - https://doi.org/10.1039/D5JA00252D SN - 0267-9477 VL - 40 IS - 10 SP - 2692 EP - 2701 PB - Royal Society of Chemistry (RSC) AN - OPUS4-64378 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Abad Andrade, Carlos Enrique A1 - Mimus, S. A1 - Recknagel, Sebastian A1 - Jakubowski, N. A1 - Panne, Ulrich A1 - Becker-Ross, H. A1 - Huang, M.-D. T1 - Determination of organic chlorine in water via AlCl derivatization and detection by high-resolution continuum source graphite furnace molecular absorption spectrometry N2 - High-resolution continuum source graphite furnace molecular absorption spectrometry (HR-CS-GF-MAS) was employed for determining adsorbable organic chlorine (AOCl) in water. Organic chlorine was indirectly quantified by monitoring the molecular absorption of the transient aluminum monochloride molecule (AlCl) around a wavelength of 261.42 nm in a graphite furnace. An aluminum solution was used as the molecularforming modifier. A zirconium coated graphite furnace, as well as Sr and Ag solutions were applied as modifiers for a maximal enhancement of the absorption signal. The pyrolysis and vaporization temperatures were 600 °C and 2300 °C, respectively. Non-spectral interferences were observed with F, Br, and I at concentrations higher than 6 mg L-1, 50 mg L-1, and 100 mg L-1, respectively. Calibration curves with NaCl, 4-chlorophenol, and trichlorophenol present the same slope and dynamic range, which indicates the chlorine atom specificity of the method. This method was evaluated and validated using synthetic water samples, following the current standard DIN EN ISO 9562:2004 for the determination of the sum parameter adsorbable organic halides (AOX) for water quality. These samples contain 4-chlorophenol as the chlorinated organic standard in an inorganic chloride matrix. Prior to analysis, organic chlorine was extracted from the inorganic matrix via solid-phase extraction with a recovery rate >95%. There were no statistically significant differences observed between measured and known values and for a t-test a confidence level of 95% was achieved. The limits of detection and characteristic mass were found to be 48 and 22 pg, respectively. The calibration curve was linear in the range 0.1–2.5 ng with a correlation coefficient R2 = 0.9986. KW - Chlorides KW - Chlorine KW - Graphite furnace KW - Spectrometry KW - Diatomic molecule KW - Water KW - AlCl PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-534426 DO - https://doi.org/10.1039/D1AY00430A SN - 1759-9660 VL - 13 IS - 33 SP - 3724 EP - 3730 PB - The Royal Society of Chemistry CY - London, UK AN - OPUS4-53442 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Abram, Sarah-Luise A1 - Tavernaro, Isabella A1 - Resch-Genger, Ute A1 - Johnston, L. J. A1 - Zou, S. T1 - Nanoscale reference and test materials for the validation of characterization methods for engineered nanomaterials — current state, limitations, and needs N2 - The rational design of engineered nanomaterials (NMs) with improved functionality and their increasing industrial application requires reliable, validated, and ultimately standardized characterization methods for their application-relevant, physicochemical key properties such as size, size distribution, shape, or surface chemistry. This calls for nanoscale (certified) reference materials (CRMs; RMs) and well-characterized reference test materials (RTMs) termed also quality control (QC) samples, assessed, e.g., in interlaboratory comparisons, for the validation and standardization of commonly used characterization methods. Thereby, increasing concerns regarding potential risks of NMs are also addressed and the road for safe and sustainable-by-design concepts for the development of new functional NMs and their use as nanomedicines is paved. With this respect, we will provide an overview of relevant international standardization and regulatory activities, definitions, and recommendations on characterization methods and review currently available organic or inorganic nanoscale CRMs, RMs, and RTMs, including their characterization or certification. In addition, we will highlight typical applications to streamline the regulatory approval process and improve manufacturability including the special challenges imposed by the colloidal nature and sometimes limited stability of NMs. Subsequently, we will critically assess the limitations of currently available nanoscale RMs and RTMs and address the gaps to be filled in the future such as the availability of NMs that come with reference data on properties other than commonly addressed particle size, such as surface chemistry or particle number concentration, or more closely resemble commercially available formulations or address application-relevant matrices. KW - Nano KW - Particle KW - Silica KW - Quality assurance KW - Reference material KW - Review KW - Surface chemistry KW - Size KW - Shape KW - Particle number concentration KW - Lipid nanoparticles KW - Metal nanoparticles KW - Liposomes PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-625746 DO - https://doi.org/10.1007/s00216-024-05719-6 SN - 1618-2650 SP - 1 EP - 21 PB - Springer AN - OPUS4-62574 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Adams, L. C. A1 - Brangsch, J. A1 - Kaufmann, Jan Ole A1 - Mangarova, D. B. A1 - Moeckel, J. A1 - Kader, A. A1 - Buchholz, R. A1 - Karst, U. A1 - Botnar, R. M. A1 - Hamm, B. A1 - Makowski, M. R. A1 - Keller, S. T1 - Effect of Doxycycline on Survival in Abdominal Aortic Aneurysms in a Mouse Model N2 - Background. Currently, there is no reliable nonsurgical treatment for abdominal aortic aneurysm (AAA). This study, therefore, investigates if doxycycline reduces AAA growth and the number of rupture-related deaths in a murine ApoE−/− model of AAA and whether gadofosveset trisodium-based MRI differs between animals with and without doxycycline treatment. Methods. Nine ApoE−/− mice were implanted with osmotic minipumps continuously releasing angiotensin II and treated with doxycycline (30 mg/kg/d) in parallel. After four weeks, MRI was performed at 3T with a clinical dose of the albumin-binding probe gadofosveset (0.03 mmol/kg). Results were compared with previously published wild-type control animals and with previously studied ApoE−/− animals without doxycycline treatment. Differences in mortality were also investigated between these groups. Results. In a previous study, we found that approximately 25% of angiotensin II-infused ApoE−/− mice died, whereas in the present study, only one out of 9 angiotensin II-infused and doxycycline-treated ApoE−/− mice (11.1%) died within 4 weeks. Furthermore, doxycycline-treated ApoE−/− mice showed significantly lower contrast-to-noise (CNR) values in MRI compared to ApoE−/− mice without doxycycline treatment. In vivo measurements of relative signal enhancement (CNR) correlated significantly with ex vivo measurements of albumin staining (R2 = 0.58). In addition, a strong visual colocalization of albumin-positive areas in the fluorescence albumin staining with gadolinium distribution in LA-ICP-MS was shown. However, no significant difference in aneurysm size was observed after doxycycline treatment. Conclusion. The present experimental in vivo study suggests that doxycycline treatment may reduce rupture-related deaths in AAA by slowing endothelial damage without reversing aneurysm growth. KW - Ggadolinium KW - MRI KW - Magnetic resonance imaging KW - Osmotic minipumps KW - Tetracyclin KW - Antibiotics KW - Angiotensin II KW - LA-ICP-MS PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-527015 DO - https://doi.org/10.1155/2021/9999847 SP - 9999847 PB - Hindawi CY - London AN - OPUS4-52701 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Adams, L. C. A1 - Brangsch, J. A1 - Reimann, C. A1 - Kaufmann, Jan Ole A1 - Buchholz, R. A1 - Karst, U. A1 - Botnar, R. M. A1 - Hamm, B. A1 - Makowski, M. R. T1 - Simultaneous molecular MRI of extracellular matrix collagen and inflammatory activity to predict abdominal aortic aneurysm rupture N2 - Abdominal aortic aneurysm (AAA) is a life-threatening vascular disease with an up to 80% mortality in case of rupture. Current biomarkers fail to account for size-independent risk of rupture. By combining the information of different molecular probes, multi-target molecular MRI holds the potential to enable individual characterization of AAA. In this experimental study, we aimed to examine the feasibility of simultaneous imaging of extracellular collagen and inflammation for size-independent prediction of risk of rupture in murine AAA. The study design consisted of: (1) A outcome-based longitudinal study with imaging performed once after one week with follow-up and death as the end-point for assessment of rupture risk. (2) A week-by-week study for the characterization of AAA development with imaging after 1, 2, 3 and 4 weeks. For both studies, the animals were administered a type 1 collagen-targeted gadolinium-based probe (surrogate marker for extracellular matrix (ECM) remodeling) and an iron oxide-based probe (surrogate marker for inflammatory activity), in one imaging session. In vivo measurements of collagen and iron oxide probes showed a significant correlation with ex vivo histology (p < 0.001) and also corresponded well to inductively-coupled plasma-mass spectrometry and laser-ablation inductively-coupled plasma mass spectrometry. Combined evaluation of collagen-related ECM remodeling and inflammatory activity was the most accurate predictor for AAA rupture (sensitivity 80%, specificity 100%, area under the curve 0.85), being superior to information from the individual probes alone. Our study supports the feasibility of a simultaneous assessment of collagen-related extracellular matrix remodeling and inflammatory activity in a murine model of AAA. KW - Atherosclerosis KW - Specific probe KW - Magnetic resonance imaging KW - Gadolinium KW - Iron oxide KW - Ferumoxytol KW - Inductively‑coupled mass spectrometry KW - ICP-MS KW - LA-ICP-MS KW - Laser ablation PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-525864 UR - https://www.nature.com/articles/s41598-020-71817-x DO - https://doi.org/10.1038/s41598-020-71817-x VL - 10 IS - 1 SP - 15206 PB - Springer Nature Limited CY - London, New York, Berlin, Shanghai and Tokyo AN - OPUS4-52586 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Adams, L. C. A1 - Brangsch, J. A1 - Reimann, C. A1 - Kaufmann, Jan Ole A1 - Nowak, K. A1 - Buchholz, R. A1 - Karst, U. A1 - Botnar, R. M. A1 - Hamm, B. A1 - Makowski, M. R. T1 - Noninvasive imaging of vascular permeability to predict the risk of rupture in abdominal aortic aneurysms using an albumin binding probe N2 - Abdominal aortic aneurysm (AAA) remains a fatal disease. Its development encompasses a complex interplay between hemodynamic stimuli on and changes in the arterial wall. Currently available biomarkers fail to predict the risk of AAA rupture independent of aneurysm size. Therefore, novel biomarkers for AAA characterization are needed. In this study, we used a mouse model of AAA to investigate the potential of magnetic resonance imaging (MRI) with an albumin-binding probe to assess changes in vascular permeability at different stages of aneurysm growth. Two imaging studies were performed: a longitudinal study with follow-up and death as endpoint to predict rupture risk and a week-by-week study to characterize AAA development. AAAs, which eventually ruptured, demonstrated a significantly higher in vivo MR signal enhancement from the albumin-binding probe (p = 0.047) and a smaller non-enhancing thrombus area compared to intact AAAs (p = 0.001). The ratio of albumin-binding-probe enhancement of the aneurysm wall to size of non-enhancing-thrombus-area predicted AAA rupture with high sensitivity/specificity (100%/86%). More advanced aneurysms with higher vascular permeability demonstrated an increased uptake of the albumin-binding-probe. These results indicate that MRI with an albumin-binding probe may enable noninvasive assessment of vascular permeability in murine AAAs and prediction of rupture risk. KW - Magnetic resonance imaging KW - Imaging KW - Tomography KW - Gadolinium KW - Contrast agent KW - Atherosclerosis KW - ICP-MS KW - Gadofosveset KW - Angiography KW - LA-ICP-MS PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-525541 DO - https://doi.org/10.1038/s41598-020-59842-2 VL - 10 SP - Article number: 3231 PB - Springer Nature Limited CY - London, New York, Berlin, Shanghai and Tokyo AN - OPUS4-52554 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Adamus, A. A1 - Ali, I. A1 - Vasileiadis, V. A1 - Al-Hileh, L. A1 - Lisec, Jan A1 - Frank, M. A1 - Seitz, G. A1 - Engel, N. T1 - Vincetoxicum arnottianum modulates motility features and metastatic marker expression in pediatric rhabdomyosarcoma by stabilizing the actin cytoskeleton N2 - Background: Prevention of metastatic invasion is one of the main challenges in the treatment of alveolar rhabdomyosarcoma. Still the therapeutic options are limited. Therefore, an anti-tumor screening was initiated focusing on the anti-metastatic and anti-invasion properties of selected medicinal plant extracts and phytoestrogens, already known to be effective in the prevention and treatment of different cancer entities. Methods: Treatment effects were first evaluated by cell viability, migration, invasion, and colony forming assays on the alveolar rhabdomyosarcoma cell line RH-30 in comparison with healthy primary cells. Results: Initial anti-tumor screenings of all substances analyzed in this study, identified the plant extract of Vincetoxicum arnottianum (VSM) as the most promising candidate, harboring the highest anti-metastatic potential. Those significant anti-motility properties were proven by a reduced ability for migration (60%), invasion (99%) and colony formation (61%) under 48 h exposure to 25 μg/ml VSM. The restricted motility features were due to an induction of the stabilization of the cytoskeleton – actin fibers were 2.5-fold longer and were spanning the entire cell. Decreased proliferation (PCNA, AMT, GCSH) and altered metastasis (e. g. SGPL1, CXCR4, stathmin) marker expression on transcript and protein level confirmed the significant lowered tumorigenicity under VSM treatment. Finally, significant alterations in the cell metabolism were detected for 25 metabolites, with levels of uracil, N-acetyl serine and propanoyl phosphate harboring the greatest alterations. Compared to the conventional therapy with cisplatin, VSM treated cells demonstrated a similar metabolic shutdown of the primary cell metabolism. Primary control cells were not affected by the VSM treatment. Conclusions: This study revealed the VSM root extract as a potential, new migrastatic drug candidate for the putative treatment of pediatric alveolar rhabdomyosarcoma with actin filament stabilizing properties and accompanied by a marginal effect on the vitality of primary cells. KW - Mass Spectroscopy KW - Metabolomics KW - Cancer PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-533530 DO - https://doi.org/10.1186/s12906-021-03299-x VL - 21 IS - 1 PB - Springer Nature AN - OPUS4-53353 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ahiboz, D. A1 - Andresen, Elina A1 - Manley, P. A1 - Resch-Genger, Ute A1 - Würth, Christian A1 - Becker, C. T1 - Metasurface-Enhanced Photon Upconversion upon 1550 nm Excitation N2 - Photon upconversion upon 1550 nm excitation is of high relevance for applications in the third biological excitation window, for photovoltaics beyond current limitations, and enables appealing options in the field of glass Fiber telecommunications. Trivalent doped erbium ions (Er3+) are the material of choice for 1550 nm excited upconversion, however, they suffer from a low absorption cross-section and a low brightness. Therefore, the ability of Silicon metasurfaces to provide greatly enhanced electrical near-fields is employed to enable efficient photon upconversion even at low external Illumination conditions. Hexagonally shaped β-NaYF4:Er3+ nanoparticles are placed on large-area silicon metasurfaces designed to convert near-infrared (1550 nm) to visible light. More than 2400-fold enhanced photon upconversion luminescence is achieved by using this metasurface instead of a planar substrate. With the aid of optical simulations based on the finite-element method, this result is attributed to the coupling of the excitation source with metasurface resonances at appropriate incident angles. Analysis of the excitation power density dependence of upconversion luminescence and red-to-green-emission ratios enables the estimation of nanoscale near-field enhancement on the metasurface. The findings permit the significant reduction of required external excitation intensities for photon upconversion of 1550 nm light, opening perspectives in biophotonics, telecommunication, and photovoltaics. KW - Nano KW - Nanomaterial KW - Upconversion nanoparticle KW - Lanthanide KW - Photoluminescence KW - Quantum yield KW - Photophysics KW - Lifetime KW - Sensor KW - Excitation power density KW - Single particle KW - Brightness KW - NIR KW - Mechanism KW - Single enhancement KW - SWIR KW - Method PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-537193 DO - https://doi.org/10.1002/adom.202101285. SN - 2195-1071 VL - 9 IS - 24 SP - 2101285 PB - Wiley-VCH-GmbH AN - OPUS4-53719 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ahmed, A. A. A. A1 - Alegret, N. A1 - Almeida, B. A1 - Alvarez-Puebla, R. A1 - Andrews, A. M. A1 - Ballerini, L. A1 - Barrios-Capuchino, J. J. A1 - Becker, C. A1 - Blick, R. H. A1 - Bonakdar, S. A1 - Chakraborty, I. A1 - Chen, X. A1 - Cheon, J. A1 - Chilla, G. A1 - Conceicao, A. L. C. A1 - Delehanty, J. A1 - Dulle, M. A1 - Efros, A. L. A1 - Epple, M. A1 - Fedyk, M. A1 - Feliu, N. A1 - Feng, M. A1 - Fernandez-Chacon, R. A1 - Fernandez-Cuesta, I. A1 - Fertig, N. A1 - Förster, S. A1 - Garrido, J. A. A1 - George, M. A1 - Guse, A. H. A1 - Hampp, N. A1 - Harberts, J. A1 - Han, J. A1 - Heekeren, H. R. A1 - Hofmann, U. G. A1 - Holzapfel, M. A1 - Hosseinkazemi, H. A1 - Huang, Y. A1 - Huber, P. A1 - Hyeon, T. A1 - Ingebrandt, S. A1 - Ienca, M. A1 - Iske, A. A1 - Kang, Y. A1 - Kasieczka, G. A1 - Kim, D.-H. A1 - Kostarelos, K. A1 - Lee, J.-H. A1 - Lin, K.-W. A1 - Liu, S. A1 - Liu, X. A1 - Liu, Y. A1 - Lohr, C. A1 - Mailänder, V. A1 - Maffongelli, L. A1 - Megahed, S. A1 - Mews, A. A1 - Mutas, M. A1 - Nack, L. A1 - Nakatsuka, N. A1 - Oertner, T. G. A1 - Offenhäusser, A. A1 - Oheim, M. A1 - Otange, B. A1 - Otto, F. A1 - Patrono, E. A1 - Peng, B. A1 - Picchiotti, A. A1 - Pierini, F. A1 - Pötter-Nerger, M. A1 - Pozzi, M. A1 - Pralle, A. A1 - Prato, M. A1 - Qi, B. A1 - Ramos-Cabrer, P. A1 - Resch-Genger, Ute A1 - Ritter, N. A1 - Rittner, M. A1 - Roy, S. A1 - Santoro, F. A1 - Schuck, N. W. A1 - Schulz, F. A1 - Seker, E. A1 - Skiba, M. A1 - Sosniok, M. A1 - Stephan, H. A1 - Wang, R. A1 - Wang, T. A1 - Wegner, Karl David A1 - Weiss, P. S. A1 - Xu, M. A1 - Yang, C. A1 - Zargarin, S. S. A1 - Zeng, Y. A1 - Zhou, Y. A1 - Zhu, D. A1 - Zierold, R. A1 - Parak, W. J. T1 - Interfacing with the Brain: How Nanotechnology Can Contribute N2 - Interfacing artificial devices with the human brain is the central goal of neurotechnology. Yet, our imaginations are often limited by currently available paradigms and technologies. Suggestions for brain−machine interfaces have changed over time, along with the available technology. Mechanical levers and cable winches were used to move parts of the brain during the mechanical age. Sophisticated electronic wiring and remote control have arisen during the electronic age, ultimately leading to plug-and-play computer interfaces. Nonetheless, our brains are so complex that these visions, until recently, largely remained unreachable dreams. The general problem, thus far, is that most of our technology is mechanically and/or electrically engineered, whereas the brain is a living, dynamic entity. As a result, these worlds are difficult to interface with one another. Nanotechnology, which encompasses engineered solid-state objects and integrated circuits, excels at small length scales of single to a few hundred nanometers and, thus, matches the sizes of biomolecules, biomolecular assemblies, and parts of cells. Consequently, we envision nanomaterials and nanotools as opportunities to interface with the brain in alternative ways. Here, we review the existing literature on the use of nanotechnology in brain−machine interfaces and look forward in discussing perspectives and limitations based on the authors’ expertise across a range of complementary disciplines from neuroscience, engineering, physics, and chemistry to biology and medicine, computer science and mathematics, and social science and jurisprudence. We focus on nanotechnology but also include information from related fields when useful and complementary. KW - Nanoneuro interface KW - Brain-on-a-chip KW - Nanostructured interface KW - Electrode arrays KW - Neuro-implants KW - Advanced nanomaterials KW - Quality assurance PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-634893 DO - https://doi.org/10.1021/acsnano.4c10525 SN - 1936-086X VL - 19 IS - 11 SP - 10630 EP - 10717 PB - ACS Publications AN - OPUS4-63489 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Anderhalten, L. A1 - Silva, R. V. A1 - Morr, A. A1 - Wang, S. A1 - Smorodchenko, A. A1 - Saatz, Jessica A1 - Traub, Heike A1 - Mueller, S. A1 - Boehm-Sturm, P. A1 - Rodriguez-Sillke, Y. A1 - Kunkel, D. A1 - Hahndorf, J. A1 - Paul, F. A1 - Taupitz, M. A1 - Sack, I. A1 - Infante-Duarte, C. T1 - Different Impact of Gadopentetate and Gadobutrol on Inflammation-Promoted Retention and Toxicity of Gadolinium Within the Mouse Brain N2 - Objectives: Using a murine model of multiple sclerosis, we previously showed that repeated administration of gadopentetate dimeglumine led to retention of gadolinium (Gd) within cerebellar structures and that this process was enhanced with inflammation. This study aimed to compare the kinetics and retention profiles of Gd in inflamed and healthy brains after application of the macrocyclic Gd-based contrast agent (GBCA) gadobutrol or the linear GBCA gadopentetate. Moreover, potential Gd-induced neurotoxicity was investigated in living hippocampal slices ex vivo. Materials and Methods: Mice at peak of experimental autoimmune encephalomyelitis (EAE; n = 29) and healthy control mice (HC; n = 24) were exposed to a cumulative dose of 20 mmol/kg bodyweight of either gadopentetate dimeglumine or gadobutrol (8 injections of 2.5 mmol/kg over 10 days). Magnetic resonance imaging (7 T) was performed at baseline as well as at day 1, 10, and 40 post final injection (pfi) of GBCAs. Mice were sacrificed after magnetic resonance imaging and brain and blood Gd content was assessed by laser ablation-inductively coupled plasma (ICP)-mass spectrometry (MS) and ICP-MS, respectively. In addition, using chronic organotypic hippocampal slice cultures, Gd-induced neurotoxicity was addressed in living brain tissue ex vivo, both under control or inflammatory (tumor necrosis factor α [TNF-α] at 50 ng/μL) conditions. Results: Neuroinflammation promoted a significant decrease in T1 relaxation times after multiple injections of both GBCAs as shown by quantitative T1 mapping of EAE brains compared with HC. This corresponded to higher Gd retention within the EAE brains at 1, 10, and 40 days pfi as determined by laser ablation-ICP-MS. In inflamed cerebellum, in particular in the deep cerebellar nuclei (CN), elevated Gd retention was observed until day 40 after last gadopentetate application (CN: EAE vs HC, 55.06 ± 0.16 μM vs 30.44 ± 4.43 μM). In contrast, gadobutrol application led to a rather diffuse Gd content in the inflamed brains, which strongly diminished until day 40 (CN: EAE vs HC, 0.38 ± 0.08 μM vs 0.17 ± 0.03 μM). The analysis of cytotoxic effects of both GBCAs using living brain tissue revealed an elevated cell death rate after incubation with gadopentetate but not gadobutrol at 50 mM. The cytotoxic effect due to gadopentetate increased in the presence of the inflammatory mediator TNF-α (with vs without TNF-α, 3.15% ± 1.18% vs 2.17% ± 1.14%; P = 0.0345). Conclusions: In the EAE model, neuroinflammation promoted increased Gd retention in the brain for both GBCAs. Whereas in the inflamed brains, efficient clearance of macrocyclic gadobutrol during the investigated time period was observed, the Gd retention after application of linear gadopentetate persisted over the entire observational period. Gadopentetate but not gadubutrol appeared to be neurotoxic in an ex vivo paradigm of neuronal inflammation. KW - Imaging KW - ICP-MS KW - Gadolinium KW - Contrast agent KW - Laser ablation KW - Brain KW - Multiple sclerosis PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-546910 DO - https://doi.org/10.1097/RLI.0000000000000884 SN - 0020-9996/22/0000–0000 VL - 57 IS - 10 SP - 677 EP - 688 PB - Wolters Kluwer N.V. CY - Alphen aan den Rijn, The Netherlands AN - OPUS4-54691 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Andresen, Elina A1 - Islam, Fahima A1 - Prinz, Carsten A1 - Gehrmann, P. A1 - Licha, K. A1 - Roik, Janina A1 - Recknagel, Sebastian A1 - Resch-Genger, Ute T1 - Assessing the reproducibility and up‑scaling of the synthesis of Er,Yb‑doped NaYF4‑based upconverting nanoparticles and control of size, morphology, and optical properties N2 - Lanthanide-based, spectrally shifting, and multi-color luminescent upconverting nanoparticles (UCNPs) have received much attention in the last decades because of their applicability as reporter for bioimaging, super-resolution microscopy, and sensing as well as barcoding and anti-counterfeiting tags. A prerequisite for the broad application of UCNPs in areas such as sensing and encoding are simple, robust, and easily upscalable synthesis protocols that yield large quantities of UCNPs with sizes of 20 nm or more with precisely controlled and tunable physicochemical properties from lowcost reagents with a high reproducibility. In this context, we studied the reproducibility, robustness, and upscalability of the synthesis of β-NaYF4:Yb, Er UCNPs via thermal decomposition. Reaction parameters included solvent, precursor chemical compositions, ratio, and concentration. The resulting UCNPs were then examined regarding their application-relevant physicochemical properties such as size, size distribution, morphology, crystal phase, chemical composition, and photoluminescence. Based on these screening studies, we propose a small volume and high-concentration synthesis approach that can provide UCNPs with different, yet controlled size, an excellent phase purity and tunable morphology in batch sizes of up to at least 5 g which are well suited for the fabrication of sensors, printable barcodes or authentication and recycling tags. KW - Photoluminescence KW - Nano KW - Nanomaterial KW - Synthesis KW - Reproducibility KW - Upconversion nanoparticle KW - Lanthanide PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-570170 DO - https://doi.org/10.1038/s41598-023-28875-8 SN - 2045-2322 VL - 13 IS - 1 SP - 1 EP - 13 AN - OPUS4-57017 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Andresen, Elina A1 - Radunz, Sebastian A1 - Resch-Genger, Ute T1 - Novel PET-Operated Rosamine Sensor Dyes with Substitution Pattern-Tunable pKa Values and Temperature Sensitivity N2 - We present the synthesis and characterization of a family of regioisomerically pure pH-sensitive rosamine fluorophores consisting of xanthene fluorophore cores, which determine the dyes’ photophysical properties such as excitation/emission wavelength, fluorescence quantum yield, and fluorescence lifetime, and differently substituted phenol moieties. The hydroxyl substituent of the phenol moiety introduces a pH sensitivity of the dyes’ fluorescence exploiting a photoinduced electron transfer (PET), that leads to a protonation-induced switching ON of the rosamine emission. Rational tuning of the pKa value of the rosamine fluorescence between 4 to 9 is achieved by altering the substitution pattern and degree of bromination of the phenolic subunits. Additionally, a temperature sensitivity of the fluorescence quantum yield is introduced or suppressed based upon the degree of rigidity of the xanthene scaffold. KW - Fluorescence KW - Optical probe KW - Sensor KW - Dye KW - Rosamine KW - Synthesis KW - Photophysics KW - PH KW - Quantum yield KW - Quality assurancemechanism KW - temperature PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-530562 DO - https://doi.org/10.1039/d1nj02505h VL - 45 IS - 31 SP - 13934 EP - 13940 PB - Royal Society of Chemistry AN - OPUS4-53056 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Auxillos, J. A1 - Crouigneau, R. A1 - Li, Y.-F. A1 - Dai, Y. A1 - Stigliani, A. A1 - Tavernaro, Isabella A1 - Resch-Genger, Ute A1 - Sandelin, A. A1 - Marie, R. A1 - Pedersen, S. F. T1 - Spatially resolved analysis of microenvironmental gradient impact on cancer cell phenotypes N2 - Despite the physiological and pathophysiological significance of microenvironmental gradients, e.g., for diseases such as cancer, tools for generating such gradients and analyzing their impact are lacking. Here, we present an integrated microfluidic-based workflow that mimics extracellular pH gradients characteristic of solid tumors while enabling high-resolution live imaging of, e.g., cell motility and chemotaxis, and preserving the capacity to capture the spatial transcriptome. Our microfluidic device generates a pH gradient that can be rapidly controlled to mimic spatiotemporal microenvironmental changes over cancer cells embedded in a 3D matrix. The device can be reopened allowing immunofluorescence analysis of selected phenotypes, as well as the transfer of cells and matrix to a Visium slide for spatially resolved analysis of transcriptional changes across the pH gradient. This workflow is easily adaptable to other gradients and multiple cell types and can therefore prove invaluable for integrated analysis of roles of microenvironmental gradients in biology. KW - Bioimaging KW - Fluorescence KW - Cell KW - Cancer KW - Method KW - Microfluids KW - Model KW - Calibration KW - Sensor KW - Ph KW - Probe KW - Workflow PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-604631 DO - https://doi.org/10.1126/sciadv.adn3448 VL - 19 IS - 18 SP - 1 EP - 17 AN - OPUS4-60463 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Azimzada, Agil A1 - Meermann, Björn T1 - AF4/ICP-ToF-MS for the investigation of species-specific adsorption of organometallic contaminants on natural colloidal particles N2 - Organotin (OT) compounds, while crucial in many industrial applications, pose substantial risks to the environment and human health. The toxicity and environmental behaviour of OTs depend on their chemical form, i.e., the type and number of organic substituents. Each species thus exhibits distinct toxicity profiles and varying binding affinities to environmental colloids, which influence their mobility, bioavailability, and environmental impacts. To date, however, most studies addressed speciation and colloidal characterization separately, leaving the combined determinations of organometallics along with their carrier colloids largely elusive. Here, we develop and validate an on-line measurement system to quantify the adsorption dynamics of 10 OT species on natural colloidal particles (<500 nm). The approach integrates a versatile fractionation technique (AF4), with a state-of-the-art multi-element analyzer (ICP-ToF-MS), achieving Sn detection limits as low as 6.0 ng/L. The method separates colloid-free OT species from those bound to colloids and enables the determination of OT interactions with distinct colloidal fractions. Validated in both fractionation and detection, the method provides reliable data that could elucidate the species-specific and temporal aspects of species-colloids adsorption processes. The results feature comparative studies of 10 OT species, offering critical insights into OT mobility and distribution in environmental systems. KW - Fractionation KW - Speciation KW - Adsorption KW - Colloids KW - Organotin KW - AF4 KW - Nanoparticle characterization PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-625244 DO - https://doi.org/10.1016/j.jhazmat.2025.137320 SN - 1873-3336 VL - 488 SP - 1 EP - 11 PB - Elsevier B.V. AN - OPUS4-62524 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Backes, A. T. A1 - Reinmuth-Selzle, K. A1 - Leifke, A. L. A1 - Ziegler, K. A1 - Krevert, C. S. A1 - Tscheuschner, Georg A1 - Lucas, K. A1 - Weller, Michael G. A1 - Berkemeier, T. A1 - Pöschl, U. A1 - Fröhlich-Nowoisky, J. T1 - Oligomerization and Nitration of the Grass Pollen Allergen Phl p 5 by Ozone, Nitrogen Dioxide, and Peroxynitrite: Reaction Products, Kinetics, and Health Effects N2 - The allergenic and inflammatory potential of proteins can be enhanced by chemical modification upon exposure to atmospheric or physiological oxidants. The molecular mechanisms and kinetics of such modifications, however, have not yet been fully resolved. We investigated the oligomerization and nitration of the grass pollen allergen Phl p 5 by ozone (O3), nitrogen dioxide (NO2), and peroxynitrite (ONOO–). Within several hours of exposure to atmospherically relevant concentration levels of O3 and NO2, up to 50% of Phl p 5 were converted into protein oligomers, likely by formation of dityrosine cross-links. Assuming that tyrosine residues are the preferential site of nitration, up to 10% of the 12 tyrosine residues per protein monomer were nitrated. For the reaction with peroxynitrite, the largest oligomer mass fractions (up to 50%) were found for equimolar concentrations of peroxynitrite over tyrosine residues. With excess peroxynitrite, the nitration degrees increased up to 40% whereas the oligomer mass fractions decreased to 20%. Our results suggest that protein oligomerization and nitration are competing processes, which is consistent with a two-step mechanism involving a reactive oxygen intermediate (ROI), as observed for other proteins. The modified proteins can promote pro-inflammatory cellular signaling that may contribute to chronic inflammation and allergies in response to air pollution. KW - Protein KW - Nitrotyrosine KW - Dityrosine KW - Allergy KW - Hay fever KW - Diesel exhaust KW - Combustion KW - Exhaust PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-529729 DO - https://doi.org/10.3390/ijms22147616 VL - 22 IS - 14 PB - MDPI CY - Basel AN - OPUS4-52972 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Balderas-Xicohtencatl, R. A1 - Villajos Collado, José Antonio A1 - Casabán, J. A1 - Wong, D. A1 - Maiwald, Michael A1 - Hirscher, M. T1 - ZIF‑8 Pellets as a Robust Material for Hydrogen Cryo-Adsorption Tanks N2 - Cryoadsorption on the inner surface of porous materials is a promising solution for safe, fast, and reversible hydrogen storage. Within the class of highly porous metal−organic frameworks, zeolitic imidazolate frameworks (ZIFs) show high thermal, chemical, and mechanical stability. In this study, we selected ZIF-8 synthesized mechanochemically by twin-screw extrusion as powder and pellets. The hydrogen storage capacity at 77 K and up to 100 bar has been analyzed in two laboratories applying three different measurement setups showing a high reproducibility. Pelletizing ZIF-8 increases the packing density close to the corresponding value for a single crystal without loss of porosity, resulting in an improved volumetric hydrogen storage capacity close to the upper limit for a single crystal. The high volumetric uptake combined with a low and constant heat of adsorption provides ca. 31 g of usable hydrogen per liter of pellet assuming a temperature−pressure swing adsorption process between 77 K − 100 bar and 117 K − 5 bar. Cycling experiments do not indicate any degradation in storage capacity. The excellent stability during preparation, handling, and operation of ZIF-8 pellets demonstrates its potential as a robust adsorbent material for technical application in pilot- and full-scale adsorption vessel prototypes. KW - Hydrogen adsorption storage KW - Metal−organic frameworks KW - ZIF-8 KW - Cryoadsorption KW - Hydrogen Storage KW - MefHySto PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-569473 DO - https://doi.org/10.1021/acsaem.2c03719 SN - 2574-0962 SP - 1 EP - 8 PB - ACS Publications CY - Washington DC AN - OPUS4-56947 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bandow, N. A1 - Aitken, M. D. A1 - Geburtig, Anja A1 - Kalbe, Ute A1 - Piechotta, Christian A1 - Schoknecht, Ute A1 - Simon, Franz-Georg A1 - Stephan, Ina T1 - Using Environmental Simulations to Test the Release of Hazardous Substances from Polymer-Based Products: Are Realism and Pragmatism Mutually Exclusive Objectives? N2 - The potential release of hazardous substances from polymer-based products is currently in the focus of environmental policy. Environmental simulations are applied to expose such products to selected aging conditions and to investigate release processes. Commonly applied aging exposure types such as solar and UV radiation in combination with water contact, corrosive gases, and soil contact as well as expected general effects on polymers and additional ingredients of polymer-based products are described. The release of substances is based on mass-transfer processes to the material surfaces. Experimental approaches to investigate transport processes that are caused by water contact are presented. For tailoring the tests, relevant aging exposure types and release quantification methods must be combined appropriately. Several studies on the release of hazardous substances such as metals, polyaromatic hydrocarbons, flame retardants, antioxidants, and carbon nanotubes from polymers are summarized exemplarily. Differences between natural and artificial exposure tests are discussed and demonstrated for the release of flame retardants from several polymers and for biocides from paints. Requirements and limitations to apply results from short-term artificial environmental exposure tests to predict long-term environmental behavior of polymers are presented. KW - Environmental simulations KW - Polymer-based products KW - Artificial weathering KW - Degradation KW - Leaching KW - Soil contact PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-509310 DO - https://doi.org/10.3390/ma13122709 SN - 1996-1944 VL - 13 IS - 12 SP - Paper 2709, 22 PB - MDPI CY - Basel, Switzerland AN - OPUS4-50931 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bastos, V. A1 - Oskoei, P. A1 - Andresen, Elina A1 - Saleh, Maysoon I. A1 - Rühle, Bastian A1 - Resch-Genger, Ute A1 - Oliveira, H. T1 - Stability, dissolution, and cytotoxicity of NaYF4‑upconversion nanoparticles with different coatings N2 - Upconversion nanoparticles (UCNPs) have attracted considerable attention owing to their unique photophysical properties. Their utilization in biomedical applications depends on the understanding of their transformations under physiological conditions and their potential toxicity. In this study, NaYF4: Yb,Er UCNPs, widely used for luminescence and photophysical studies, were modified with a set of four different coordinatively bound surface ligands, i.e., citrate, alendronate (AA), ethylendiamine tetra(methylene phosphonate) (EDTMP), and poly(maleic anhydride-alt-1-octadecene) (PMAO), as well as silica coatings with two different thicknesses. Subsequently, the aging-induced release of fluoride ions in water and cell culture media and their cytotoxic profile to human keratinocytes were assessed in parallel to the cytotoxic evaluation of the ligands, sodium fluoride and the lanthanide ions. The cytotoxicity studies of UCNPs with different surface modifications demonstrated the good biocompatibility of EDTMP-UCNPs and PMAO-UCNPs, which is in line with the low amount of fluoride ions released from these samples. An efficient prevention of UCNP dissolution and release of cytotoxic ions, as well as low cytotoxicity was also observed for UCNPs with a sufficiently thick silica shell. Overall, our results provide new insights into the understanding of the contribution of surface chemistry to the stability, dissolution behavior, and cytotoxicity of UCNPs. Altogether, the results obtained are highly important for future applications of UCNPs in the life sciences and bioimaging studies. KW - Nano KW - Nanomaterial KW - Upconversion nanoparticle KW - Lanthanide KW - Photoluminescence KW - Quantum yield KW - Photophysics KW - Excitation power density KW - Surface chemistry KW - Coating PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-544681 DO - https://doi.org/10.1038/s41598-022-07630-5 SN - 2045-2322 VL - 12 SP - 1 EP - 13 PB - Springer Nature CY - London AN - OPUS4-54468 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bayat, Mehmet Emin A1 - Kipphardt, Heinrich A1 - Tiebe, Carlo A1 - Tuma, Dirk A1 - Engelhard, Carsten T1 - Trace-Level Ammonia–Water Interactions in Hydrogen: Challenges in Gas Purity Analysis Using Optical-Feedback Cavity-Enhanced Absorption Spectroscopy (OF-CEAS) N2 - Ammonia is a critical impurity in hydrogen fuel due to its irreversible poisoning effect on proton exchange membrane fuel cells. Therefore, international standards (e.g., ISO 14687) set a stringent threshold of 100 nmol/mol. Furthermore, with the growing potential use of ammonia as a hydrogen carrier, its accurate quantification is becoming increasingly important. However, the presence of trace humidity poses analytical challenges, as ammonia may interact with water or interfaces, thereby affecting its detectability. Therefore, the goal of this work is to enable accurate trace ammonia quantification for hydrogen purity measurements through fundamental studies of the methodological challenges. Here, low-pressure sampling (ultra)long-path Optical-Feedback Cavity-Enhanced Absorption Spectroscopy (OF-CEAS) was applied with an effective optical path length of approximately 6.17 km. We studied three average amounts of ammonia: (38.2 ± 0.8) nmol/mol, (74.8 ± 0.7) nmol/mol, and (112.1 ± 1.2) nmol/mol. Furthermore, these amounts were investigated at trace-humidity levels ranging from 0.8 to 8.5 ppmV. We observed a systematic, nonlinear, and humidity-dependent positive measurement bias of up to + (1.0 ± 0.2) nmol/mol at the maximum investigated trace-humidity volume fraction of 8.5 ppmV. This bias was not caused by spectral interference but rather by water-induced accumulation of ammonia within the optical cavity. Moreover, time-resolved measurements in the presence of trace ammonia showed that water desorption follows first-order kinetics, whereas water adsorption followed mixed-order kinetics with an apparent reaction order of 1.57 ± 0.03. Distinct hydration states of surface-bound ammonia were identified, whereas under dry conditions and with increasing amounts of ammonia, enhanced surface adhesion through intermolecular clustering was observed. In addition, the presence of ammonium species within the sorption layer was indirectly confirmed by our experiments. In conclusion, we provide a deeper insight into trace-level ammonia–water interactions and establish a framework for optimizing methodologies, particularly for (ultra)long-path optical gas measurement systems. KW - Ammonia KW - Hydrogen KW - OF-CEAS KW - Humidity KW - Surface Interactions KW - Adsorption PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-643627 DO - https://doi.org/10.1021/acsmeasuresciau.5c00105 SN - 2694-250X SP - 1 EP - 15 PB - American Chemical Society (ACS) AN - OPUS4-64362 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bayerl, C. A1 - Shahryari, M. A1 - Reiter, R. A1 - Proß, V. A1 - Lehmann, K. A1 - Kühl, A. A. A1 - Becker, Dorit A1 - Schulz, Andreas A1 - Infante Duarte, C. A1 - Taupitz, M. A1 - Geisel, D. A1 - Tzschätzsch, H. A1 - Saatz, Jessica A1 - Traub, Heike A1 - Asbach, P. T1 - Quantitative Analysis of Gadolinium Deposits in Liver Tissue of Patients After Single or Multiple Gadolinium-based Contrast Agent Application N2 - Gadolinium-based contrast agents (GBCAs) are widely used in magnetic resonance imaging. Concerns exist regarding gadolinium deposition and its potential histopathologic tissue alterations, especially after repeated administrations of linear, less stable GBCAs. This study aimed to quantify gadolinium mass fractions in liver specimens of subjects exposed to GBCAs in correlation with histopathologic features. In this study, mass fractions of gadolinium in human liver specimens from 25 subjects who underwent liver tumor resection surgery and had received GBCA (1 to 9 times over 4 years), were quantitatively analyzed using inductively coupled plasma–mass spectrometry (ICP-MS). Histomorphology was assessed based on the nonalcoholic fatty liver disease activity score (NAS). Our results suggest that after intravenous administration of GBCA, a small fraction of gadolinium is retained in the liver over a time period of at least several weeks. A relationship was observed between Gadolinium retention and the number of GBCA administrations, but not with the cumulative dose and the degree of fatty liver disease. KW - ICP-MS KW - Contrast agent KW - Gadolinium KW - Liver PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-646608 DO - https://doi.org/10.1097/RLI.0000000000001254 SN - 1536-0210 SP - 1 EP - 10 PB - Lippincott Williams & Wilkins CY - Philadelphia, Pa. AN - OPUS4-64660 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bayerlein, Bernd A1 - Hanke, T. A1 - Muth, Thilo A1 - Riedel, Jens A1 - Schilling, Markus A1 - Schweizer, C. A1 - Skrotzki, Birgit A1 - Todor, A. A1 - Moreno Torres, Benjami A1 - Unger, Jörg F. A1 - Völker, Christoph A1 - Olbricht, Jürgen T1 - A Perspective on Digital Knowledge Representation in Materials Science and Engineering N2 - The amount of data generated worldwide is constantly increasing. These data come from a wide variety of sources and systems, are processed differently, have a multitude of formats, and are stored in an untraceable and unstructured manner, predominantly in natural language in data silos. This problem can be equally applied to the heterogeneous research data from materials science and engineering. In this domain, ways and solutions are increasingly being generated to smartly link material data together with their contextual information in a uniform and well-structured manner on platforms, thus making them discoverable, retrievable, and reusable for research and industry. Ontologies play a key role in this context. They enable the sustainable representation of expert knowledge and the semantically structured filling of databases with computer-processable data triples. In this perspective article, we present the project initiative Materials-open-Laboratory (Mat-o-Lab) that aims to provide a collaborative environment for domain experts to digitize their research results and processes and make them fit for data-driven materials research and development. The overarching challenge is to generate connection points to further link data from other domains to harness the promised potential of big materials data and harvest new knowledge. KW - Data infrastructures KW - Digital representations KW - Digital workflows KW - Knowledge graphs KW - Materials informatics KW - Ontologies KW - Vocabulary providers PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-546729 DO - https://doi.org/10.1002/adem.202101176 SN - 1438-1656 SP - 1 EP - 14 PB - Wiley-VCH GmbH CY - Weinheim AN - OPUS4-54672 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Becker, Roland A1 - Heyn, L. A1 - Jung, Christian T1 - Indoor exposure to airborne polycyclic aromatic hydrocarbons: A comparison of stir bar sorptive extraction and pump sampling N2 - Stir bar sorptive extraction (SBSE) was compared with standardized pump sampling regarding the prospects to assess airborne levels of polycyclic aromatic hydrocarbons (PAHs) in indoor environments. A historic railway water tower, which will be preserved as a technical monument for museum purposes, was sampled with both approaches because the built-in insulationmaterial was suspected to release PAHs to the indoor air. The 16 PAHs on the US EPA list were quantified using gas chromatography with mass spectrometric detection in filters from pump sampling after solvent extraction and on SBSE devices after thermal desorption. SBSEwas seen to sample detectable PAHmasseswith excellent repeatability and a congener pattern largely similar to that observed with pump sampling. Congener patterns were however significantly different from that in the PAH source because release from the insulation material is largely triggered by the respective congener vapor pressures. Absolute masses in the ng range sampled by SBSE corresponded to airborne concentrations in the ng L−1 range determined by pump sampling. Principle differences between SBSE and pump sampling as well as prospects of SBSE as cost-effective and versatile complement of pump sampling are discussed. KW - Polycyclic aromatic hydrocarbons KW - Adsorption KW - Extraction KW - Indoor air PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-537427 DO - https://doi.org/10.1002/eng2.12419 VL - 3 IS - 12 SP - 1 EP - 10 PB - John Wiley & Sons Ltd. AN - OPUS4-53742 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bell, A. M. A1 - von der Au, Marcus A1 - Regnery, J. A1 - Schmid, M. A1 - Meermann, Björn A1 - Reifferscheid, G. A1 - Ternes, T. A1 - Buchinger, S. T1 - Does galvanic cathodic protection by aluminum anodes impact marine organisms? N2 - Background: Cathodic protection by sacrifcial anodes composed of aluminum-zinc-indium alloys is often applied to protect ofshore support structures of wind turbines from corrosion. Given the considerable growth of renewable energies and thus ofshore wind farms in Germany over the last decade, increasing levels of aluminum, Indium and zinc are released to the marine environment. Although these metals are ecotoxicologically well-studied, data regarding their impact on marine organisms, especially sediment-dwelling species, as well as possible ecotoxicological efects of galvanic anodes are scarce. To investigate possible ecotoxicological efects to the marine environment, the diatom Phaedactylum tricornutum, the bacterium Aliivibrio fscheri and the amphipod Corophium volutator were exposed to dissolved galvanic anodes and solutions of aluminum and zinc, respectively, in standardized laboratory tests using natural seawater. In addition to acute toxicological efects, the uptake of these elements by C. volutator was investigated. Results: The investigated anode material caused no acute toxicity to the tested bacteria and only weak but signifcant efects on algal growth. In case of the amphipods, the single elements Al and Zn showed signifcant efects only at the highest tested concentrations. Moreover, an accumulation of Al and In was observed in the crustacea species. Conclusions: Overall, the fndings of this study indicated no direct environmental impact on the tested marine organisms by the use of galvanic anodes for cathodic protection. However, the accumulation of metals in, e.g., crustaceans might enhance their trophic transfer within the marine food web. KW - Galvanic anodes KW - Metal toxicity KW - Metal uptake KW - Corophium volutator KW - Seawater PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-520769 DO - https://doi.org/10.1186/s12302-020-00441-3 VL - 32 IS - 1 SP - Article number 157 AN - OPUS4-52076 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Beslic, D. A1 - Tscheuschner, Georg A1 - Renard, B. Y. A1 - Weller, Michael G. A1 - Muth, Thilo T1 - Comprehensive evaluation of peptide de novo sequencing tools for monoclonal antibody assembly N2 - Monoclonal antibodies are biotechnologically produced proteins with various applications in research, therapeutics and diagnostics. Their ability to recognize and bind to specific molecule structures makes them essential research tools and therapeutic agents. Sequence information of antibodies is helpful for understanding antibody–antigen interactions and ensuring their affinity and specificity. De novo protein sequencing based on mass spectrometry is a valuable method to obtain the amino acid sequence of peptides and proteins without a priori knowledge. In this study, we evaluated six recently developed de novo peptide sequencing algorithms (Novor, pNovo 3, DeepNovo, SMSNet, PointNovo and Casanovo), which were not specifically designed for antibody data. We validated their ability to identify and assemble antibody sequences on three multi-enzymatic data sets. The deep learning-based tools Casanovo and PointNovo showed an increased peptide recall across different enzymes and data sets compared with spectrum-graph-based approaches. We evaluated different error types of de novo peptide sequencing tools and their performance for different numbers of missing cleavage sites, noisy spectra and peptides of various lengths. We achieved a sequence coverage of 97.69–99.53% on the light chains of three different antibody data sets using the de Bruijn assembler ALPS and the predictions from Casanovo. However, low sequence coverage and accuracy on the heavy chains demonstrate that complete de novo protein sequencing remains a challenging issue in proteomics that requires improved de novo error correction, alternative digestion strategies and hybrid approaches such as homology search to achieve high accuracy on long protein sequences. KW - De novo peptide sequencing KW - Bioinformatics KW - Benchmarking study KW - Monoclonal antibody KW - Mass spectrometry KW - Sequence coverage KW - Light chains KW - Heavy chains KW - IgG KW - Immunoglobulins KW - Error correction KW - Sequencing algorithm KW - Preprocessing KW - Missing fragmentation sites KW - Deep learning-based tools PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-570363 DO - https://doi.org/10.1093/bib/bbac542 VL - 24 IS - 1 SP - 1 EP - 12 PB - Oxford University Press AN - OPUS4-57036 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Beyer, S. A1 - Kimani, Martha Wamaitha A1 - Zhang, Y. A1 - Verhassel, A. A1 - Sternbæk, L. A1 - Wang, T. A1 - Persson, J. L. A1 - Härkönen, P. A1 - Johansson, E. A1 - Caraballo, R. A1 - Elofsson, M. A1 - Gawlitza, Kornelia A1 - Rurack, Knut A1 - Ohlsson, L. A1 - El-Schich, Z. A1 - Gjörloff Wingren, A. A1 - Stollenwerk, M. M. T1 - Fluorescent Molecularly Imprinted Polymer Layers against Sialic Acid on Silica-coated Polystyrene Cores - Assessment of the Binding Behavior to Cancer Cells N2 - Sialic acid (SA) is a monosaccharide usually linked to the terminus of glycan chains on the cell surface. It plays a crucial role in many biological processes, and hypersialylation is a common feature in cancer. Lectins are widely used to analyze the cell surface expression of SA. However, these protein molecules are usually expensive and easily denatured, which calls for the development of alternative glycan-specific receptors and cell imaging technologies. In this study, SA-imprinted fluorescent core-shell molecularly imprinted polymer particles (SA-MIPs) were employed to recognize SA on the cell surface of cancer cell lines. The SA-MIPs improved suspensibility and scattering properties compared with previously used core-shell SA-MIPs. Although SA-imprinting was performed using SA without preference for the alpha-2,3- and alpha-2,6-SA forms, we screened the cancer cell lines analyzed using the lectins Maackia Amurensis Lectin I (MAL I, alpha-2,3-SA) and Sambucus Nigra Lectin (SNA, alpha-2,6-SA). Our results show that the selected cancer cell lines in this study presented a varied binding behavior with the SA-MIPs. The binding pattern of the lectins was also demonstrated. Moreover, two different pentavalent SA conjugates were used to inhibit the binding of the SA-MIPs to breast, skin, and lung cancer cell lines, demonstrating the specificity of the SA-MIPs in both flow cytometry and confocal fluorescence microscopy. We concluded that the synthesized SA-MIPs might be a powerful future tool in the diagnostic analysis of various cancer cells. KW - Cancer KW - Imprinting KW - Molecularly imprinted polymers KW - SA conjugates KW - Sialic acid PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-546625 DO - https://doi.org/110.3390/cancers14081875 SN - 2072-6694 VL - 14 IS - 8 PB - MDPI CY - Basel AN - OPUS4-54662 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bhattacharya, Biswajit A1 - Michalchuk, Adam A1 - Silbernagl, Dorothee A1 - Rautenberg, Max A1 - Schmid, Thomas A1 - Feiler, Torvid A1 - Reimann, K. A1 - Ghalgaoui, A. A1 - Sturm, Heinz A1 - Paulus, B. A1 - Emmerling, Franziska T1 - A Mechanistic Perspective on Plastically Flexible Coordination Polymers N2 - Mechanical flexibility in single crystals of covalently bound materials is a fascinating and poorly understood phenomenon. We present here the first example of a plastically flexible one-dimensional (1D) coordination polymer. The compound [Zn(m-Cl)2(3,5-dichloropyridine)2]n is flexible over two crystallographic faces. Remarkably, the single crystal remains intact when bent to 1808. A combination of microscopy, diffraction, and spectroscopic studies have been used to probe the structural response of the crystal lattice to mechanical bending. Deformation of the covalent polymer chains does not appear to be responsible for the observed macroscopic bending. Instead, our results suggest that mechanical bending occurs by displacement of the coordination polymer chains. Based on experimental and theoretical evidence, we propose a new model for mechanical flexibility in 1D coordination polymers. Moreover, our calculations propose a cause of the different mechanical properties of this compound and a structurally similar elastic material KW - Coordination polymer KW - Flexible crystals KW - Mechanical properties KW - Plastic deformation PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-504755 DO - https://doi.org/10.1002/anie.201914798 VL - 59 IS - 14 SP - 5557 EP - 5561 PB - Wiley-VCH AN - OPUS4-50475 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bhuckory, S. A1 - Wegner, Karl David A1 - Qiu, X. A1 - Wu, Y.T. A1 - Jennings, T. L. A1 - Incamps, A. A1 - Hildebrandt, N. T1 - Triplexed CEA-NSE-PSA Immunoassay Using Time-Gated Terbium-to-Quantum Dot FRET N2 - Time-gated Förster resonance energy transfer (TG-FRET) between Tb complexes and luminescent semiconductor quantum dots (QDs) provides highly advantageous photophysical properties for multiplexed biosensing. Multiplexed Tb-to-QD FRET immunoassays possess a large potential for in vitro diagnostics, but their performance is often insufficient for their application under clinical conditions. Here, we developed a homogeneous TG-FRET immunoassay for the quantification of carcinoembryonic antigen (CEA), neuron-specific enolase (NSE), and prostatespecific antigen (PSA) from a single serum sample by multiplexed Tb-to-QD FRET. Tb–IgG antibody donor conjugates were combined with compact QD-F(ab’)2 antibody acceptor conjugates with three different QDs emitting at 605, 650, and 705 nm. Upon antibody–antigen–antibody Sandwich complex formation, the QD acceptors were sensitized via FRET from Tb, and the FRET ratios of QD and Tb TG luminescence intensities increased specifically with increasing antigen concentrations. Although limits of detection (LoDs: 3.6 ng/mL CEA, 3.5 ng/mL NSE, and 0.3 ng/mL PSA) for the triplexed assay were slightly higher compared to the single-antigen assays, they were still in a clinically relevant concentration range and could be quantified in 50 μL serum samples on a B·R·A·H·M·S KRYPTOR Compact PLUS clinical immunoassay plate reader. The simultaneous quantification of CEA, NSE, and PSA at different concentrations from the same serum sample demonstrated actual multiplexing Tb-to-QD FRET immunoassays and the potential of this technology for translation into clinical diagnostics. KW - Lanthanides KW - Nanoparticles KW - Biosensing KW - Multiplexing KW - FRET KW - Fluorescence KW - PSA KW - NSE KW - CEA PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-512290 DO - https://doi.org/10.3390/molecules25163679 VL - 25 IS - 16 SP - 3679 PB - MDPI AN - OPUS4-51229 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Biesen, L. A1 - Krenzer, J. A1 - Nirmalananthan-Budau, Nithiya A1 - Resch-Genger, Ute A1 - Müller, Th. J. J. T1 - Asymmetrically bridged aroyl-S,N-ketene acetalbased multichromophores with aggregationinduced tunable emission N2 - Asymmetrically bridged aroyl-S,N-ketene acetals and aroyl-S,N-ketene acetal multichromophores can be readily synthesized in consecutive three-, four-, or five-component syntheses in good to excellent yields by several successive Suzuki-couplings of aroyl-S,N-ketene acetals and bis(boronic)acid esters. Different aroyl-S,N-ketene acetals as well as linker molecules yield a library of 23 multichromophores with substitution and linker pattern-tunable emission properties. This allows control of different communication pathways between the chromophores and of aggregation-induced emission (AIE) and energy transfer (ET) properties, providing elaborate aggregation-based fluorescence switches. KW - Dye KW - Aggregation KW - Aggregation induced emission KW - Signal enhancement KW - Energy transfer KW - Switch KW - Sensor KW - Quantum yield KW - Lifetime KW - Photophysics KW - Sythesis KW - Nanaoparticle PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-550719 DO - https://doi.org/10.1039/d2sc00415a VL - 13 SP - 5374 EP - 5381 PB - Royal Society of Chemistry AN - OPUS4-55071 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Biesen, L. A1 - May, L. A1 - Nirmalananthan-Budau, Nithiya A1 - Hoffmann, Katrin A1 - Resch-Genger, Ute A1 - Müller, T. J. J. T1 - Communication of Bichromophore Emission upon Aggregation – Aroyl-S,N-ketene Acetals as Multifunctional Sensor Merocyanines N2 - Aroyl-S,N-ketene acetal-based bichromophores can be readily synthesized in a consecutive three-component synthesis in good to excellent yields by condensation of aroyl chlorides and an N-(p-bromobenzyl) 2-methyl benzothiazolium salt followed by a Suzuki coupling, yielding a library of 31 bichromophoric fluorophores with substitution patterntunable emission properties. Varying both chromophores enables different communication pathways between the chromophores, exploiting aggregation-induced emission (AIE) and energy transfer (ET) properties, and thus, furnishing aggregation-based fluorescence switches. Possible applications range from fluorometric analysis of alcoholic beverages to pH sensors. KW - Dye KW - Fluorescence KW - Aggregation induced emission KW - Signal enhancement KW - Energy transfer KW - Switch KW - Sensor KW - Quantum yield KW - Lifetime KW - Photophysics KW - Synthesis PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-531123 DO - https://doi.org/10.1002/chem.202102052 VL - 27 IS - 53 SP - 13426 EP - 13434 PB - Wiley-VCH AN - OPUS4-53112 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Biesen, L. A1 - Nirmalananthan-Budau, Nithiya A1 - Hoffmann, Katrin A1 - Resch-Genger, Ute A1 - Müller, T. J. J. T1 - Solid-State Emissive Aroyl-S,N-Ketene Acetals with Tunable N2 - N-Benzyl aroyl-S,N-ketene acetals can be readily synthesized by condensation of aroyl chlorides and N-Benzyl 2-methyl benzothiazolium salts in good to excellent yields, yielding a library of 35 chromophores with bright solid-state emission and aggregation-induced emission characteristics. Varying the substituent from electron-donating to electronwithdrawing enables the tuning of the solid-state emission Color from deep blue to red. KW - Nano KW - Nanoparticle KW - Photoluminescence KW - Fluorescence KW - Quantum yield KW - Photophysics KW - Lifetime KW - Sensor KW - dye KW - Enhancement KW - Particle KW - Polarity KW - AIE KW - Aggregation KW - Aggregation-induced emission KW - Solid state emission PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-509072 DO - https://doi.org/10.1002/anie.201916396 VL - 59 IS - 25 SP - 10037 EP - 10041 PB - Wiley Online Libary AN - OPUS4-50907 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Blumrich, A. A1 - Vogler, G. A1 - Dresen, S. A1 - Diop, S. B. A1 - Jaeger, Carsten A1 - Leberer, S. A1 - Grune, J. A1 - Wirth, E. K. A1 - Hoeft, B. A1 - Renko, K. A1 - Foryst-Ludwig, A. A1 - Spranger, J. A1 - Sigrist, S. A1 - Bodmer, R. A1 - Kintscher, U. T1 - Fat-body brummer lipase determines survival and cardiac function during starvation in Drosophila melanogaster N2 - The cross talk between adipose tissue and the heart has an increasing importance for cardiac function under physiological and pathological conditions. This study characterizes the role of fat body lipolysis for cardiac function in Drosophila melanogaster. Perturbation of the function of the key lipolytic enzyme, brummer (bmm), an ortholog of themammalian ATGL (adipose triglyceride lipase) exclusively in the fly’s fat body, protected the heart against starvation-induced dysfunction. We further provide evidence that this protection is caused by the preservation of glycerolipid stores, resulting in a starvation-resistant maintenance of energy supply and adequate cardiac ATP synthesis. Finally, we suggest that alterations of lipolysis are tightly coupled to lipogenic processes, participating in the preservation of Lipid energy substrates during starvation. Thus, we identified the inhibition of adipose tissue lipolysis and subsequent energy preservation as a protective mechanism against cardiac dysfunction during catabolic stress. KW - High-resolution mass spectrometry KW - Nontarget analysis PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-528756 DO - https://doi.org/10.1016/j.isci.2021.102288 VL - 24 IS - 4 SP - 102288 AN - OPUS4-52875 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bornemann-Pfeiffer, Martin A1 - Kern, Simon A1 - Maiwald, Michael A1 - Meyer, Klas T1 - Calibration-Free Chemical Process and Quality Control Units as Enablers for Modular Production N2 - Modular chemical production is a tangible translation of the digital transformation of the process industry for specialty chemicals. In particular, it enables the speeding-up of process development and thus a quicker time to market by flexibly connecting and orchestrating standardised physical modules and bringing them to life (i.e., parameterising them) with digitally accumulated process knowledge. We focus on the specific challenges of chemical process and quality control, which in its current form is not well suited for modular production and provide possible approaches and examples of the change towards direct analytical methods, analytical model transfer or machine-supported processes. KW - Modular Production KW - Chemical Process Control KW - Process Analytical Technology KW - Digital Transformation KW - Industry 4.0 PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-517264 DO - https://doi.org/10.1002/cite.202000150 SN - 1522-2640 VL - 93 IS - 1-2 SP - 62 EP - 70 PB - Wiley-VCH CY - Weinheim AN - OPUS4-51726 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bornemann-Pfeiffer, Martin A1 - Meyer, Klas A1 - Lademann, J. A1 - Kraume, M. A1 - Maiwald, Michael T1 - Contributions towards variable temperature shielding for compact NMR instruments N2 - The application of compact NMR instruments to hot flowing samples or exothermically reacting mixtures is limited by the temperature sensitivity of permanent magnets. Typically, such temperature effects directly influence the achievable magnetic field homogeneity and hence measurement quality. The internal-temperature control loop of the magnet and instruments is not designed for such temperature compensation. Passive insulation is restricted by the small dimensions within the magnet borehole. Here, we present a design approach for active heat shielding with the aim of variable temperature control of NMR samples for benchtop NMR instruments using a compressed airstream which is variable in flow and temperature. Based on the system identification and surface temperature measurements through thermography, a model predictive control was set up to minimise any disturbance effect on the permanent magnet from the probe or sample temperature. This methodology will facilitate the application of variable-temperature shielding and, therefore, extend the application of compact NMR instruments to flowing sample temperatures that differ from the magnet temperature. KW - Benchtop NMR KW - Continuous Processes KW - Inline Analytics KW - Model Predictive Control KW - Process Analytical Tecnology KW - Temperature Control PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-579219 DO - https://doi.org/10.1002/mrc.5379 SN - 1097-458X SP - 1 EP - 10 PB - John Wiley & Sons Ltd. AN - OPUS4-57921 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bosc-Bierne, Gaby A1 - Ewald, Shireen A1 - Kreuzer, Oliver J. A1 - Weller, Michael G. T1 - Efficient Quality Control of Peptide Pools by UHPLC and Simultaneous UV and HRMS Detection N2 - Peptide pools consist of short amino acid sequences and have proven to be versatile tools in various research areas in immunology and clinical applications. They are commercially available in many different compositions and variants. However, unlike other reagents that consist of only one or a few compounds, peptide pools are highly complex products which makes their quality control a major challenge. Quantitative peptide analysis usually requires sophisticated methods, in most cases isotope-labeled standards and reference materials. Usually, this would be prohibitively laborious and expensive. Therefore, an approach is needed to provide a practical and feasible method for quality control of peptide pools. With insufficient quality control, the use of such products could lead to incorrect experimental results, worsening the well-known reproducibility crisis in the biomedical sciences. Here we propose the use of ultra-high performance liquid chromatography (UHPLC) with two detectors, a standard UV detector at 214 nm for quantitative analysis and a high-resolution mass spectrometer (HRMS) for identity confirmation. To be cost-efficient and fast, quantification and identification are performed in one chromatographic run. An optimized protocol is shown, and different peak integration methods are compared and discussed. This work was performed using a peptide pool known as CEF advanced, which consists of 32 peptides derived from cytomegalovirus (CMV), Epstein–Barr virus (EBV) and influenza virus, ranging from 8 to 12 amino acids in length. N2 - Peptidpools bestehen aus kurzen Aminosäuresequenzen und haben sich als vielseitige Werkzeuge in verschiedenen Forschungsbereichen der Immunologie und bei klinischen Anwendungen erwiesen. Sie sind in vielen verschiedenen Zusammensetzungen und Varianten im Handel erhältlich. Im Gegensatz zu anderen Reagenzien, die nur aus einer oder wenigen Verbindungen bestehen, sind Peptidpools jedoch hochkomplexe Produkte, was ihre Qualitätskontrolle zu einer großen Herausforderung macht. Die quantitative Peptidanalyse erfordert in der Regel ausgefeilte Methoden, in den meisten Fällen isotopenmarkierte Standards und Referenzmaterialien. Dies ist in der Regel sehr aufwändig und teuer. Daher wird ein Ansatz benötigt, der eine praktische und praktikable Methode zur Qualitätskontrolle von Peptidpools bietet. Bei unzureichender Qualitätskontrolle könnte die Verwendung solcher Produkte zu falschen Versuchsergebnissen führen, was das bekannte Problem der Reproduzierbarkeit in den biomedizinischen Wissenschaften noch verschärfen würde. Hier schlagen wir die Verwendung der Ultrahochleistungs-Flüssigkeitschromatographie (UHPLC) mit zwei Detektoren vor, einem Standard-UV-Detektor bei 214 nm für die quantitative Analyse und einem hochauflösenden Massenspektrometer (HRMS) für die Identitätsbestätigung. Um kosteneffizient und schnell zu sein, werden Quantifizierung und Identifizierung in einem einzigen chromatographischen Lauf durchgeführt. Es wird ein optimiertes Protokoll gezeigt, und es werden verschiedene Peak-Integrationsmethoden verglichen und diskutiert. Für diese Arbeit wurde ein Peptidpool verwendet, der als CEF advanced bekannt ist und aus 32 Peptiden besteht, die vom Cytomegalovirus (CMV), Epstein-Barr-Virus (EBV) und Influenzavirus stammen und zwischen 8 und 12 Aminosäuren lang sind. KW - Synthetic peptides KW - Quality control KW - Impurites KW - Byproducts KW - Degradation KW - Mass spectrometry KW - Orbitrap PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-602299 DO - https://doi.org/10.3390/separations11050156 SN - 2297-8739 VL - 11 IS - 5 SP - 1 EP - 18 PB - MDPI CY - Basel AN - OPUS4-60229 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bosc-Bierne, Gaby A1 - Weller, Michael G. T1 - Investigation of impurities in peptide pools T1 - Untersuchung von Verunreinigungen in Peptidpools N2 - Peptide pools are important research tools in different biomedical fields. They consist of a complex mixture of defined peptides, which places high demands on the production and quality control of these products. Previously it has been shown that the combination of UHPLC with high-resolution mass-spectrometry (HRMS) is a fast and powerful method to confirm the relative concentration and the structural identity of all peptides expected to be in the pool. In this work, the additional information contained in the UV chromatograms and mass spectra is used to search for impurities due to synthesis by-products and degradation during storage and transportation and to identify possible analytical artifacts. It was shown that most impurities are only present in trace amounts and can be considered uncritical for most applications. The most frequent and perhaps unexpected impurities were homo- and heterodimers caused by the free cysteines contained in these peptide pools. Furthermore, pyroglutamate and aspartimide formation, deamidation, methionine oxidation, and amino acid deletions could be found. This list is not intended to be comprehensive, but rather a brief guide to quickly identify impurities and, in the long term, to suggest possible changes in the composition of the peptide pools to avoid such impurities by design or by special precautions. N2 - Peptidpools sind wichtige Forschungsinstrumente in verschiedenen biomedizinischen Bereichen. Sie bestehen aus einer komplexen Mischung definierter Peptide, was hohe Anforderungen an die Herstellung und Qualitätskontrolle dieser Produkte stellt. In der Vergangenheit wurde gezeigt, dass die Kombination von UHPLC mit hochauflösender Massenspektrometrie (HRMS) eine schnelle und leistungsfähige Methode zur Bestätigung der relativen Konzentration und der strukturellen Identität aller Peptide ist, die in dem Pool erwartet werden. In dieser Arbeit werden die zusätzlichen Informationen, die in den UV-Chromatogrammen und Massenspektren enthalten sind, genutzt, um nach Verunreinigungen zu suchen, die auf Nebenprodukte der Synthese und den Abbau während der Lagerung und des Transports zurückzuführen sind, und um mögliche analytische Artefakte zu identifizieren. Es hat sich gezeigt, dass die meisten Verunreinigungen nur in Spuren vorhanden sind und für die meisten Anwendungen als unkritisch angesehen werden können. Die häufigsten und vielleicht unerwartetsten Verunreinigungen waren Homo- und Heterodimere, die durch die in diesen Peptidpools enthaltenen freien Cysteine verursacht werden. Außerdem wurden Pyroglutamat- und Aspartimidbildung, Deamidierung, Methioninoxidation und Aminosäuredeletionen festgestellt. Diese Liste erhebt keinen Anspruch auf Vollständigkeit, sondern ist eher ein kurzer Leitfaden, um Verunreinigungen schnell zu identifizieren und langfristig mögliche Änderungen in der Zusammensetzung der Peptidpools vorzuschlagen, um solche Verunreinigungen durch Design oder besondere Vorsichtsmaßnahmen zu vermeiden. KW - Synthetic peptides KW - Degradation KW - Synthetic artifacts KW - Peptide losses KW - Stability of peptides KW - Disulfide dimers KW - Cysteine dimers KW - Isomers KW - Cysteine alkylation PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-626987 DO - https://doi.org/10.3390/separations12020036 SN - 2297-8739 VL - 12 IS - 2 SP - 1 EP - 18 PB - MDPI AG CY - Basel AN - OPUS4-62698 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bourgon, Nicolas A1 - Oelze, Marcus A1 - Roberts, Patrick T1 - Less is more: Limiting semi-invasive sampling for multi-isotope analyses and increasing data output from single aliquot samples N2 - Developments in multi-isotope applications now enable the production of direct and precise life history data of studied archeological and paleoanthropological specimens, with analysis of tooth enamel proving particularly powerful in deep-time preservation contexts. However, the increasing amount of sample material necessary too-often compromises the specimen's structural integrity. Finding ways of minimizing semi-invasive sampling while maximizing produced data thus becomes increasingly crucial. In this study, we examine ways of optimizing sample use for state-of-the-art isotope measurements of enamel-bound zinc (δ66Zn), an increasingly used method in multi-isotope archeological research. We show that certain desolvating nebulizer introduction systems can be used to measure δ66Zn with high efficiency and accuracy using less than half the usual sample size. Moreover, we demonstrate that remaining samples subjected to typical pretreatments used for tooth enamel carbonate (δ13C and δ18O) studies can be safely used without alterations to δ66Zn values. Similarly, we highlight that the often-discarded matrix fraction from zinc chromatography can be utilized for further analyses, such as measurements of 87Sr/86Sr ratios. Our results underscore the possibility of extracting the maximum information from specimens while altogether avoiding or significantly reducing semi-invasive sampling. KW - Multi-isotope KW - Zinc isotope analysis KW - Tooth enamel PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-637986 DO - https://doi.org/10.1016/j.jas.2025.106308 SN - 0305-4403 VL - 180 SP - 1 EP - 8 PB - Elsevier Ltd. AN - OPUS4-63798 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Brangsch, J. A1 - Reimann, C. A1 - Kaufmann, Jan Ole A1 - Adams, L. C. A1 - Onthank, D. A1 - Thöne-Reineke, C. A1 - Robinson, S. A1 - Ponader, Marco A1 - Weller, Michael G. A1 - Buchholz, R. A1 - Karst, U. A1 - Botnar, R. A1 - Hamm, B. A1 - Makowski, M. R. T1 - Molecular MR-Imaging for Noninvasive Quantification of the Anti-Inflammatory Effect of Targeting Interleukin-1β in a Mouse Model of Aortic Aneurysm N2 - Background: Molecular-MRI is a promising imaging modality for the assessment of abdominal aortic aneurysms (AAAs). Interleukin-1β (IL-1β) represents a new therapeutic tool for AAA-treatment, since pro-inflammatory cytokines are key-mediators of inflammation. This study investigates the potential of molecular-MRI to evaluate therapeutic effects of an anti-IL-1β-therapy on AAA-formation in a mouse-model. Methods: Osmotic-minipumps were implanted in apolipoprotein-deficient-mice (N = 27). One group (Ang-II+01BSUR group, n = 9) was infused with angiotensin-II (Ang-II) for 4 weeks and received an anti-murine IL-1β-antibody (01BSUR) 3 times. One group (Ang-II-group, n = 9) was infused with Ang-II for 4 weeks but received no treatment. Control-group (n = 9) was infused with saline and received no treatment. MR-imaging was performed using an elastin-specific gadolinium-based-probe (0.2 mmol/kg). Results: Mice of the Ang-II+01BSUR-group showed a lower aortic-diameter compared to mice of the Ang-II-group and control mice (p < 0.05). Using the elastin-specific-probe, a significant decrease in elastin-destruction was observed in mice of the Ang-II+01BSUR-group. In vivo MR-measurements correlated well with histopathology (y = 0.34x-13.81, R2 = 0.84, p < 0.05), ICP-MS (y = 0.02x+2.39; R2 = 0.81, p < 0.05) and LA-ICP-MS. Immunofluorescence and western-blotting confirmed a reduced IL-1β-expression. Conclusions: Molecular-MRI enables the early visualization and quantification of the anti-inflammatory-effects of an IL-1β-inhibitor in a mouse-model of AAAs. Responders and non-responders could be identified early after the initiation of the therapy using molecular-MRI. KW - Cardiovascular KW - Molecular-MRI KW - Magnetic resonance imaging KW - Gadolinium-based contrast agent KW - Elastin-specific contrast agent ESMA KW - Gadovist KW - Gadofosveset KW - MR Angiography KW - Inductively Coupled Mass Spectroscopy KW - Element Specific Bioimaging Using Laser Ablation KW - Visualization PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-517150 DO - https://doi.org/10.1177/1536012120961875 N1 - Geburtsname von Ponader, Marco: Wilke, M. - Birth name of Ponader, Marco: Wilke, M. VL - 19 SP - 61875 PB - SAGE AN - OPUS4-51715 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Brauckmann, C. A1 - Pramann, A. A1 - Rienitz, O. A1 - Schulze, A. A1 - Phukphatthanachai, Pranee A1 - Vogl, Jochen T1 - Combining Isotope Dilution and Standard Addition—Elemental Analysis in Complex Samples N2 - A new method combining isotope dilution mass spectrometry (IDMS) and standard addition has been developed to determine the mass fractions w of different elements in complex matrices: (a) silicon in aqueous tetramethylammonium hydroxide (TMAH), (b) sulfur in biodiesel fuel, and (c) iron bound to transferrin in human serum. All measurements were carried out using inductively coupled plasma mass spectrometry (ICP–MS). The method requires the gravimetric preparation of several blends (bi)—each consisting of roughly the same masses (mx,i) of the sample solution (x) and my,i of a spike solution (y) plus different masses (mz,i) of a reference solution (z). Only these masses and the isotope ratios (Rb,i) in the blends and reference and spike solutions have to be measured. The derivation of the underlying equations based on linear regression is presented and compared to a related concept reported by Pagliano and Meija. The uncertainties achievable, e.g., in the case of the Si blank in extremely pure TMAH of urel (w(Si)) = 90% (linear regression method, this work) and urel (w(Si)) = 150% (the method reported by Pagliano and Meija) seem to suggest better applicability of the new method in practical use due to the higher robustness of regression analysis. KW - Isotope dilution mass spectrometry KW - tandard addition KW - ICP-MS KW - lank characterization KW - Silicon KW - Sulfur KW - Transferrin KW - Tetramethylammonium hydroxide KW - Biodiesel fuel KW - Human serum PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-526376 DO - https://doi.org/10.3390/molecules26092649 VL - 26 IS - 9 SP - 2649 PB - MDPI CY - Basel AN - OPUS4-52637 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Braun, Jennifer A1 - Engelhard, Carsten A1 - Kaul, Peter T1 - Optimized fast gas chromatography coupled with proton-transfer-reaction time-of-flight mass spectrometry for the selective near real-time analysis of herbivore-induced plant volatiles N2 - The analysis of herbivore-induced plant volatiles (HIPVs) is essential for understanding plant-environment interactions and defense strategies against herbivores. Proton transfer reaction time-of-flight mass spectrometry (PTR–TOF–MS) is a powerful analytical tool that enables real-time monitoring and quantification of diverse groups of HIPVs. However, the PTR–TOF–MS technique is constrained in its ability to effectively differentiate between isomers. When analyzing complex mixtures of HIPVs, the separation of isomers becomes crucial as major compound classes such as terpenes comprise thousands of isomers. In this study, we present an optimized fast gas chromatography (fastGC) based on a modified version of the commercially available fastGC add-on integrated into a mobile PTR–TOF. The system was optimized for the analysis of emissions from enclosed trunks of Acer platanoides infested by Anoplophora glabripennis (Motschulsky), commonly known as Asian longhorned beetle (ALB). The development of fastGC was primarily focused on the sesquiterpenes α-longipinene, cyclosativene and α-copaene, which serve as strong indicators of ALB infestation. These sesquiterpenes were separated in less than three minutes, with intra-day retention time RSD < 0.6 % and resolutions of 2.6 ± 0.3 and 1.3 ± 0.2. In comparison to the original system, the optimized fastGC demonstrates more than tripled sesquiterpene resolution, twice the sensitivity relative to direct inlet mode, and an approximately 10 % reduction in total analysis time. The optimized fastGC–PTR–TOF allows for near real-time analysis of complex mixtures of biogenic VOCs, making it a powerful tool for environmental monitoring, integrated pest management, and forest protection. KW - Mass Spectrometry KW - PTR-TOF-MS KW - Gas Chromatography KW - Herbivore-induced plant volatiles KW - Sesquiterpenes PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-639513 DO - https://doi.org/10.1016/j.chroma.2025.466236 SN - 0021-9673 VL - 1759 SP - 1 EP - 16 PB - Elsevier B.V. AN - OPUS4-63951 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Braymer, Joseph J. A1 - Knauer, Lukas A1 - Crack, Jason C. A1 - Oltmanns, Jonathan A1 - Heghmanns, Melanie A1 - Soares, Jéssica C. A1 - Le Brun, Nick E. A1 - Schünemann, Volker A1 - Kasanmascheff, Müge T1 - Yeast [FeFe]-hydrogenase-like protein Nar1 binds a [2Fe–2S] cluster N2 - Nar1 is an essential eukaryotic protein proposed to function as an iron–sulphur (Fe/S) cluster trafficking factor in the cytosolic iron–sulphur protein assembly (CIA) machinery. However, such a role has remained unclear due to difficulties in purifying adequate amounts of cofactor-bound protein. The [FeFe]-hydrogenase-like protein has two conserved binding sites for [4Fe–4S] clusters but does not show hydrogenase activity in vivo due to the lack of an active site [2Fe]H cofactor. Here, we report a new preparation procedure for Nar1 that facilitated studies by UV-vis, EPR, and Mössbauer spectroscopies, along with native mass spectrometry. Nar1 recombinantly produced in E. coli contained a [4Fe–4S] cluster, bound presumably at site 1, along with an unexpected [2Fe–2S] cluster bound at an unknown site. Fe/S reconstitution reactions installed a second [4Fe–4S] cluster at site 2, leading to protein with up to three Fe/S cofactors. It is proposed that the [2Fe–2S] cluster occupies a cavity in Nar1 that is filled by the [2Fe]H cofactor in [FeFe]-hydrogenases. Strikingly, two of the Fe/S clusters were rapidly destroyed by molecular oxygen, linking Nar1 oxygen sensitivity in vitro to phenotypes observed previously in vivo. Our biochemical results, therefore, validate a direct link between cellular oxygen concentrations and the functioning of the CIA pathway. These advances also now allow for the pursuit of in vitro Fe/S cluster transfer assays, which will shed light on Fe/S trafficking and insertion by CIA components. KW - Biocorrosion KW - Hydrogenases KW - Metalloprotein KW - Yeast PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-649463 DO - https://doi.org/10.1039/D5SC04860E SN - 2041-6520 VL - 17 IS - 1 SP - 373 EP - 380 PB - Royal Society of Chemistry (RSC) AN - OPUS4-64946 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Braymer, Joseph J. A1 - Stehling, Oliver A1 - Stümpfig, Martin A1 - Rösser, Ralf A1 - Spantgar, Farah A1 - Blinn, Catharina M. A1 - Mühlenhoff, Ulrich A1 - Pierik, Antonio J. A1 - Lill, Roland T1 - Requirements for the biogenesis of [2Fe-2S] proteins in the human and yeast cytosol N2 - The biogenesis of iron–sulfur (Fe/S) proteins entails the synthesis and trafficking of Fe/S clusters, followed by their insertion into target apoproteins. In eukaryotes, the multiple steps of biogenesis are accomplished by complex protein machineries in both mitochondria and cytosol. The underlying biochemical pathways have been elucidated over the past decades, yet the mechanisms of cytosolic [2Fe-2S] protein assembly have remained ill-defined. Similarly, the precise site of glutathione (GSH) requirement in cytosolic and nuclear Fe/S protein biogenesis is unclear, as is the molecular role of the GSH-dependent cytosolic monothiol glutaredoxins (cGrxs). Here, we investigated these questions in human and yeast cells by various in vivo approaches. [2Fe-2S] cluster assembly of cytosolic target apoproteins required the mitochondrial ISC machinery, the mitochondrial transporter Atm1/ABCB7 and GSH, yet occurred independently of both the CIA system and cGrxs. This mechanism was strikingly different from the ISC-, Atm1/ABCB7-, GSH-, and CIA-dependent assembly of cytosolic–nuclear [4Fe-4S] proteins. One notable exception to this cytosolic [2Fe-2S] protein maturation pathway defined here was yeast Apd1 which used the CIA system via binding to the CIA targeting complex through its C-terminal tryptophan. cGrxs, although attributed as [2Fe-2S] cluster chaperones or trafficking proteins, were not essential in vivo for delivering [2Fe-2S] clusters to either CIA components or target apoproteins. Finally, the most critical GSH requirement was assigned to Atm1-dependent export, i.e. a step before GSH-dependent cGrxs function. Our findings extend the general model of eukaryotic Fe/S protein biogenesis by adding the molecular requirements for cytosolic [2Fe-2S] protein maturation. KW - Biokorrosion KW - Hydrogenasen KW - Microbially Induced Corrosion PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-602328 DO - https://doi.org/10.1073/pnas.2400740121 SN - 0027-8424 VL - 121 IS - 21 SP - 1 EP - 12 PB - Proceedings of the National Academy of Sciences CY - Washington D.C. AN - OPUS4-60232 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Breuninger, Esther S. A1 - Tolu, Julie A1 - Aemisegger, Franziska A1 - Thurnherr, Iris A1 - Bouchet, Sylvain A1 - Mestrot, Adrien A1 - Ossola, Rachele A1 - McNeill, Kristopher A1 - Tukhmetova, Dariya A1 - Vogl, Jochen A1 - Meermann, Björn A1 - Sonke, Jeroen E. A1 - Winkel, Lenny H. E. T1 - Marine and terrestrial contributions to atmospheric deposition fluxes of methylated arsenic species N2 - Arsenic, a toxic element from both anthropogenic and natural sources, reaches surface environments through atmospheric cycling and dry and wet deposition. Biomethylation volatilizes arsenic into the atmosphere and deposition cycles it back to the surface, affecting soil-plant systems. Chemical speciation of deposited arsenic is important for understanding further processing in soils and bioavailability. However, the range of atmospheric transport and source signature of arsenic species remain understudied. Here we report significant levels ofmethylated arsenic in precipitation, cloudwater and aerosols collected under free tropospheric conditions at Pic du Midi Observatory (France) indicating long-range transport, which is crucial for atmospheric budgets. Through chemical analyses andmoisture source diagnostics, we identify terrestrial and marine sources for distinct arsenic species. Estimated atmospheric deposition fluxes of methylated arsenic are similar to reported methylation rates in soils, highlighting atmospheric deposition as a significant, overlooked source of potentially bioavailable methylated arsenic species impacting plant uptake in soils. KW - Arsenic KW - Speciation KW - Fluxes KW - Marine KW - Terrestrial KW - Sulfur isotopes PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-615551 DO - https://doi.org/10.1038/s41467-024-53974-z SN - 2041-1723 VL - 15 IS - 1 SP - 1 EP - 13 PB - Springer Science and Business Media LLC AN - OPUS4-61555 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bruno, Francesco A1 - Fiorucci, Letizia A1 - Vignoli, Alessia A1 - Meyer, Klas A1 - Maiwald, Michael A1 - Ravera, Enrico T1 - pyIHM: Indirect Hard Modeling, in Python N2 - NMR is a powerful analytical technique that combines an exquisite qualitative power, related to the unicity of the spectra of each molecule in a mixture, with an intrinsic quantitativeness, related to the fact that the integral of each peak only depends on the number of nuclei (i.e., the amount of substance times the number of equivalent nuclei in the signal), regardless of the molecule. Signal integration is the most common approach in quantitative NMR but has several drawbacks (vide infra). An alternative is to use hard modeling of the peaks. In this paper, we present pyIHM, a Python package for the quantification of the components of NMR spectra through indirect hard modeling, and we discuss some numerical details of the implementation that make this approach robust and reliable. KW - Algorithms KW - Chemical Structure KW - Deconvolution KW - Mixtures KW - NMR spectroscopy PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-626793 DO - https://doi.org/10.1021/acs.analchem.4c06484 SN - 1520-6882 VL - 97 IS - 8 SP - 4598 EP - 4605 PB - ACS Publications CY - Washington D.C. AN - OPUS4-62679 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Bröcker, S. A1 - Klaer, R.-H. A1 - Kockmann, N. A1 - Maiwald, Michael T1 - Process Industry United in the Digital World - The current landscape of research for the digitalization of the process industry N2 - The Tutzing Symposium "100 % digital: survival strategies for the process industry" (see 4.1) in April 2018 was characterized by a great momentum which has been taken up and continued until today. The aim was to implement the ideas from the Tutzing Symposium in a coordinated and targeted manner. For this purpose, development needs as well as the numerous currently planned or already started research and development activities in the context of digitalisation were first compiled and analysed. This resulted in the current research landscape for digitalization in the process industry. It now enables to identify open topics and to translate them into research funding programs as well as to define new projects in the dialogue between users, suppliers and research, which are to be meaningfully interlinked and consolidated with existing projects. Due to the strong interest in digitalisation, activities are constantly being added, so that this paper can only provide a snapshot of the situation in the period 2019-2020. KW - Process Industry KW - Digitalisation KW - Tutzing Symposion KW - research landscape KW - Process Control PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-512265 UR - https://processnet.org/en/TAKdigital.html SP - 1 EP - 15 AN - OPUS4-51226 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Burnage, Samual A1 - Bell, Jérémy A1 - Wan, Wei A1 - Kislenko, Evgeniia A1 - Rurack, Knut T1 - Combining a hybrid chip and tube microfluidic system with fluorescent molecularly imprinted polymer (MIP) core–shell particles for the derivatisation, extraction, and detection of peptides with N-terminating phosphorylated tyrosine N2 - The reliable identification and quantitation of phosphorylated amino acids, peptides and proteins is one of the key challenges in contemporary bioanalytical research, an area of particular interest when attempting to diagnose and treat diseases at an early stage. We have developed a synthetic probe for targeting phosphorylated amino acids, based on core–shell submicron-sized particles consisting of a silica core, coated with a molecularly imprinted polymer (MIP) shell. The MIP layer contains a fluorescent probe crosslinker which binds selectively to phosphorylated tyrosine (pY) moieties with a significant imprinting factor (IF) and responds with a "light-up” fluorescence signal. The bead-based ratiometric detection scheme has been successfully transferred to a microfluidic chip format and its applicability to rapid assays has been exemplarily shown by discriminating a pY-terminating oligopeptide against its nonphosphorylated counterpart. Such miniaturised devices could lead to an automated pY or pY N-terminated peptide measurement system in the future. The setup combines a modular microfluidic system for amino acid derivatisation, extraction (by micropillar co-flow) and selective adsorption and detection with the fluorescent MIP core–shell particle probes. A miniaturised optical assembly for low-light fluorescence measurements was also developed, based on miniaturised opto-electronic parts and optical fibres. The emission from the MIP particles upon binding of pY or pY N-terminated peptides could be monitored in real-time. KW - Microfluidics KW - Molecularly imprinted polymers KW - Phosphorylated peptides KW - Fluorescence KW - Core-shell particles PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-569204 DO - https://doi.org/10.1039/d2lc00955b SN - 1473-0197 VL - 23 IS - 3 SP - 466 EP - 474 PB - Royal Society of Chemistry CY - Cambridge AN - OPUS4-56920 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Cairns, Warren R. L. A1 - Braysher, Emma C. A1 - Butler, Owen T. A1 - Cavoura, Olga A1 - Davidson, Christine M. A1 - Todoli Torro, Jose Luis A1 - von der Au, Marcus T1 - Atomic spectrometry update: review of advances in environmental analysis N2 - This review covers advances in the analysis of air, water, plants, soils and geological materials by a range of atomic spectrometric techniques including atomic emission, absorption, fluorescence and mass spectrometry. KW - Environmental analysis KW - Review KW - Trend Article PY - 2026 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-653977 DO - https://doi.org/10.1039/D5JA90058A SN - 0267-9477 VL - 41 IS - 1 SP - 16 EP - 70 PB - Royal Society of Chemistry (RSC) AN - OPUS4-65397 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Chan, George C.-Y. A1 - Hieftje, Gary M. A1 - Omenetto, Nicoló A1 - Axner, Ove A1 - Bengtson, Arne A1 - Bings, Nicolas H. A1 - Blades, Michael W. A1 - Bogaerts, Annemie A1 - Bolshov, Mikhail A. A1 - Broekaert, José A.C. A1 - Chan, WingTat A1 - Costa-Fernández, José M. A1 - Crouch, Stanley R. A1 - De Giacomo, Alessandro A1 - D’Ulivo, Alessandro A1 - Engelhard, Carsten A1 - Falk, Heinz A1 - Farnsworth, Paul B. A1 - Florek, Stefan A1 - Gamez, Gerardo A1 - Gornushkin, Igor B. A1 - Günther, Detlef A1 - Hahn, David W. A1 - Hang, Wei A1 - Hoffmann, Volker A1 - Jakubowski, Norbert A1 - Karanassios, Vassili A1 - Koppenaal, David W. A1 - Kenneth Marcus, R. A1 - Noll, Reinhard A1 - Olesik, John W. A1 - Palleschi, Vincenzo A1 - Panne, Ulrich A1 - Pisonero, Jorge A1 - Ray, Steven J. A1 - Resano, Martín A1 - Russo, Richard E. A1 - Scheeline, Alexander A1 - Smith, Benjamin W. A1 - Sturgeon, Ralph E. A1 - Todolí, José-Luis A1 - Tognoni, Elisabetta A1 - Vanhaecke, Frank A1 - Webb, Michael R. A1 - Winefordner, James D. A1 - Yang, Lu A1 - Yu, Jin A1 - Zhang, Zhanxia T1 - Landmark Publications in Analytical Atomic Spectrometry: Fundamentals and Instrumentation Development N2 - The almost-two-centuries history of spectrochemical analysis has generated a body of literature so vast that it has become nearly intractable for experts, much less for those wishing to enter the field. Authoritative, focused reviews help to address this problem but become so granular that the overall directions of the field are lost. This broader perspective can be provided partially by general overviews but then the thinking, experimental details, theoretical underpinnings and instrumental innovations of the original work must be sacrificed. In the present compilation, this dilemma is overcome by assembling the most impactful publications in the area of analytical atomic spectrometry. Each entry was proposed by at least one current expert in the field and supported by a narrative that justifies its inclusion. The entries were then assembled into a coherent sequence and returned to contributors for a round-robin review. KW - Analytical atomic spectrometry KW - Spectroscopy KW - Instrumental analysis PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-621588 DO - https://doi.org/10.1177/00037028241263567 SN - 1943-3530 VL - 78 SP - 1 EP - 456 PB - Sage CY - London AN - OPUS4-62158 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Chapartegui-Arias, Ander A1 - Raysyan, A. A1 - Belenguer, A. M. A1 - Jaeger, Carsten A1 - Tchipilov, Teodor A1 - Prinz, Carsten A1 - Abad Andrade, Carlos Enrique A1 - Beyer, S. A1 - Schneider, Rudolf A1 - Emmerling, Franziska T1 - Tailored mobility in a zeolite imidazolate framework (ZIF) antibody conjugate N2 - Zeolitic imidazolate framework (ZIF) hybrid fluorescent nanoparticles and ZIF antibody conjugates have been synthesized, characterized, and employed in lateral-flow immunoassay (LFIA). The bright fluorescence of the conjugates and the possibility to tailor their mobility gives a huge potential for diagnostic assays. An enzyme-linked immunosorbent assay (ELISA) with horseradish peroxidase (HRP) as label, proved the integrity, stability, and dispersibility of the antibody conjugates, LC-MS/MS provided evidence that a covalent link was established between these metal-organic frameworks and lysine residues in IgG antibodies. KW - ZIF KW - ELISA PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-532096 DO - https://doi.org/10.1002/chem.202100803 SN - 0947-6539 SN - 1521-3765 VL - 27 IS - 36 SP - 9414 EP - 9421 PB - Wiley-VCH CY - Weinheim AN - OPUS4-53209 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Chen, Xinyue A1 - Dong, Ximan A1 - Zhang, Chuyan A1 - Zhu, Meng A1 - Ahmed, Essraa A1 - Krishnamurthy, Giridharan A1 - Rouzbahani, Rozita A1 - Pobedinskas, Paulius A1 - Gauquelin, Nicolas A1 - Jannis, Daen A1 - Kaur, Kawaljit A1 - Hafez, Aly Mohamed Elsayed A1 - Thiel, Felix A1 - Bornemann, Rainer A1 - Engelhard, Carsten A1 - Schönherr, Holger A1 - Verbeeck, Johan A1 - Haenen, Ken A1 - Jiang, Xin A1 - Yang, Nianjun T1 - Interlayer Affected Diamond Electrochemistry N2 - Diamond electrochemistry is primarily influenced by quantities of sp3‐carbon, surface terminations, and crystalline structure. In this work, a new dimension is introduced by investigating the effect of using substrate‐interlayers for diamond growth. Boron and nitrogen co‐doped nanocrystalline diamond (BNDD) films are grown on Si substrate without and with Ti and Ta as interlayers, named BNDD/Si, BNDD/Ti/Si, and BNDD/Ta/Ti/Si, respectively. After detailed characterization using microscopies, spectroscopies, electrochemical techniques, and density functional theory simulations, the relationship of composition, interfacial structure, charge transport, and electrochemical properties of the interface between diamond and metal is investigated. The BNDD/Ta/Ti/Si electrodes exhibit faster electron transfer processes than the other two diamond electrodes. The interlayer thus determines the intrinsic activity and reaction kinetics. The reduction in their barrier widths can be attributed to the formation of TaC, which facilitates carrier tunneling, and simultaneously increases the concentration of electrically active defects. As a case study, the BNDD/Ta/Ti/Si electrode is further employed to assemble a redox‐electrolyte‐based supercapacitor device with enhanced performance. In summary, the study not only sheds light on the intricate relationship between interlayer composition, charge transfer, and electrochemical performance but also demonstrates the potential of tailored interlayer design to unlock new capabilities in diamond‐based electrochemical devices. KW - Nanocrystalline diamond KW - Interfaces KW - Electrochemistry KW - TOF-SIMS KW - SEM PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-621576 DO - https://doi.org/10.1002/smtd.202301774 SN - 2366-9608 VL - 9 IS - 2 SP - 1 EP - 10 PB - Wiley VHC-Verlag CY - Weinheim AN - OPUS4-62157 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Chronakis, Michail Ioannis A1 - Meermann, Björn A1 - von der Au, Marcus T1 - The evolution of data treatment tools in single-particle and single-cell ICP-MS analytics N2 - Single-particle inductively coupled plasma-mass spectrometry (sp-ICP-MS) is one of the most powerful tools in the thriving field of nanomaterial analysis. Along the same lines, single-cell ICP-MS (sc-ICP-MS) has become an invaluable tool in the study of the variances of cell populations down to a per-cell basis. Their importance and application fields have been listed numerous times, across various reports and reviews. However, not enough attention has been paid to the immense and ongoing development of the tools that are currently available to the analytical community for the acquisition, and more importantly, the treatment of single-particle and single-cell-related data. Due to the ever-increasing demands of modern research, the efficient and dependable treatment of the data has become more important than ever. In addition, the field of single-particle and single-cell analysis suffers due to a large number of approaches for the generated data—with varying levels of specificity and applicability. As a result, finding the appropriate tool or approach, or even comparing results, can be challenging. This article will attempt to bridge these gaps, by covering the evolution and current state of the tools at the disposal of sp-ICP-MS users. Graphical Abstract KW - Trend Article KW - spICP-MS KW - Data Tools KW - scICP-MS PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-610539 DO - https://doi.org/10.1007/s00216-024-05513-4 SP - 1 EP - 7 PB - Springer Science and Business Media LLC AN - OPUS4-61053 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Clark, P.C.J A1 - Andresen, Elina A1 - Sear, M. J. A1 - Favaro, M. A1 - Girardi, L. A1 - van de Krol, R. A1 - Resch-Genger, Ute A1 - Starr, D.E. T1 - Quantification of the Activator and Sensitizer Ion Distributions in NaYF4:Yb3+, Er3+ Upconverting Nanoparticles Via Depth-Profiling with Tender X-Ray Photoemission N2 - The spatial distribution and concentration of lanthanide activator and sensitizer dopant ions are of key importance for the luminescence color and efficiency of upconverting nanoparticles (UCNPs). Quantifying dopant ion distributions and intermixing, and correlating them with synthesis methods require suitable analytical techniques. Here, X-ray photoelectron spectroscopy depth-profiling with tender X-rays (2000–6000 eV), providing probe depths ideally matched to UCNP sizes, is used to measure the depth-dependent concentration ratios of Er3+ to Yb3+, [Er3+]/[Yb3+], in three types of UCNPs prepared using different reagents and synthesis methods. This is combined with data simulations and inductively coupled plasma-optical emission spectroscopy (ICP-OES) measurements of the lanthanide ion concentrations to construct models of the UCNPs’ dopant ion distributions. The UCNP sizes and architectures are chosen to demonstrate the potential of this approach. Core-only UCNPs synthesized with XCl3·6H2O precursors (β-phase) exhibit a homogeneous distribution of lanthanide ions, but a slightly surface-enhanced [Er3+]/[Yb3+] is observed for UCNPs prepared with trifluroacetate precursors (α-phase). Examination of Yb-core@Er-shell UCNPs reveals a co-doped, intermixed region between the single-doped core and shell. The impact of these different dopant ion distributions on the UCNP's optical properties is discussed to highlight their importance for UCNP functionality and the design of efficient UCNPs. KW - Shell KW - Nanomaterial KW - Nano KW - Upconversion nanoparticle KW - Lanthanide KW - Photoluminescence KW - Quantum yield KW - Photophysics KW - Excitation power density KW - Surface KW - Coating KW - Core-shell KW - XPS KW - Intermixing KW - HAXPES KW - Method PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-552075 DO - https://doi.org/10.1002/smll.202107976 SN - 1613-6813 SP - 1 EP - 13 PB - Wiley-VCH-Verlag CY - Weinheim, Germany AN - OPUS4-55207 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Climent Terol, Estela A1 - Biyikal, Mustafa A1 - Gröninger, Delia A1 - Weller, Michael G. A1 - Martínez Mánez, R. A1 - Rurack, Knut ED - Climent Terol, Estela T1 - Multiplexed Detection of Analytes on Single Test Strips with Antibody-Gated Indicator-Releasing Mesoporous Nanoparticles N2 - Rapid testing methods for the use directly at apointof need are expected to unfold their true potential especiallywhen offering adequate capabilities for the simultaneousmeasurement of multiple analytes of interest. Considering theunique modularity,high sensitivity,and selectivity of antibody-gated indicator delivery (gAID) systems,amultiplexed assayfor three small-molecule explosives (TATP, TNT,PETN) wasthus developed, allowing to detect the analytes simultaneouslywith asingle test strip at lower ppb concentrations in the liquidphase in < 5min using afluorescence reader or asmartphonefor readout. While the TNT and PETN systems were newlydeveloped here,all the three systems also tolerated harshermatrices than buffered aqueous model solutions.Besidesasingle-track strip,the outstanding modularity of the hybridbiosensor materials in combination with strip-patterningtechnologies allowed us to obtain amultichannel strip inastraightforwardmanner,offering comparable analyticalperformance while allowing to be tailored even more to theusersneed. KW - Multiplexing KW - Explosives detection KW - Gated materials KW - Fluorescence PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-518424 DO - https://doi.org/10.1002/anie.202009000 SN - 1433-7851 SN - 1521-3773 VL - 59 IS - 52 SP - 23862 EP - 23869 PB - Wiley-VCH CY - Weinheim AN - OPUS4-51842 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Climent Terol, Estela A1 - Rurack, Knut A1 - Hecht, Mandy T1 - Loading and Release of Charged and Neutral Fluorescent Dyes into and from Mesoporous Materials: A Key Role for Sensing Applications N2 - The aim of this study is to determine the efficiency of loading and release of several zwitterionic, neutral, anionic and cationic dyes into/from mesoporous nanoparticles to find the optimum loading and release conditions for their application in detection protocols. The loading is carried out for MCM-41 type silica supports suspended in phosphate-buffered saline (PBS) buffer (pH 7.4) or in acetonitrile, involving the dyes (rhodamine B chloride, rhodamine 101 chloride, rhodamine 101 perchlorate, rhodamine 101 inner salt, meso-(4-hydroxyphenyl)-boron–dipyrromethene (BODIPY), sulforhodamine B sodium salt and fluorescein 27). As a general trend, rhodamine-based dyes are loaded with higher efficiency, when compared with BODIPY and fluorescein dyes. Between the rhodamine-based dyes, their charge and the solvent in which the loading process is carried out play important roles for the amount of cargo that can be loaded into the materials. The delivery experiments carried out in PBS buffer at pH 7.4 reveal for all the materials that anionic dyes are more efficiently released compared to their neutral or cationic counterparts. The overall best performance is achieved with the negatively charged sulforhodamine B dye in acetonitrile. This material also shows a high delivery degree in PBS buffer. KW - Mesoporous materials KW - Charged dyes KW - Neutral dyes KW - Dye loading optimisation KW - Dye release PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-522596 UR - https://www.mdpi.com/2072-666X/12/3/249 DO - https://doi.org/10.3390/mi12030249 VL - 12 IS - 3 SP - 249 PB - MDPI AN - OPUS4-52259 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Climent Terol, Estela A1 - Wan, Wei A1 - Rurack, Knut T1 - Toward Label-Free Optical Multiplexing of Analytes in Indicator Release Lateral Flow Assays via Detection Zones Containing Tailored Capture Materials N2 - The use of macromolecules and materials immobilized in the detection zone of test strips for indicator capture and focusing in label-free lateral flow assays (LFAs) is described, with emphasis on its future use in low number multiplexing. Several materials such as polyelectrolytes, functionalized mesoporous silica micro- and nanoparticles, chemically modified cellulose or glass fibre (GF) membranes and molecularly imprinted polymer gels coated onto membranes were studied in model assays, before the most promising materials were combined with antibody-gated indicator delivering (gAID) sensor materials. Cellulose, nitrocellulose and GF membranes were used as supports and highly fluorescent dyes of different charge states as model indicators. Combination of the best performing capture materials with gAID systems made it possible to distinctly increase the sensitivity and reduce the measurement uncertainty in the LFA testing of pentaerythritol tetranitrate (PETN) in aqueous samples. In addition, dual-plexing of PETN and 2,4,6-trinitrotoluene (TNT) was realized on a single test strip containing two dedicated capture zones. KW - Rapid tests KW - Vor-Ort-Analytik KW - Multiplexing KW - Teststreifen KW - Molecularly imprinted polymers PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-557873 DO - https://doi.org/10.1002/anse.202100062 VL - 2 IS - 4 SP - 1 EP - 10 PB - Wiley-VCH CY - Weinheim AN - OPUS4-55787 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Coplen, T. B. A1 - Holden, N. E. A1 - Ding, T. A1 - Meijer, H. A. J. A1 - Vogl, Jochen A1 - Zhu, X. T1 - The Table of Standard Atomic Weights—An exercise in consensus N2 - The present Table of Standard Atomic Weights (TSAW) of the elements is perhaps one of the most familiar data sets in science. Unlike most parameters in physical science whose values and uncertainties are evaluated using the “Guide to the Expression of Uncertainty in Measurement” (GUM), the majority of standard atomic weight values and their uncertainties are consensus values, not GUM-evaluated values. The Commission on Isotopic Abundances and Atomic Weights of the International Union of Pure and Applied Chemistry (IUPAC) regularly evaluates the literature for new isotopic-abundance measurements that can lead to revised standard atomic-weight values, Ar(E) for element E. The Commission strives to provide utmost clarity in products it disseminates, namely the TSAW and the Table of Isotopic Compositions of the Elements (TICE). In 2016, the Commission recognized that a guideline recommending the expression of uncertainty listed in parentheses following the standard atomic-weight value, for example, Ar(Se) = 78.971(8), did not agree with the GUM, which suggests that this parenthetic notation be reserved to express standard uncertainty, not the expanded uncertainty used in the TSAW and TICE. In 2017, to eliminate this noncompliance with the GUM, a new format was adopted in which the uncertainty value is specified by the “±” symbol, for example, Ar(Se) = 78.971 ± 0.008. To clarify the definition of uncertainty, a new footnote has been added to the TSAW. This footnote emphasizes that an atomic-weight uncertainty is a consensus (decisional) uncertainty. Not only has the Commission shielded users of the TSAW and TICE from unreliable measurements that appear in the literature as a result of unduly small uncertainties, but the aim of IUPAC has been fulfilled by which any scientist, taking any natural sample from commerce or research, can expect the sample atomic weight to lie within Ar(E) ± its uncertainty almost all of the time. KW - Atomic weight KW - Standard atomic weight KW - Uncertainty PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-551299 DO - https://doi.org/10.1002/rcm.8864 SN - 1097-0231 VL - 36 IS - 15 SP - 1 EP - 15 PB - Wiley AN - OPUS4-55129 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Costa, Elena A1 - Climent Terol, Estela A1 - Gawlitza, Kornelia A1 - Wan, Wei A1 - Weller, Michael G. A1 - Rurack, Knut T1 - Optimization of analytical assay performance of antibody-gated indicator-releasing mesoporous silica particles N2 - Antibody-gated indicator delivery (gAID) systems based on mesoporous silica nano- and microparticle scaffolds are a promising class of materials for the sensitive chemical detection of small-molecule analytes in simple test formats such as lateral flow assays (LFAs) or microfluidic chips. Their architecture is reminiscent of drug delivery systems, only that reporter molecules instead of drugs are stored in the voids of a porous host particle. In addition, the pores are closed with macromolecular “caps” through a tailored “gatekeeping” recognition chemistry so that the caps are opened when an analyte has reacted with a “gatekeeper”. The subsequent uncapping leads to a release of a large number of indicator molecules, endowing the system with signal amplification features. Particular benefits of such systems are their modularity and adaptability. With the example of the immunochemical detection of type-I pyrethroids by fluorescent dye-releasing gAID systems, the influence of several tuning modes on the optimisation of such hybrid sensory materials is introduced here. In particular, different mesoporous silica supports (from nano- and microparticles to platelets and short fibres), different functionalisation routes and different loading sequences were assessed. The materials’ performances were evaluated by studying their temporal response behaviour and detection sensitivity, including the tightness of pore closure (through the amount of blank release in the absence of analyte) and the release kinetics. Our results indicate that the better the paratope-accommodating Fab region of the antibody “cap” fits into the host material's pore opening, the better the closing/opening mechanism can be controlled. Because such materials are well-suited for LFAs, performance assessment included a test-strip format besides conventional assays in suspension. In combination with dyes as indicators and smartphones for read-out, simple analytical tests for use by untrained personnel directly at a point-of-need such as an aeroplane cabin can be devised, allowing for sensitivities down to the μg kg−1 range in <5 min with case-required selectivities. KW - Antibody-gated indicator delivery KW - Lateral flow assay KW - SBA-15 KW - SBA-16 KW - Type-I pyrethroids KW - Phenothrin KW - Permethrin KW - Etofenprox KW - Amplification KW - Biosensors KW - Immunoassays KW - Mesoporous particles KW - Optical detection PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-517053 DO - https://doi.org/10.1039/d0tb00371a VL - 8 IS - 22 SP - 4950 EP - 4961 PB - Royal Society of Chemistry AN - OPUS4-51705 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - D'Agostino, Giancarlo A1 - Oelze, Marcus A1 - Vogl, Jochen A1 - Ghestem, Jean-Philippe A1 - Lafaurie, Nicolas A1 - Klein, Ole A1 - Pröfrock, Daniel A1 - Di Luzio, Marco A1 - Bergamaschi, Luigi A1 - Jaćimović, Radojko A1 - Oster, Caroline A1 - Irrgeher, Johanna A1 - Lancaster, Shaun T. A1 - Walch, Anna A1 - Röthke, Anita A1 - Michaliszyn, Lena A1 - Pramann, Axel A1 - Rienitz, Olaf A1 - Sara-Aho, Timo A1 - Cankur, Oktay A1 - Kutan, Derya A1 - Noireaux, Johanna T1 - Development and application of reference and routine analytical methods providing SI-traceable results for the determination of technology-critical elements in PCB from WEEE N2 - The recovery and reprocessing of technology-critical elements (TCE) present in printed circuit boards (PCB) from electrical and electronic waste is essential both for recycling valuable materials subject to supply risk and for reducing the environmental impact. Although the quantitative knowledge of TCE amounts in endof- life PCB plays a key role, there are neither matrix certified reference materials nor harmonized analytical methods available to establish the traceability of the results to the International System of Units. To fill these gaps, we developed and applied five reference analytical methods based on ICP-MS standard addition calibrations and INAA k0- and relative calibrations suitable to certify reference materials. In addition, we developed and tested six analytical methods based on more commonly used ICP-MS external standard calibrations to provide industry with routine analysis methods. Twenty TCE (Ag, Au, Co, Cu, Dy, Ga, Gd, Ge, In, La, Li, Nd, Ni, Pd, Pr, Pt, Rh, Sm, Ta and Ti) were selected as target analytes and a batch of powdered PCB was used as measurement material. An overall mutual agreement was observed among data collected by reference methods at a few percent relative uncertainty levels. Moreover, all but one of the methods developed for routine analysis demonstrated their suitability in industrial applications by producing data within ± 20% of the values established with reference methods. KW - Technology critical elements KW - Electronic waste KW - Printed circuit boards KW - Traceability KW - Uncertainty PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-612416 DO - https://doi.org/10.1039/d4ja00235k SN - 1364-5544 VL - 39 IS - 11 SP - 2809 EP - 2823 PB - Royal Society of Chemistry (RSC) AN - OPUS4-61241 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dariz, P. A1 - Schmid, Thomas T1 - Trace compounds in Early Medieval Egyptian blue carry information on provenance, manufacture, application, and ageing N2 - Only a few scientific evidences for the use of Egyptian blue in Early Medieval wall paintings in Central and Southern Europe have been reported so far. The monochrome blue fragment discussed here belongs to the second church building of St. Peter above Gratsch (South Tyrol, Northern Italy, fifth/ sixth century A.D.). Beyond cuprorivaite and carbon black (underpainting), 26 accessory minerals down to trace levels were detected by means of Raman microspectroscopy, providing unprecedented insights into the raw materials blend and conversion reactions during preparation, application, and ageing of the pigment. In conjunction with archaeological evidences for the manufacture of Egyptian blue in Cumae and Liternum and the concordant statements of the antique Roman writers Vitruvius and Pliny the Elder, natural impurities of the quartz sand speak for a pigment produced at the northern Phlegrean Fields (Campania, Southern Italy). Chalcocite (and chalcopyrite) suggest the use of a sulphidic copper ore, and water-insoluble salts a mixed-alkaline flux in the form of plant ash. Not fully reacted quartz crystals partly intergrown with cuprorivaite and only minimal traces of silicate glass portend solid-state reactions predominating the chemical reactions during synthesis, while the melting of the raw materials into glass most likely played a negligible role. KW - Egyptian blue KW - Raman microspectroscopy KW - Spectoscopic imaging KW - Cuprorivaite KW - Amorphous carbon PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-537591 DO - https://doi.org/10.1038/s41598-021-90759-6 VL - 11 SP - 1 EP - 12 PB - Nature Portfolio AN - OPUS4-53759 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dariz, P. A1 - Schmid, Thomas T1 - Raman focal point on Roman Egyptian blue elucidates disordered cuprorivaite, green glass phase and trace compounds N2 - The discussed comparative analyses of Roman Imperial pigment balls and fragmentary murals unearthed in the ancient cities of Aventicum and Augusta Raurica (Switzerland) by means of Raman microspectroscopy pertain to a predecessor study on trace compounds in Early Medieval Egyptian blue (St. Peter, Gratsch, South Tyrol, Northern Italy). The plethora of newly detected associated minerals of the raw materials surviving the synthesis procedure validate the use of quartz sand matching the composition of sediments transported by the Volturno river into the Gulf of Gaeta (Campania, Southern Italy) with a roasted sulphidic copper ore and a mixed-alkaline plant ash as fluxing agent. Thus, the results corroborate a monopolised pigment production site located in the northern Phlegrean Fields persisting over the first centuries A.D., this in line with statements of the antique Roman writers Vitruvius and Pliny the Elder and recent archaeological evidences. Beyond that, Raman spectra reveal through gradual peak shifts and changes of band width locally divergent process conditions and compositional inhomogeneities provoking crystal lattice disorder in the chromophoric cuprorivaite as well as the formation of a copper-bearing green glass phase, the latter probably in dependency of the concentration of alkali flux, notwithstanding that otherwise solid-state reactions predominate the synthesis. KW - Raman microspectroscopy KW - Egyptian blue KW - Cuprorivaite PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-559028 DO - https://doi.org/10.1038/s41598-022-19923-w SN - 2045-2322 VL - 12 IS - 1 SP - 1 EP - 12 PB - Nature Publishing Group CY - London AN - OPUS4-55902 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dariz, P. A1 - Wortmann, U. G. A1 - Vogl, Jochen A1 - Schmid, Thomas T1 - Beautiful Pietàs in South Tyrol (Northern Italy): local or imported works of art? N2 - The study, dedicated to Beautiful Pietàs conserved in South Tyrol (Northern Italy), aims to establish, for the first time, a connection between Austroalpine raw materials and the high-fired gypsum mortars constituting the Gothic figure groups in question. The origin and chronology of this stylistically and qualitatively differing ensemble have been subject of art historical debate for nearly a century. The discourse is dominated by three main hypotheses: itinerary of an Austrian artist versus itinerary of the work of art created in an artist’s workshop in Austria versus itinerary of the stylistic vocabulary via graphical or three-dimensional models. The comparison of the δ34S values and the 87Sr/86Sr ratios of the gypsum mortars and Austroalpine sulphate deposits (in a compilation of own reference samples and literature data) points to the exploitation of sediments in the Salzkammergut and possibly also in the evaporite district of the Eastern Calcareous Alps, thus evidencing the import of the sculptures and not the activities of local South Tyrolean or itinerant artists. Two geochronological units are distinguishable: The Pietà in the Church St. Martin in Göflan can be assigned to Upper Permian raw material, whereas the metrologically consistent sculptures in the Church of Our Lady of the Benedictine Abbey Marienberg and in the Chapel St. Ann in Mölten correlate with deposits of the Early Triassic (or the Lower-Middle Triassic transition). The medieval gypsum mortars also differ in their mineralogical characteristics, i.e. in their geologically related minor components, as in the first case, characterised by a significant proportion of primary anhydrite, natural carbonate impurities mainly consist of calcite (partly converted to lime-lump-like aggregates), whereas in the second group dolomite (or rather its hydration products after pyrometamorphic decomposition) predominates, accompanied by celestine, quartz and potassium feldspar. The Pietà in the Cathedral Maria Himmelfahrt in Bozen turned out to be made of Breitenbrunn calcareous sandstone (Leitha Mountains, Burgenland, Austria), which is why the sample is not considered in the geochemical analysis. KW - High-fired gypsum mortar KW - Sulphur isotope KW - Strontium isotope KW - Polarised light microscopy KW - Raman microspectroscopy PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-545610 DO - https://doi.org/10.1186/s40494-022-00678-6 SN - 2050-7445 VL - 10 IS - 1 SP - 1 EP - 17 PB - Springer Nature AN - OPUS4-54561 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - de Krom, I. A1 - Heikens, D. A1 - Horn, Wolfgang A1 - Wilke, Olaf A1 - Richter, Matthias A1 - Baldan, A. T1 - Metrological generation of SI-traceable gas-phase standards and reference materials for (semi-) volatile organic compounds N2 - EN 16516 sets specifications for the determination of emissions into indoor air from construction products. Reliable, accurate and International System of Unit (SI)-traceable measurement results of the emissions are the key to consumer protection. Such measurement results can be obtained by using metrologically traceable reference materials. Gas-phase standards of volatile organic compounds (VOCs) in air can be prepared by a variety of dynamic methods according to the ISO 6145 series. However, these methods are not always applicable for semi-VOCs (SVOCs) due to their high boiling point and low vapour pressure. Therefore, a novel dynamic gas mixture generation system has been developed. With this system gas-phase standards with trace level VOCs and SVOCs in air can be prepared between 10 nmol mol−1 and 1000 nmol mol−1. The VOCs and SVOCs in this study have normal boiling points ranging from 146 °C to 343 °C. Metrologically traceable reference materials of the gas-phase standard were obtained by sampling of the VOC gas-phase standard into Tenax TA® sorbent material in SilcoNert® coated stainless steel tubes. Accurately known masses between 10 ng and 1000 ng per VOC were sampled. These reference materials were used to validate the dynamic system. Furthermore, the storage and stability periods of the VOCs in the reference materials were determined as these are crucial characteristics to obtain accurate and SI-traceable reference materials. In a round robin test (RRT), the reference materials were used with the aim of demonstrating the feasibility of providing SI-traceable standard reference values for SVOCs for interlaboratory comparison purposes. Based on the results from the validation, the storage and stability studies and the RRT, gas-phase standards and reference materials of VOCs and SVOCs with relative expanded uncertainties between 5% and 12% (k = 2) have been developed. These reference standards can be used as calibrants, reference materials or quality control materials for the analysis of VOC emissions. KW - SVOC KW - Dynamic calibration gas mixtures KW - Reference materials KW - Indoor air KW - Thermal desorption PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-565978 DO - https://doi.org/10.1088/1361-6501/aca704 VL - 34 IS - 3 SP - 1 EP - 13 PB - IOP Publishing AN - OPUS4-56597 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Deumer, J. A1 - Andresen, Elina A1 - Gollwitzer, C. A1 - Schürmann, R. A1 - Resch-Genger, Ute T1 - Adding More Shape to Nanoscale Reference Materials-LiYF4:Yb,Tm Bipyramids as Standards for Sizing Methods and Particle Number Concentration N2 - The increasing industrial use of nanomaterials calls for the reliable characterization of their physicochemical key properties like size, size distribution, shape, and surface chemistry, and test and reference materials (RMs) with sizes and shapes, closely matching real-world nonspheric nano-objects. An efficient strategy to minimize efforts in producing nanoscale RMs (nanoRMs) for establishing, validating, and standardizing methods for characterizing nanomaterials are multimethod nanoRMs. Ideal candidates are lanthanide-based, multicolor luminescent, and chemically inert nanoparticles (NPs) like upconversion nanoparticles (UCNPs), which can be prepared in different sizes, shapes, and chemical composition with various surface coatings. This makes UCNPs interesting candidates as standards not only for sizing methods, but also for element-analytical methods like laser ablation-inductively coupled plasma mass spectrometry (LA-ICP-MS), quantitative bioimaging methods like X-ray fluorescence computed tomography (XFCT), and luminescence methods and correlative measurements. Here, we explore the potential of two monodisperse LiYF4:Yb,Tm bipyramids with peak-to-peak distances of (43 ± 2) nm and (29 ± 2) nm as size standards for small-angle X-ray scattering (SAXS) and tools for establishing and validating the sophisticated simulations required for the analysis of SAXS data derived from dispersions of nonspheric nano-objects. These SAXS studies are supplemented by two-dimensional (2D)-transmission electron microscopy measurements of the UCNP bipyramids. Additionally, the particle number concentration of cyclohexane dispersions of these UCNP bipyramids is determined by absolute SAXS measurements, complemented by gravimetry, thermogravimetric analysis (TGA), and inductively coupled plasma optical emission spectrometry (ICP-OES). This approach enables traceable particle number concentration measurements of ligand-capped nonspheric particles with unknown chemical composition. KW - Fluorescence KW - Upconversion nanoparticles KW - SAXS KW - Particle number concentration KW - Reference material KW - Traceability KW - Quality assurance KW - Quantum yield KW - Spectroscopy KW - Synthesis KW - Quantification KW - NanoRM KW - Nano KW - Particle KW - Bipyramid KW - Reference data KW - Simulation PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-617940 DO - https://doi.org/10.1021/acs.analchem.4c03641 SP - 1 EP - 8 PB - ACS Publications AN - OPUS4-61794 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dhamo, Lorena A1 - Carulli, F. A1 - Nickl, Philip A1 - Wegner, Karl David A1 - Hodoroaba, Vasile-Dan A1 - Würth, Christian A1 - Brovelli, S. A1 - Resch-Genger, Ute T1 - Efficient luminescent solar concentrators based on environmentally friendly Cd-free ternary AIS/ZnS quantum dots N2 - Luminescent solar concentrators (LSC) allow to obtain renewable energy from building integrated photovoltaic systems. As promising efficient and long-term stable LSC fluorophores semiconductor nanocrystals like Quantum dots (QDs) with size and composition tunable optoelectronic properties have recently emerged. The most popular II/VI or IV/VI semiconductor QDs contain, however, potentially hazardous cadmium or lead ions, which is a bottleneck for commercial applications. A simple aqueous based, microwaveassisted synthesis for environmentally friendly and highly emissive AgInS2/ ZnS QDs is developed using 3-mercaptopropionic acid (MPA) and glutathione (GSH) and their incorporation into polylaurylmethacrylate (PLMA) polymer slabs integrable in LSC devices (10.4 × 10.4 × 0.2 cm3, G = 12.98). With this simple approach, optical power efficiencies (OPE) of 3.8% and 3.6% and optical quantum efficiencies (OQE) of 24.1% and 27.4% are obtained, which are among the highest values yet reported. KW - Solar energy KW - Solar concentrator KW - Quantum dots KW - Advanced material KW - Quantum yield PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-529735 DO - https://doi.org/10.1002/adom.202100587 SN - 2195-1071 SN - 0935-9648 VL - 9 IS - 17 SP - 1 EP - 8 PB - Wiley-VCH CY - Weinheim AN - OPUS4-52973 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dhamo, Lorena A1 - Wegner, Karl David A1 - Würth, Christian A1 - Häusler, I. A1 - Hodoroaba, Vasile-Dan A1 - Resch-Genger, Ute T1 - Assessing the influence of microwave-assisted synthesis parameters and stabilizing ligands on the optical properties of AIS/ZnS quantum dots N2 - Luminescent semiconductor quantum dots (QDs) are frequently used in the life and material sciences as reporter for bioimaging studies and as active components in devices such as displays, light-emitting diodes, solar cells, and sensors. Increasing concerns regarding the use of toxic elements like cadmium and lead, and hazardous organic solvents during QD synthesis have meanwhile triggered the search for heavy-metal free QDs using green chemistry syntheses methods. Interesting candidates are ternary AgInS2 (AIS) QDs that exhibit broad photoluminescence (PL) bands, large effective Stokes shifts, high PL quantum yields (PL QYs), and long PL lifetimes, which are particularly beneficial for applications such as bioimaging, white light-emitting diodes, and solar concentrators. In addition, these nanomaterials can be prepared in high quality with a microwave-assisted (MW) synthesis in aqueous solution. The homogeneous heat diffusion and instant temperature rise of the MW synthesis enables a better control of QD nucleation and growth and thus increases the batch-to-batch reproducibility. In this study, we systematically explored the MW synthesis of AIS/ZnS QDs by varying parameters such as the order of reagent addition, precursor concentration, and type of stabilizing thiol ligand, and assessed their influence on the optical properties of the resulting AIS/ZnS QDs. Under optimized synthesis conditions, water-soluble AIS/ZnS QDs with a PL QY of 65% and excellent colloidal and long-term stability could be reproducible prepared. KW - Quantum dots KW - Microwave-assisted synthesis KW - AgInS KW - Aqueous synthesis PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-567091 DO - https://doi.org/10.1038/s41598-022-25498-3 SN - 2045-2322 VL - 12 IS - 1 SP - 1 EP - 11 PB - Nature Publishing Group CY - London AN - OPUS4-56709 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dorgerloh, Ute A1 - Becker, Roland A1 - Freeling, Finnian A1 - Scheurer, Marco A1 - Gökçe, Emine A1 - Strack, Katrin A1 - Sommerfeld, Thomas A1 - Sauer, Andreas A1 - Schneider, Jonas A1 - Härtel, Christoph A1 - Valkov, Vassil A1 - Moser, Lukas A1 - Geiß, Sabine A1 - Junginger, Sabine A1 - Schlittenbauer, Linda A1 - Suess, Elke A1 - Ruth, Katinka T1 - Standardising the quantification of trifluoroacetic acid in water: Interlaboratory validation trial using liquid chromatography-mass spectrometric detection (LC–MS/MS) N2 - The concentration of trifluoroacetic acid in surface and groundwaters and drinking water is subject of increasing concern. Since there is no standardised procedure available, German standardisation body DIN has initiated the first draft standard using liquid chromatography with tandem mass spectrometry (LC–MS/MS) after direct injection for the concentration range between ≥ 0.1 and 3 µg/L. Herein, the interlaboratory comparison as final validation step involving 12 expert laboratories from Germany and Switzerland is described. Two groundwaters, two surface waters, a drinking water, a rainwater, and two fortified groundwater samples displayed relative repeatability standard deviations between 3 and 7% and relative reproducibility standard deviation between 6 and 20% and were included in the draft standard DIN 38407-53. KW - TFA Trifluoroacetic acid KW - LC/MS-MS KW - Validation trial PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-632376 DO - https://doi.org/10.1007/s00769-025-01640-2 SN - 0949-1775 SP - 1 EP - 4 PB - Springer CY - Berlin AN - OPUS4-63237 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dorgerloh, Ute A1 - Becker, Roland A1 - Riedel, Juliane A1 - Hofmann, Andrea T1 - Comparison of gas- and liquid chromatography-mass spectrometry for trace analysis of anilines in groundwater N2 - Three chromatographic procedures were investigated regarding their potential for the quantification of aniline and 19 of its methylated and chlorinated derivatives in groundwater. These methods were based on liquid-liquid-extraction in combination with gas chromatography and single quadrupole mass spectrometry (GC/MS) according to German standard DIN 38407-16:1999 and its extension using tandem mass spectrometry (GC/MS-MS), both following liquid-liquid extraction, and as third alternative the direct injection of the water sample into a liquid chromatograph coupled to tandem mass spectrometry (LC/MS-MS). Results were compared using fortified water and real-world contaminated groundwater used in an interlaboratory comparison. It could be shown that GC/MS and GC/MS-MS yielded results deviating less than 10% from each other while all three procedure displayed quantification results deviating less than 15% from the intercomparison reference values in case of each analyte in the concentration range between 1 and 45 µg L-1. Though GC/MS-MS displays a ten-fold higher sensitivity than single quadrupole GC/MS, the precision of both methods in the concentration range was similar. LC/MS-MS has the advantage of no further sample preparation due to the direct injection and leads for methylanilines and meta-, para- substituted chloroanilines to results sufficiently equivalent to the standardised GC/MS method. However, LC/MS-MS is not suitable for ortho-chloroaniline derivates due to significantly lower ion yields than meta- and para-substituted chloroanilines. KW - Interlaboratory comparison KW - Aniline KW - Chloroanilines KW - Methylanilines KW - Groundwater KW - GC/MS KW - GC/MS-MS KW - LC/MS-MS PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-535793 DO - https://doi.org/10.1080/03067319.2021.1987423 VL - 103 IS - 19 SP - 8465 EP - 8477 PB - Taylor & Francis CY - London AN - OPUS4-53579 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Duarte Bernardino, Carolina A1 - Lee, Mihyun A1 - Ren, Qun A1 - Ruehle, Bastian T1 - Facile Spray-Coating of Antimicrobial Silica Nanoparticles for High-Touch Surface Protection N2 - The rising threat from infectious pathogens poses an ever-growing challenge. Metal-based nanomaterials have gained a great deal of attention as active components in antimicrobial coatings. Here, we report on the development of readily deployable, sprayable antimicrobial surface coatings for high-touch stainless steel surfaces that are ubiquitous in many healthcare facilities to combat the spread of pathogens. We synthesized mesoporous silica nanoparticles (MSNs) with different surface functional groups, namely, amine (MSN-NH2), carboxy (MSN-COOH), and thiol groups (MSN-SH). These were chosen specifically due to their high affinity to copper and silver ions, which were used as antimicrobial payloads and could be incorporated into the mesoporous structure through favorable host−guest interactions, allowing us to find the most favorable combinations to achieve antimicrobial efficacy against various microbes on dry or semidry high-touch surfaces. The antimicrobial MSNs were firmly immobilized on stainless steel through a simple two-step spray-coating process. First, the stainless steel surfaces are primed with sprayable polyelectrolyte solutions acting as adhesion layers, and then, the loaded nanoparticle dispersions are spray-coated on top. The employed polyelectrolytes were selected and functionalized specifically to adhere well to stainless steel substrates while at the same time being complementary to the MSN surface groups to enhance the adhesion, wettability, homogeneity, and stability of the coatings. The antimicrobial properties of the nanoparticle suspension and the coatings were tested against three commonly found pathogenic bacteria, Staphylococcus aureus, Pseudomonas aeruginosa, and Escherichia coli, as well as a fungal pathogen, Candida albicans. Especially MSN-SH loaded with silver ions showed excellent antimicrobial efficacy against all tested pathogens under application-relevant, (semi)dry conditions. The findings obtained here facilitate our understanding of the correlation between the surface properties, payloads, and antimicrobial activity and show a new pathway toward simple and easily deployable solutions to combat the spread of pathogens with the help of sprayable antimicrobial surface coatings. KW - Mesoporous silica nanoparticles KW - Thin films KW - Antimicrobial coatings KW - Spray-coating KW - Infectious diseases KW - Pathogen transmission KW - High-touch surfaces PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-626269 DO - https://doi.org/10.1021/acsami.4c18916 SN - 1944-8252 SP - 1 EP - 13 PB - ACS Publications CY - Washington, DC AN - OPUS4-62626 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - GEN A1 - Döring, Sarah T1 - Corundum Particles as Trypsin Carrier for Efficient Protein Digestion N2 - This dataset contains raw LC–MS/MS files of trypsin-digested NISTmAb acquired on a SCIEX TripleTOF 6600 mass spectrometer in DIA (SWATH) mode for antibody quantification. In addition, it includes MALDI-TOF MS peptide mass fingerprints of trypsin-digested Herceptin as well as reference spectra that can be used for antibody identification using the open-source software ABID 2.0 (https://bam.de/ABID). The data were generated within a study demonstrating the applicability of corundum-immobilized trypsin for antibody digestion and its suitability for peptide-based LC–MS/MS quantification and MALDI-TOF MS fingerprinting–based antibody identification. KW - NISTmAb KW - Herceptin KW - MALDI-TOF MS peptide mass fingerprint KW - ABID 2.0 PY - 2025 DO - https://doi.org/10.5281/zenodo.17416536 PB - Zenodo CY - Geneva AN - OPUS4-65365 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Döring, Sarah A1 - Konthur, Zoltán A1 - Weller, Michael G. A1 - Jaeger, Carsten A1 - Reinders, Yvonne T1 - Challenges and Insights in Absolute Quantification of Recombinant Therapeutic Antibodies by Mass Spectrometry: An Introductory Review N2 - This review describes mass spectrometry (MS)-based approaches for the absolute quantification of therapeutic monoclonal antibodies (mAbs), focusing on technical challenges in sample treatment and calibration. Therapeutic mAbs are crucial for treating cancer and inflammatory, infectious, and autoimmune diseases. We trace their development from hybridoma technology and the first murine mAbs in 1975 to today’s chimeric and fully human mAbs. With increasing commercial relevance, the absolute quantification of mAbs, traceable to an international standard system of units (SI units), has attracted attention from science, industry, and national metrology institutes (NMIs). Quantification of proteotypic peptides after enzymatic digestion using high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) has emerged as the most viable strategy, though methods targeting intact mAbs are still being explored. We review peptide-based quantification, focusing on critical experimental steps like denaturation, reduction, alkylation, choice of digestion enzyme, and selection of signature peptides. Challenges in amino acid analysis (AAA) for quantifying pure mAbs and peptide calibrators, along with software tools for targeted MS data analysis, are also discussed. Short explanations within each chapter provide newcomers with an overview of the field’s challenges. We conclude that, despite recent progress, further efforts are needed to overcome the many technical hurdles along the quantification workflow and discuss the prospects of developing standardized protocols and certified reference materials (CRMs) for this goal. We also suggest future applications of newer technologies for absolute mAb quantification. KW - Monoclonal antibody KW - Therapeutic antibodies KW - Mass spectrometry KW - Liquid chromatography KW - Absolute quantification KW - Metrology KW - Traceability KW - Certified reference material PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-623707 DO - https://doi.org/10.3390/antib14010003 SN - 2073-4468 VL - 14 IS - 1 SP - 1 EP - 26 PB - MDPI CY - Basel, Schweiz AN - OPUS4-62370 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Döring, Sarah A1 - Tscheuschner, Georg A1 - Flemig, Sabine A1 - Weller, Michael G. A1 - Konthur, Zoltán T1 - Cost-Effective Method for Full-Length Sequencing of Monoclonal Antibodies from Hybridoma Cells N2 - Background: Monoclonal antibodies play an important role in therapeutic and analytical applications. For recombinant expression, the coding sequences of the variable regions of the heavy and light chains are required. In addition, cloning antibody sequences, including constant regions, reduces the impact of hybridoma cell loss and ensures preservation of the naturally occurring full antibody sequence. Method: We combined amplification of IgG antibody variable regions from hybridoma mRNA with an advanced method for fulllength cloning of monoclonal antibodies in a simple two-step workflow. Following Sanger sequencing and evaluation of consensus sequences, the best matching variable, diversity, and joining (V-(D-)J) gene segments were identified according to identity scores from IgBLAST reference sequences. Simultaneously, the mouse IgG subclass was determined at the DNA level based on isotype-specific sequence patterns in the CH1 domain. Knowing the DNA sequence of V-(D-)J recombination responsible for the complementary determining region 3 (CDR 3), variable region-specific primers were designed and used to amplify the corresponding antibody constant regions. Results: To verify the approach, we applied it to the hybridoma clone BAM-CCMV-29-81 and obtained identical full-length antibody sequences as with RNA Illumina sequencing. Further validation at the protein level using an established MALDI-TOF MS-fingerprinting protocol showed that five out of six genetically encoded CDR domains of the monoclonal antibody BAM-CCMV-29-81 could be efficiently correlated. Conclusion: This simple, streamlined method enables the cost-effective determination of the full-length sequence of monoclonal antibodies from hybridoma cell lines, with the added benefit of obtaining the DNA sequence of the antibody ready for recombinant expression. KW - Full-length antibody sequencing KW - Hybridoma cell loss KW - MALDI-TOF MS KW - Immunoglobulin isotyping KW - RNA Illumina sequencing PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-639599 DO - https://doi.org/10.3390/antib14030072 SN - 2073-4468 VL - 14 IS - 3 SP - 1 EP - 17 PB - MDPI CY - Basel AN - OPUS4-63959 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ebel, Kenny A1 - Bald, Ilko T1 - Length and Energy Dependence of Low-Energy Electron-Induced Strand Breaks in Poly(A) DNA N2 - The DNA in living cells can be effectively damaged by high-energy radiation, which can lead to cell death. Through the ionization of water molecules, highly reactive secondary species such as low-energy electrons (LEEs) with the most probable energy around 10 eV are generated, which are able to induce DNA strand breaks via dissociative electron attachment. Absolute DNA strand break cross sections of specific DNA sequences can be efficiently determined using DNA origami nanostructures as platforms exposing the target sequences towards LEEs. In this paper, we systematically study the effect of the oligonucleotide length on the strand break cross section at various irradiation energies. The present work focuses on poly-adenine sequences (d(A4), d(A8), d(A12), d(A16), and d(A20)) irradiated with 5.0, 7.0, 8.4, and 10 eV electrons. Independent of the DNA length, the strand break cross section shows a maximum around 7.0 eV electron energy for all investigated oligonucleotides confirming that strand breakage occurs through the initial formation of negative ion resonances. When going from d(A4) to d(A16), the strand break cross section increases with oligonucleotide length, but only at 7.0 and 8.4 eV, i.e., close to the maximum of the negative ion resonance, the increase in the strand break cross section with the length is similar to the increase of an estimated geometrical cross section. For d(A20), a markedly lower DNA strand break cross section is observed for all electron energies, which is tentatively ascribed to a conformational change of the dA20 sequence. The results indicate that, although there is a general length dependence of strand break cross sections, individual nucleotides do not contribute independently of the absolute strand break cross section of the whole DNA strand. The absolute quantification of sequence specific strand breaks will help develop a more accurate molecular level understanding of radiation induced DNA damage, which can then be used for optimized risk estimates in cancer radiation therapy. KW - DNA origami KW - DNA radiation damage KW - DNA strand breaks KW - Low-energy electrons KW - Sequence dependence PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-503563 DO - https://doi.org/10.3390/ijms21010111 VL - 21 IS - 1 SP - 1 EP - 11 PB - MDPI CY - Basel, Switzerland AN - OPUS4-50356 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ecke, Alexander A1 - Bell, Jérémy A1 - Schneider, Rudolf T1 - A three-dimensional microfluidic flow cell and system integration for improved electrochemical substrate detection in HRP/TMB-based immunoassays N2 - Immunoassays, based on the recognition and capture of analytes by highly selective antibodies, are now used extensively in all areas of diagnostics, but the challenge is to further integrate them into online sensors. To improve the transition from laboratory immunoassays to immunosensors, we have developed a complete flow system, based on a microfluidic core flow cell to enable automated detection of one of the most commonly used immunoassay substrates, TMB, by chronoamperometry. The architecture and fluidic optimisation of the system showed that a specially designed 3D flow cell allows higher flow rates (500 μL min−1) than a standard enlarged microfluidic channel (50 μL min−1) resulting in a significantly shorter detection time of 30 seconds per sample and making the system more robust against interferences due to bubble formation in the chip. The electrochemical measurements showed an improved signal-to-noise ratio (SNR) and thus higher sensitivity for a model immunoassay for diclofenac (SNR = 59), compared to the analytical performance of a conventional laboratory microplate-based assay with optical detection (SNR = 19). In general, this system facilitates the conversion of any conventional immunoassay into an immunosensor with automatic and continuous detection. KW - Microfluidic KW - Immunoassay KW - Electrochemical KW - Mikrofluidik KW - Immunassay KW - Elektrochemie PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-580159 DO - https://doi.org/10.1039/d3sd00095h VL - 2 SP - 887 EP - 892 PB - Royal Society of Chemistry CY - London, United Kingdom AN - OPUS4-58015 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ecke, Alexander A1 - Schneider, Rudolf T1 - Pitfalls in the Immunochemical Determination of β-Lactam Antibiotics in Water N2 - Contamination of waters with pharmaceuticals is an alarming problem as it may support the evolution of antimicrobial resistance. Therefore, fast and cost-effective analytical methods for potential on-site analysis are desired in order to control the water quality and assure the safety of its use as a source of drinking water. Antibody-based methods, such as the enzyme-linked immunosorbent assay (ELISA), can be helpful in this regard but can also have certain pitfalls in store, depending on the analyte. As shown here for the class of β-lactam antibiotics, hydrolysis of the β-lactam ring is a key factor in the immunochemical analysis as it influences antibody recognition. With the antibody used in this study, the limit of detection (LOD) in the immunoassay could be significantly reduced by hydrolysis for the five tested penicillins, with the lowest LOD for carbenicillin (0.2 nmol/L) and the greatest impact on penicillins G and V (reduction by 85%). In addition to enhanced quantification, our strategy also provides access to information about the degree of hydrolysis in water samples as shown for the most abundant penicillin amoxicillin. KW - ELISA KW - Immunoassay KW - β-Lactam KW - Amoxicillin KW - Hydrolysis PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-522832 DO - https://doi.org/10.3390/antibiotics10030298 SN - 2079-6382 VL - 10 IS - 3 SP - 298 PB - MDPI CY - Basel, CH AN - OPUS4-52283 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Ecke, Alexander A1 - Westphalen, Tanja A1 - Hornung, J. A1 - Voetz, M. A1 - Schneider, Rudolf T1 - A rapid magnetic bead-based immunoassay for sensitive determination of diclofenac N2 - Increasing contamination of environmental waters with pharmaceuticals represents an emerging threat for the drinking water quality and safety. In this regard, fast and reliable analytical methods are required to allow quick countermeasures in case of contamination. Here, we report the development of a magnetic bead-based immunoassay (MBBA) for the fast and cost-effective determination of the analgesic diclofenac (DCF) in water samples, based on diclofenac-coupled magnetic beads and a robust monoclonal anti-DCF antibody. A novel synthetic strategy for preparation of the beads resulted in an assay that enabled for the determination of diclofenac with a significantly lower limit of detection (400 ng/L) than the respective enzyme-linked immunosorbent assay (ELISA). With shorter incubation times and only one manual washing step required, the assay demands for remarkably shorter time to result (< 45 min) and less equipment than ELISA. Evaluation of assay precision and accuracy with a series of spiked water samples yielded results with low to moderate intra- and inter-assay variations and in good agreement with LC–MS/MS reference analysis. The assay principle can be transferred to other, e.g., microfluidic, formats, as well as applied to other analytes and may replace ELISA as the standard immunochemical method. KW - Immunoassay KW - Magnetic beads KW - Diclofenac KW - Water analysis KW - LC-MS/MS PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-542346 DO - https://doi.org/10.1007/s00216-021-03778-7 SN - 1618-2650 VL - 414 SP - 1563 EP - 1573 PB - Springer CY - Heidelberg AN - OPUS4-54234 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Eifert, T. A1 - Eisen, K. A1 - Maiwald, Michael A1 - Herwig, C. T1 - Current and future requirements to industrial analytical infrastructure—part 2: smart sensors N2 - Complex processes meet and need Industry 4.0 capabilities. Shorter product cycles, flexible production needs, and direct assessment of product quality attributes and raw material attributes call for an increased need of new process analytical technologies (PAT) concepts. While individual PAT tools may be available since decades, we need holistic concepts to fulfill above industrial needs. In this series of two contributions, we want to present a combined view on the future of PAT (process analytical technology), which is projected in smart labs (Part 1) and smart sensors (Part 2). Part 2 of this feature article series describes the future functionality as well as the ingredients of a smart sensor aiming to eventually fuel full PAT functionality. The smart sensor consists of (i) chemical and process information in the physical twin by smart field devices, by measuring multiple components, and is fully connected in the IIoT 4.0 environment. In addition, (ii) it includes process intelligence in the digital twin, as to being able to generate knowledge from multi-sensor and multi-dimensional data. The cyber-physical system (CPS) combines both elements mentioned above and allows the smart sensor to be self-calibrating and self-optimizing. It maintains its operation autonomously. Furthermore, it allows—as central PAT enabler—a flexible but also target-oriented predictive control strategy and efficient process development and can compensate variations of the process and raw material attributes. Future cyber-physical production systems—like smart sensors—consist of the fusion of two main pillars, the physical and the digital twins. We discuss the individual elements of both pillars, such as connectivity, and chemical analytics on the one hand as well as hybrid models and knowledge workflows on the other. Finally, we discuss its integration needs in a CPS in order to allow is versatile deployment in efficient process development and advanced optimum predictive process control. KW - Smart sensors KW - Industry 4.0 KW - Digital twins KW - Process intelligence KW - Process analytical technology KW - Physical twin KW - Cyber-physical system PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-503980 DO - https://doi.org/10.1007/s00216-020-02421-1 SN - 1618-2642 VL - 412 IS - 9 SP - 2037 EP - 2045 PB - Springer CY - Berlin Heidelberg AN - OPUS4-50398 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Eisen, K A1 - Eifert, T A1 - Herwig, C A1 - Maiwald, Michael T1 - Current and future requirements to industrial analytical infrastructure—part 1: process analytical laboratories N2 - The competitiveness of the chemical and pharmaceutical industry is based on ensuring the required product quality while making optimum use of plants, raw materials, and energy. In this context, effective process control using reliable chemical process analytics secures global competitiveness. The setup of those control strategies often originate in process development but need to be transferable along the whole product life cycle. In this series of two contributions, we want to present a combined view on the future of PAT (process analytical technology), which is projected in smart labs (part 1) and smart sensors (part 2). In laboratories and pilot plants, offline chemical analytical methods are frequently used, where inline methods are also used in production. Here, a transferability from process development to the process in operation would be desirable. This can be obtained by establishing PAT methods for production already during process development or scale-up. However, the current PAT (Bakeev 2005, Org Process Res 19:3–62; Simon et al. 2015, Org Process Res Dev 19:3–62) must become more flexible and smarter. This can be achieved by introducing digitalization-based knowledge management, so that knowledge from product development enables and accelerates the integration of PAT. Conversely, knowledge from the production process will also contribute to product and process development. This contribution describes the future role of the laboratory and develops requirements therefrom. In part 2, we examine the future functionality as well as the ingredients of a smart sensor aiming to eventually fuel full PAT functionality—also within process development or scale-up facilities (Eifert et al. 2020, Anal Bioanal Chem). KW - Smart test laboratories KW - Laboratory 4.0 KW - Sustainable Production KW - Industry 4.0 PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-504020 DO - https://doi.org/10.1007/s00216-020-02420-2 SN - 1618-2642 VL - 412 IS - 9 SP - 2027 EP - 2035 PB - Springer CY - Berlin Heidelberg AN - OPUS4-50402 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - El-Dahshan, O. A1 - Deniaud, A. A1 - Ling, W. L. A1 - Wegner, Karl David A1 - Proux, O. A1 - Veronesi, G. A1 - Reiss, P. T1 - Hydrothermal microwave synthesis of water soluble NIR-II emitting Ag2S quantum dots N2 - Hydrothermal-based synthetic methods of quantum dots allow for the exploration of reaction parameters normally inaccessible to typical aqueous-based batch reactions, such as elevated reaction temperatures (>100 °C) and reaction pressures above atmospheric pressure. Coupled with microwave heating, new instantaneously bio-compatible quantum dots (QDs) with enhanced opitcal properties can be yielded. As of today, aqueous-based synthetic methods often lag behind their organic analogues in terms of the photophysical properties of the QDs obtained and the ease of modulation of both the emission wavelength and crystallite size. Using a novel microwave-assisted hydrothermal approach, the synthesis of silver sulphide (Ag2S) QDs exhibiting NIR emission spanning the biological transparency windows via modulation of the reaction parameters has been developed. The intrinsic link between their optical and structural properties is explored via laboratory and synchrotron-based structural analysis techniques. Their toxicity towards a hepatic cell line was assessed, and related back to their structure and size. Overall this work aims to not only further develop the repertoire of synthetic methods for the synthesis of Ag2S QDs, but also paves the way for the development of safer QDs suitable for future clinical applications. KW - Quantum dots KW - Microwave synthesis KW - Quality assurance KW - NIR-II emission KW - PL quantum yield KW - Ag2S PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-634825 DO - https://doi.org/10.1039/d5nr00052a SN - 2040-3372 VL - 17 IS - 24 SP - 14637 EP - 14646 PB - RSC AN - OPUS4-63482 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Epping, Ruben A1 - Bliesener, Lilly A1 - Weiss, Tilman A1 - Koch, Matthias T1 - Marker Substances in the Aroma of Truffles N2 - The aim of this study was to identify specific truffle marker substances within the truffle aroma. The aroma profile of different truffle species was analyzed using static headspace sampling with gas chromatography mass spectrometry analysis (SHS/GC-MS). Possible marker substances were identified, taking the additional literature into account. The selected marker substances were tested in an experiment with 19 truffle dogs. The hypothesis “If trained truffle dogs recognize the substances as supposed truffles in the context of an experiment, they can be regarded as specific” was made. As it would be nearly impossible to investigate every other possible emitter of the same compounds to determine their specificity, this hypothesis was a reasonable approximation. We were interested in the question of what it is the dogs actually search for on a chemical level and whether we can link their ability to find truffles to one or more specific marker substances. The results of the dog experiment are not as unambiguous as could have been expected based on the SHS/GC-MS measurements. Presumably, the truffle aroma is mainly characterized and perceived by dogs by dimethyl sulfide and dimethyl disulfide. However, as dogs are living beings and not analytical instruments, it seems unavoidable that one must live with some degree of uncertainty regarding these results. KW - Truffle KW - Volatile organic compounds; KW - Gas chromatography KW - Mass spectrometry KW - Canine olfactometry PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-556116 DO - https://doi.org/10.3390/molecules27165169 SN - 1420-3049 VL - 27 IS - 16 SP - 1 EP - 19 PB - MDPI CY - Basel AN - OPUS4-55611 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Epping, Ruben A1 - Falkenhagen, Jana A1 - Panne, Ulrich A1 - Hiller, W. A1 - Gruendling, T. A1 - Staal, B. A1 - Lang, C. A1 - Lamprou, A. T1 - Simultaneous characterization of poly(acrylic acid) andpolysaccharide polymers and copolymers N2 - Copolymer products that result from grafting acrylic acid and other hydrophilicmonomers onto polysaccharides have recently gained significant interest in researchand industry. Originating from renewable sources, these biodegradable, low toxicity,and polar copolymer products exhibit potential to replace polymers from fossil sourcesin several applications and industries. The methods usually employed to character-ize these copolymers are, however, quite limited, especially for the measurement ofbulk properties. With more sophisticated applications, for example, in pharmaceu-tics requiring a more detailed analysis of the chemical structure, we describe a newapproach for this kind of complex polymers. Our approach utilizes chromatographyin combination with several detection methods to separate and characterize reactionproducts of the copolymerization of acrylic acid and chemically hydrolyzed starch.These samples consisted of a mixture of homopolymer poly (acrylic acid), homopoly-mer hydrolyzed starch, and – in a lower amount – the formed copolymers. Several chro-matographic methods exist that are capable of characterizing either poly (acrylic acid)or hydrolyzed starch. In contrast, our approach offers simultaneous characterization ofboth polymers. The combination of LC and UV/RI offered insight into the compositionand copolymer content of the samples. Size exclusion chromatography experimentsrevealed the molar mass distribution of homopolymers and copolymers. FTIR inves-tigations confirmed the formation of copolymers while ESI-MS gave more details onthe end groups of hydrolyzed starches and poly (acrylic acids). Evidence of copolymerstructures was obtained through NMR measurements. Finally, two-dimensional chro-matography led to the separation of the copolymers from both homopolymers as wellas the additional separation of sodium clusters. The methods described in this work area powerful toolset to characterize copolymerization products of hydrolyzed starch andpoly(acrylic acid). Together, our approach successfully correlates the physicochemicalproperties of such complex mixtures with their actual composition. KW - 2D chromatography KW - LC-MS KW - SEC KW - Renewable copolymers KW - Grafting PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-508873 DO - https://doi.org/10.1002/ansa.202000044 SP - 1 EP - 12 PB - Wiley-VCH Verlag-GmbH&Co. KGaA CY - Weinheim AN - OPUS4-50887 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Epping, Ruben A1 - Koch, Matthias T1 - On-Site Detection of Volatile Organic Compounds (VOCs) N2 - Volatile organic compounds (VOCs) are of interest in many different fields. Among them are food and fragrance analysis, environmental and atmospheric research, industrial applications, security or medical and life science. In the past, the characterization of these compounds was mostly performed via sample collection and off-site analysis with gas chromatography coupled to mass spectrometry (GC-MS) as the gold standard. While powerful, this method also has several drawbacks such as being slow, expensive, and demanding on the user. For decades, intense research has been dedicated to find methods for fast VOC analysis on-site with time and spatial resolution. We present the working principles of the most important, utilized, and researched technologies for this purpose and highlight important publications from the last five years. In this overview, non-selective gas sensors, electronic noses, spectroscopic methods, miniaturized gas chromatography, ion mobility spectrometry and direct injection mass spectrometry are covered. The advantages and limitations of the different methods are compared. Finally, we give our outlook into the future progression of this field of research. KW - Volatile organic compounds KW - On-site detection KW - Mobile analytics KW - Sensors PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-570885 DO - https://doi.org/10.3390/molecules28041598 VL - 28 IS - 4 SP - 1 EP - 19 PB - MDPI CY - Basel, Switzerland AN - OPUS4-57088 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Epping, Ruben A1 - Lisec, Jan A1 - Koch, Matthias T1 - Changes in Black Truffle (Tuber melanosporum) Aroma during Storage under Different Conditions N2 - The enticing aroma of truffles is a key factor for their culinary value. Although all truffle species tend to be pricy, the most intensely aromatic species are the most sought after. Research into the aroma of truffles encompasses various disciplines including chemistry, biology, and sensory science. This study focusses on the chemical composition of the aroma of black truffles (Tuber melanosporum) and the changes occurring under different storage conditions. For this, truffle samples were stored under different treatments, at different temperatures, and measured over a total storage time of 12 days. Measurements of the truffle aroma profiles were taken with SPME/GC–MS at regular intervals. To handle the ample data collected, a systematic approach utilizing multivariate data analysis techniques was taken. This approach led to a vast amount of data which we made publicly available for future exploration. Results reveal the complexity of aroma changes, with 695 compounds identified, highlighting the need for a comprehensive understanding. Principal component analyses offer initial insights into truffle composition, while individual compounds may serve as markers for age (formic acid, 1-methylpropyl ester), freshness (2-Methyl-1-propanal; 1-(methylthio)-propane), freezing (tetrahydrofuran), salt treatment (1-chloropentane), or heat exposure (4-hydroxy-3-methyl-2-butanone). This research suggests that heat treatment or salt contact significantly affects truffle aroma, while freezing and cutting have less pronounced effects in comparison. The enrichment of compounds showing significant changes during storage was investigated with a metabolomic pathway analysis. The involvement of some of the enriched compounds on the pyruvate/glycolysis and sulfur pathways was shown. KW - Mass Spectrometry KW - Metabolomics KW - Tuber melanosporum KW - Truffle Aroma PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-601731 DO - https://doi.org/10.3390/jof10050354 VL - 10 IS - 5 SP - 1 EP - 22 PB - MDPI AN - OPUS4-60173 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Erler, A. A1 - Riebe, D. A1 - Beitz, T. A1 - Löhmannsröben, H.-G. A1 - Leenen, M. A1 - Pätzold, S. A1 - Ostermann, Markus A1 - Wójcik, M. T1 - Mobile Laser-Induced Breakdown Spectroscopy for Future Application in Precision Agriculture—A Case Study N2 - In precision agriculture, the estimation of soil parameters via sensors and the creation of nutrient maps are a prerequisite for farmers to take targeted measures such as spatially resolved fertilization. In this work, 68 soil samples uniformly distributed over a field near Bonn are investigated using laser-induced breakdown spectroscopy (LIBS). These investigations include the determination of the total contents of macro- and micronutrients as well as further soil parameters such as soil pH, soil organic matter (SOM) content, and soil texture. The applied LIBS instruments are a handheld and a platform spectrometer, which potentially allows for the single-point measurement and scanning of whole fields, respectively. Their results are compared with a high-resolution lab spectrometer. The prediction of soil parameters was based on multivariate methods. Different feature selection methods and regression methods like PLS, PCR, SVM, Lasso, and Gaussian processes were tested and compared. While good predictions were obtained for Ca, Mg, P, Mn, Cu, and silt content, excellent predictions were obtained for K, Fe, and clay content. The comparison of the three different spectrometers showed that although the lab spectrometer gives the best results, measurements with both field spectrometers also yield good results. This allows for a method transfer to the in-field measurements KW - LIBS KW - Precision agriculture KW - Soil KW - Multivariate methods KW - Feature selection PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-580777 DO - https://doi.org/10.3390/s23167178 VL - 23 IS - 16 SP - 1 EP - 17 PB - MDPI AG CY - Basel, Schweiz AN - OPUS4-58077 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Even, Morgane A1 - Juritsch, Elevtheria A1 - Richter, Matthias T1 - On the use of Carbograph 5TD as an adsorbent for sampling VVOCs: validation of an analytical method N2 - A standardised method for the analysis of very volatile organic compounds (VVOCs) in indoor air is still missing. This study evaluates the use of Carbograph 5TD as an adsorbent for 60 compounds (47 VVOCs + 13 VOCs) by comparing their recoveries with different spiking modes. The influence of the spiking of the tubes in dry nitrogen, humidified air or along the whole flushing duration mimicking real sampling was investigated. 49 substances (36 VVOCs from C1 to C6) had recoveries over 70% on the adsorbent in humidified air and were validated. The linearity of the calibration curves was verified for every spiking mode and the limits of detection (LOD) and quantification (LOQ) were determined. The LOQs were lower than the existing indoor air guideline values. The robustness of the method was considered by studying the influence of the sampling volume, the sampling flow rate, the humidity level and the storage of the tubes. In general, the most volatile or polar substances were the less robust ones. The combined measurement uncertainty was calculated and lies below 35% for a vast majority of the substances. An example of an emission chamber test using polyurethane foam is shown: Carbograph 5TD performs much better than Tenax® TA for VVOCs and emissions from n-butane were quantified with combined measurement uncertainty. KW - VVOC KW - Gas chromatography KW - Thermal desorption KW - Air sampling PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-581113 DO - https://doi.org/10.1039/D3AY00677H VL - 15 IS - 31 SP - 3810 EP - 3821 AN - OPUS4-58111 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Faßbender, Sebastian A1 - Rodiouchkina, K. A1 - Vanhaecke, F. A1 - Meermann, Björn T1 - Method development for on-line species-specific sulfur isotopic analysis by means of capillary electrophoresis/multicollector ICP-mass spectrometry N2 - In this work, a method for species-specific isotopic analysis of sulfur via capillary electrophoresis hyphenated on-line with multicollector ICP-MS (CE/MC-ICP-MS) was developed. Correction for the mass bias caused by instrumental mass discrimination was realized via external correction with multiple-injection sample-standard bracketing. By comparing the isotope ratio measurement results obtained using the newly developed on-line CE/MC-ICP-MS method with those obtained via traditional MC-ICP-MS measurement after analyte/matrix separation by anion exchange chromatography for isotopic reference materials and an in-house bracketing standard, the most suitable data evaluation method could be identified. The repeatability for the sulfate-δ34S value (calculated from 18 measurements of a standard conducted over seven measurement sessions) was 0.57‰ (2SD) and thereby only twice that obtained with off-line measurements (0.30‰, n = 68). As a proof of concept for analysis of samples with a real matrix, the determination of the sulfur isotopic composition of naturally present sulfate was performed for different river systems. The CE/MC-ICP-MS results thus obtained agreed with the corresponding off-line MC-ICP-MS results within the 2SD ranges, and the repeatability of consecutive δ34S measurements (n = 3) was between 0.3‰ and 1.3‰ (2SD). Finally, the isotopic analysis of two different S-species in a river water sample spiked with 2-pyridinesulfonic acid (PSA) was also accomplished. KW - River water sulfate KW - Environmental speciation KW - Sulfur isotopes KW - On-line CE/MC-ICP-MS KW - Multiple-injection sample-standard bracketing PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-509549 DO - https://doi.org/10.1007/s00216-020-02781-8 SN - 1618-2642 VL - 412 IS - 23 SP - 5637 EP - 5646 PB - Springer CY - Berlin, Heidelberg AN - OPUS4-50954 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Faßbender, Sebastian A1 - von der Au, Marcus A1 - Koenig, Maren A1 - Pelzer, J. A1 - Piechotta, Christian A1 - Vogl, Jochen A1 - Meermann, Björn T1 - Species-specific isotope dilution analysis of monomethylmercury in sediment using GC/ICP-ToF-MS and comparison with ICP-Q-MS and ICP-SF-MS N2 - A recently introduced inductively coupled plasma-time-of-flight-mass spectrometer (ICP-ToF-MS) shows enhanced sensitivity compared to previous developments and superior isotope ratio precision compared to other ToF and commonly used single-collector ICP-MS instruments. Following this fact, an improvement for isotope dilution ICP-MS using the new instrumentation has been reported. This study aimed at investigating whether this improvement also meets the requirements of species-specific isotope dilution using GC/ICP-MS, where short transient signals are recorded. The results of the analysis of monomethylmercury (MMHg) of a sediment reference material show that isotope ratio precision of ICP-MS instruments equipped with quadrupole, sector-field, and time-of-flight mass analyzers is similar within a broad range of peak signal-to-noise ratio when analyzing one isotopic system. The procedural limit of quantification (LOQ) for MMHg, expressed as mass fraction of Hg being present as MMHg, w(Hg)MMHg, was similar as well for all investigated instruments and ranged between 0.003 and 0.016 μg/kg. Due to the simultaneous detection capability, the ICP-ToF-MS might, however, be more favorable when several isotopic systems are analyzed within one measurement. In a case study, the GC/ICP-ToF-MS coupling was applied for analysis of MMHg in sediments of Finow Canal, a historic German canal heavily polluted with mercury. Mass fractions between 0.180 and 41 μg/kg (w(Hg)MMHg) for MMHg, and 0.056 and 126 mg/kg (w(Hg)total) for total mercury were found in sediment samples taken from the canal upstream and downstream of a former chemical plant. KW - Methylmercury KW - Legacy pollution KW - Finow Canal KW - Isotope dilution KW - Mercury speciation PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-529967 DO - https://doi.org/10.1007/s00216-021-03497-z SN - 1618-2642 VL - 413 IS - 21 SP - 5279 EP - 5289 PB - Springer CY - Berlin AN - OPUS4-52996 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Feord, Helen K. A1 - Trautwein-Schult, Anke A1 - Keuschnig, Christoph A1 - Ostrzinski, Anne A1 - Peter, Elisa K. A1 - Jaeger, Carsten A1 - Lisec, Jan A1 - Mourot, Rey A1 - Peters, Ravi Sven A1 - Çiftçi, Ozan A1 - Tranter, Martyn A1 - Anesio, Alexandre M. A1 - Becher, Dörte A1 - Benning, Liane G. T1 - Algae-dominated metaproteomes uncover cellular adaptations to life on the Greenland Ice Sheet N2 - Eukaryotic algae-dominated microbiomes thrive on the Greenland Ice Sheet (GrIS) in harsh environmental conditions, including low temperatures, high light, and low nutrient availability. Chlorophyte algae bloom on snow, while streptophyte algae dominate bare ice surfaces. Empirical data about the cellular mechanisms responsible for their survival in these extreme conditions are scarce. This knowledge gap was addressed by quantifying proteins for both algal taxa from samples on the southern margin of the GrIS. We show that the streptophyte glacier ice algae have a relative enrichment in proteins involved in environmental signaling and nutrient transport, indicative of cellular readiness to dynamically respond to extreme GriS environmental cues, linked, for example, to photoprotection and the rapid update of scarce nutrients. In contrast, the chlorophyte snow algae have a high abundance of proteins linked to lipid and nitrogen metabolisms, providing evidence for the biological processes sustaining the cellular carbon and nitrogen stores necessary for survival in an oligotrophic environment. We also identify proteins in both taxa linked to the synthesis and breakdown of key cellular pigments. Our study gives novel insights into the cellular biology of these algae and their adaptation to extreme environments. KW - Metabolic profiling KW - Mass spectrometry KW - Ice algae PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-641037 DO - https://doi.org/10.1038/s41522-025-00770-2 SN - 2055-5008 VL - 11 IS - 1 SP - 1 EP - 11 PB - Springer Science and Business Media LLC AN - OPUS4-64103 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Fernandez-Menendez, L. J. A1 - Mendez-Lopez, C. A1 - Abad Andrade, Carlos Enrique A1 - Fandino, J. A1 - Gonzalez-Gago, C. A1 - Pisonero, J. A1 - Bordel, N. T1 - A critical evaluation of the chlorine quantification method based on molecular emission detection in LIBS N2 - The entire process involving the determination of Cl by molecular emission detection in Laser-Induced Breakdown Spectroscopy (LIBS) is thoroughly studied in this paper. This critical evaluation considers how spectra are normalized, how interferences from other molecular species signals are removed, and how signal integration is applied. Moreover, a data treatment protocol is proposed to achieve reliable and accurate Cl determination from the CaCl molecular spectral signal, not requiring the use of more complex numerical approaches. Calcium chloride dihydrate (CaCl2⋅2H2O) and high purity anhydrite samples (CaSO4) are used to optimize the acquisition conditions and data treatment of CaCl emission signal. Using the developed protocol, calibration curves for Cl, covering the concentration range from 0 μg/g to 60,000 μg/g of Cl, are successfully achieved. Finally, the suitability of the proposed methodology for Cl determination is successfully applied in industrial gypsum waste samples, where the results obtained by LIBS are validated using high-resolution molecular absorption spectroscopy (HR-CS-MAS) and potentiometric titration. KW - Laser induced breakdown Spectrocopy (LIBS) KW - Molecular spectra KW - Chlorine determination KW - CaCl emission bands KW - Industrial gypsum PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-544292 DO - https://doi.org/10.1016/j.sab.2022.106390 SN - 0584-8547 VL - 190 SP - 1 EP - 9 PB - Elsevier B.V. CY - Amsterdam, Netherlands AN - OPUS4-54429 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Fiedler, Saskia A1 - Frenzel, Florian A1 - Würth, Christian A1 - Tavernaro, Isabella A1 - Grüne, M. A1 - Schweizer, S. A1 - Engel, A. A1 - Resch-Genger, Ute T1 - Interlaboratory Comparison on Absolute Photoluminescence Quantum Yield Measurements of Solid Light Converting Phosphors with Three Commercial Integrating Sphere Setups N2 - Scattering luminescent materials dispersed in liquid and solid matrices and luminescent powders are increasingly relevant for fundamental research and industry. Examples are luminescent nano- and microparticles and phosphors of different compositions in various matrices or incorporated into ceramics with applications in energy conversion, solid-state lighting, medical diagnostics, and security barcoding. The key parameter to characterize the performance of these materials is the photoluminescence/fluorescence quantum yield (Φf), i.e., the number of emitted photons per number of absorbed photons. To identify and quantify the sources of uncertainty of absolute measurements of Φf of scattering samples, the first interlaboratory comparison (ILC) of three laboratories from academia and industry was performed by following identical measurement protocols. Thereby, two types ofcommercial stand-alone integrating sphere setups with different illumination and detection geometries were utilized for measuring the Φf of transparent and scattering dye solutions and solid phosphors, namely, YAG:Ce optoceramics of varying surface roughness, used as converter materials for blue light emitting diodes. Special emphasis was dedicated to the influence of the measurement geometry, the optical properties of the blank utilized to determine the number of photons of the incident excitation light absorbed by the sample, and the sample-specific surface roughness. While the Φf values of the liquid samples matched between instruments, Φf measurements of the optoceramics with different blanks revealed substantial differences. The ILC results underline the importance of the measurement geometry, sample position, and blank for reliable Φf data of scattering the YAG:Ce optoceramics, with the blank’s optical properties accounting for uncertainties exceeding 20%. KW - Nano KW - Fluorescence KW - Reference material KW - Luminescence KW - Quantitative spectroscopy KW - Particle KW - Quantum yield KW - Quality assurance KW - Phosphor KW - Converter material KW - Lifetime KW - Interlaboratory comparison KW - Method KW - Uncertainty PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-600945 DO - https://doi.org/10.1021/acs.analchem.4c00372 SN - 0003-2700 SP - 6730 EP - 6737 PB - ACS Publications AN - OPUS4-60094 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Fiedler, Saskia A1 - Ton-That, C. A1 - Phillips, M. R. T1 - Defect-free ZnO nanorods with high angular distribution for enhanced excitonic emission N2 - AbstractLow-temperature hydrothermal growth has emerged as a popular method for the fabrication of ZnO nanorods (NRs), increasing the functionality and utility of ZnO-based devices. In this work, we study the influence of growth time, temperature and seed layer on the dimensions and angular distribution of ZnO NRs. High-quality NRs with a crisscrossed 60° angular distribution have been grown with a 20–60 nm diameter and 600 nm length. We show that, within the ideal range of growth parameters, the growth time and temperature have no controllable influence on NR diameter and length, while the deposition method and size of the pre-growth deposited ZnO seeds affects diameter and NR angular alignment. We demonstrate advantages of using crisscross-aligned NRs over planar ZnO for the enhancement of ZnO excitonic emission by optical coupling with gold nanoparticles. These results can be readily adapted for applications that involve surface coating-mediated enhancement of both light emission and injection. KW - ZnO nanorod KW - Hydrothermal growth KW - Seed layer KW - Angular distribution KW - Cathodoluminescence KW - Luminescence enhancement PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-618176 DO - https://doi.org/10.1557/s43578-023-00941-x SN - 0884-2914 SN - 2044-5326 VL - 38 IS - 8 SP - 2145 EP - 2155 PB - Springer CY - Berlin AN - OPUS4-61817 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Filimonova, S. M. A1 - Melnikov, E. S. A1 - Kaufmann, Jan Ole A1 - Shchepochkina, O. Y. A1 - Eremin, S. A. A1 - Gravel, I. V. A1 - Raysyan, Anna T1 - Exploring the anti‐α‐amylase activity of flavonoid aglycones in fabaceae plant extracts: a combined MALDI‐TOF‐MS and LC–MS/MS approach N2 - A combination of TLC-bioautography, MALDI-TOF-MS and LC–MS/MS methods was used to identify flavonoids with anti-α-amylase activity in extracts of Lathyrus pratensis L. (herb), L. polyphillus L. (fruits), Thermopsis lanceolata R. Br. (herb) and S. japonica L. (buds). After the TLC-autobiography assay, substances with anti-amylase activity were identified by MALDI-TOF-MS followed by confirmation of the result by LC–MS/MS. Results of the study revealed that the flavonoids apigenin, luteolin, formononetin, genistein and kaempferol display marked anti-α-amylase activity. Formononetin showed the largest activity. Compared with LC–MS/MS, MALDI-TOF-MS is a quick and convenient method; results can be obtained within minutes; and only minor sample amounts are required which allows us to analyse mixtures of substances without preliminary separation. However, the inability to distinguish between isomers is the main limitation of the method. KW - Enzyme KW - MALDI-TOF-MS KW - LC-MS/MS KW - Massenspektrometrie PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-577128 DO - https://doi.org/https://doi.org/10.1111/ijfs.16491 SN - 0950-5423 VL - 58 IS - 7 SP - 3902 EP - 3911 PB - Wiley & Sons CY - Hoboken, NJ, USA AN - OPUS4-57712 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Fischer, Janina A1 - Kaufmann, Jan Ole A1 - Weller, Michael G. T1 - Simple Determination of Affinity Constants of Antibodies by Competitive Immunoassays N2 - The affinity constant, also known as the equilibrium constant, binding constant, equilibrium association constant, or the reciprocal value, the equilibrium dissociation constant (Kd), can be considered as one of the most important characteristics for any antibody–antigen pair. Many methods based on different technologies have been proposed and used to determine this value. However, since a very large number of publications and commercial datasheets do not include this information, significant obstacles in performing such measurements seem to exist. In other cases where such data are reported, the results have often proved to be unreliable. This situation may indicate that most of the technologies available today require a high level of expertise and effort that does not seem to be available in many laboratories. In this paper, we present a simple approach based on standard immunoassay technology that is easy and quick to perform. It relies on the effect that the molar IC50 approaches the Kd value in the case of infinitely small concentrations of the reagents. A two-dimensional dilution of the reagents leads to an asymptotic convergence to Kd. The approach has some similarity to the well-known checkerboard titration used for the optimization of immunoassays. A well-known antibody against the FLAG peptide, clone M2, was used as a model system and the results were compared with other methods. This approach could be used in any case where a competitive assay is available or can be developed. The determination of an affinity constant should belong to the crucial parameters in any quality control of antibody-related products and assays and should be mandatory in papers using immunochemical protocols. N2 - Die Affinitätskonstante, auch bekannt als Gleichgewichtskonstante, Bindungskonstante, Gleichgewichtsassoziationskonstante oder der reziproke Wert, die Gleichgewichtsdissoziationskonstante (Kd), kann als eine der wichtigsten Eigenschaften für jedes Antikörper-Antigen-Paar angesehen werden. Zur Bestimmung dieses Wertes wurden zahlreiche Methoden auf der Grundlage verschiedener Technologien vorgeschlagen und verwendet. Da jedoch eine sehr große Anzahl von Veröffentlichungen und kommerziellen Datenblätter diese Information nicht enthalten, scheint es erhebliche Hindernisse bei der Durchführung solcher Messungen zu geben. In anderen Fällen, in denen solche Daten angegeben werden, haben sich die Ergebnisse häufig als unzuverlässig erwiesen. Diese Situation könnte darauf hindeuten, dass die meisten der heute verfügbaren Technologien ein hohes Maß an Fachwissen und Aufwand erfordern, das in vielen Labors nicht vorhanden zu sein scheint. In diesem Beitrag stellen wir einen einfachen Ansatz vor, der auf der Standard-Immunoassay-Technologie basiert und einfach und schnell durchführbar ist. Er beruht auf dem Effekt, dass sich der molare IC50 bei unendlich kleinen Reagenz-Konzentrationen dem Kd-Wert annähert. Eine zweidimensionale Verdünnung der Reagenzien führt zu einer asymptotischen Konvergenz zu Kd. Der Ansatz hat eine gewisse Ähnlichkeit mit der bekannten Checkerboard-Titration, die zur Optimierung von Immunoassays verwendet wird. Ein bekannter Antikörper gegen das FLAG-Peptid, Klon M2, wurde als Modellsystem verwendet, und die Ergebnisse wurden mit anderen Methoden verglichen. Dieser Ansatz kann überall dort angewendet werden, wo ein kompetitiver Assay verfügbar ist oder entwickelt werden kann. Die Bestimmung einer Affinitätskonstante sollte zu den entscheidenden Parametern bei der Qualitätskontrolle von Antikörperprodukten und -assays gehören und in Arbeiten, die immunchemische Protokolle verwenden, obligatorisch sein. KW - ELISA KW - Competitive immunoassay KW - IC50 KW - Test midpoint KW - Point of inflection KW - Equilibrium constant KW - Dissociation constant KW - Binding strength KW - Antibody antigen complex KW - Bio-interaction KW - SPR KW - Surface-plasmon resonance KW - FLAG peptide KW - Clone M2 KW - Antibody quality PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-605607 DO - https://doi.org/10.3390/mps7030049 SN - 2409-9279 VL - 7 IS - 3 SP - 1 EP - 11 PB - MDPI CY - Basel AN - OPUS4-60560 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Flierl, Lukas A1 - Rienitz, Olaf A1 - Vogl, Jochen A1 - Pramann, Axel T1 - An advancement of the gravimetric isotope mixture method rendering the knowledge of the spike purity superfluous N2 - The gravimetric isotope mixture method is the primary method to determine absolute isotope ratios. This method, however, depends on the existence of suitable spike materials and knowledge of their purities. Determining the purity of the spikes can be tedious and labour-intensive. In this publication, an advancement of the gravimetric isotope mixture method, rendering the determination of the purity of the spike materials unnecessary, is presented. The advancement combines mass spectrometry and ion chromatography leading to an approach being independent of the purity of the spike materials. In the manuscript the mathematical background and the basic idea of the novel approach are described using a two-isotope system like copper or lithium. KW - Isotope amount ratios KW - Metrology KW - Mass spectrometry KW - Ion chromatography PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-608726 DO - https://doi.org/10.1007/s00216-024-05465-9 SP - 5325 EP - 5333 PB - Springer Science and Business Media LLC AN - OPUS4-60872 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Frenzel, F. A1 - Fiedler, S. A1 - Bardan, A. A1 - Güttler, Arne A1 - Würth, Christian A1 - Resch-Genger, Ute T1 - Influence of Measurement Geometry and Blank on Absolute Measurements of Photoluminescence Quantum Yields of Scattering Luminescent Films N2 - For a series of 500 μm-thick polyurethane films containing different concentrations of luminescent and scattering YAG:Ce microparticles, we systematically explored and quantified pitfalls of absolute measurements of photoluminescence quantum yields (Φf) for often employed integrating sphere (IS) geometries, where the sample is placed either on a sample holder at the bottom of the IS surface or mounted in the IS center. Thereby, the influence of detection and illumination geometry and sample position was examined using blanks with various scattering properties for measuring the number of photons absorbed by the sample. Our results reveal that (i) setup configurations where the scattering sample is mounted in the IS center and (ii) transparent blanks can introduce systematic errors in absolute Φf measurements. For strongly scattering, luminescent samples, this can result in either an under- or overestimation of the absorbed photon flux and hence an under- or overestimation of Φf. The size of these uncertainties depends on the scattering properties of the sample and instrument parameters, such as sample position, IS size, wavelength-dependent reflectivity of the IS surface coating, and port configuration. For accurate and reliable absolute Φf measurements, we recommend (i) a blank with scattering properties closely matching those of the sample to realize similar distributions of the diffusely scattered excitation photons within the IS, and (ii) a sufficiently high sample absorption at the excitation wavelength. For IS setups with center-mounted samples, measurement geometries should be utilized that prevent the loss of excitation photons by reflections from the sample out of the IS. KW - Quality assurance KW - Fluorescence KW - Nano KW - Particle KW - Quantum yield KW - Characterization KW - Silica KW - Scattering KW - Uncertainty KW - Film KW - Pphosphor KW - YAG:Ce KW - LED KW - Converter material KW - Solid material KW - Polymer KW - Composite material KW - Advanced material PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-638304 DO - https://doi.org/10.1021/acs.analchem.4c06726 SN - 1520-6882 SP - 1 EP - 8 PB - ACS Publications AN - OPUS4-63830 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Frenzel, Olivia A1 - Westphalen, Tanja A1 - Kaminski, Katja A1 - Kluge, Stephanie A1 - Bücker, Michael A1 - Piechotta, Christian T1 - Evaluation and Validation of an Accelerated Weathering Procedure to Characterise the Release of Bisphenol A from Polycarbonate Under Exposure to Simulated Environmental Conditions N2 - Bisphenol A (BPA) has been listed as a substance of very high concern (SVHC) due to its endocrine-disrupting properties according to REACH in 2017. European competent authorities have prepared a REACH restriction proposal to reduce BPA levels in the environment. The proposed limit for the concentration of free BPA and other bisphenols in articles is 10 mg kg−1. If exceeded, migration testing can demonstrate that no more than 0.04 mg L−1 is released from the product or material over its lifetime. German authorities are drafting a new restriction proposal after the original was temporarily withdrawn. The residual and migration limits mentioned above were key requirements from the previous restriction proposal. Numerous national and international standards exist for assessing how environmental factors affect the physical and chemical properties of products and materials—such as notch impact strength and tensile strength—but these standards do not cover the release of pollutants. A standardised procedure that covers all aspects of artificial weathering and monitors the subsequent release of pollutants is necessary, especially in the context of the regulation of these substances. An accelerated weathering procedure was established for non-protected samples. This material was not intended for outdoor applications. The testing procedure applied a typical weathering scenario that represents Central European climate conditions. The procedure was validated and applied to samples under distinct quality assurance aspects. Released BPA is quantified via an organic isotope dilution LC-MS/MS method. In parallel, identical samples were weathered outdoors on a weathering rack. Haze and yellowness index are measured to compare outdoor and weathering chamber results. KW - Artificial weathering KW - Polycarbonate KW - Bisphenol A KW - Simulated environmental conditions PY - 2025 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-645020 DO - https://doi.org/10.3390/app151910361 SN - 2076-3417 VL - 15 IS - 19 SP - 1 EP - 15 PB - MDPI AG AN - OPUS4-64502 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Fricke, F. A1 - Brandalero, M. A1 - Liehr, Sascha A1 - Kern, Simon A1 - Meyer, Klas A1 - Kowarik, Stefan A1 - Hierzegger, R. A1 - Westerdick, S. A1 - Maiwald, Michael A1 - Hübner, M. T1 - Artificial Intelligence for Mass Spectrometry and Nuclear Magnetic Resonance Spectroscopy Using a Novel Data Augmentation Method N2 - Mass Spectrometry (MS) and Nuclear Magnetic Resonance Spectroscopy (NMR) are valuable analytical and quality control methods for most industrial chemical processes as they provide information on the concentrations of individual compounds and by-products. These processes are traditionally carried out manually and by a specialist, which takes a substantial amount of time and prevents their utilization for real-time closed-loop process control. This paper presents recent advances from two projects that use Artificial Neural Networks (ANNs) to address the challenges of automation and performance-efficient realizations of MS and NMR. In the first part, a complete toolchain has been realized to develop simulated spectra and train ANNs to identify compounds in MS. In the second part, a limited number of experimental NMR spectra have been augmented by simulated spectra, to train an ANN with better prediction performance and speed than state-of-the-art analysis. These results suggest that, in the context of the digital transformation of the process industry, we are now on the threshold of a strongly simplified use of MS and MRS and the accompanying data evaluation by machine-supported procedures, and can utilize both methods much wider for reaction and process monitoring or quality control. KW - Industry 4.0 KW - Cyber-Physical Systems KW - Artificial Neural Networks KW - Mass Spectrometry KW - Nuclear Magnetic Resonance Spectroscopy KW - Modular Production PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-539412 UR - https://ieeexplore.ieee.org/stamp/stamp.jsp?tp=&arnumber=9638378 DO - https://doi.org/10.1109/TETC.2021.3131371 SN - 2168-6750 VL - 10 IS - 1 SP - 87 EP - 98 PB - IEEE AN - OPUS4-53941 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Fröhlich-Nowoisky, J. A1 - Bothen, N. A1 - Backes, A. T. A1 - Weller, Michael G. A1 - Pöschl, U. T1 - Oligomerization and tyrosine nitration enhance the allergenic potential of the birch and grass pollen allergens Bet v 1 and Phl p 5 N2 - Protein modifications such as oligomerization and tyrosine nitration alter the immune response to allergens and may contribute to the increasing prevalence of allergic diseases. In this mini-review, we summarize and discuss relevant findings for the major birch and grass pollen allergens Bet v 1 and Phl p 5 modified with tetranitromethane (laboratory studies), peroxynitrite (physiological processes), and ozone and nitrogen dioxide environmental conditions). We focus on tyrosine nitration and the formation of protein dimers and higher oligomers via dityrosine cross-linking and the immunological effects studied. N2 - Proteinmodifikationen wie Oligomerisierung und Tyrosinnitrierung verändern die Immunantwort auf Allergene und tragen möglicherweise zur zunehmenden Prävalenz allergischer Erkrankungen bei. In diesem Mini-Review fassen wir relevante Befunde zu den wichtigsten Birken- und Gräserpollenallergenen Bet v 1 und Phl p 5 zusammen, die mit Tetranitromethan (Laborstudien), Peroxynitrit (physiologische Prozesse) und Ozon und Stickstoffdioxid (Umweltbedingungen). Wir konzentrieren uns auf die Tyrosin-Nitrierung und die Bildung von Proteindimeren und höheren Oligomeren durch Dityrosin-Vernetzung und deren immunologischen Auswirkungen. KW - Allergy KW - Nitration KW - Protein oligomers KW - Air pollution KW - Ozone KW - Nitrogen oxides KW - Tyrosine KW - Nitrotyrosine KW - Dityrosine KW - Dityrosine crosslinking KW - Protein degradation KW - Neoepitopes KW - Neoallergen KW - IgE KW - Immunoglobulin E PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-591453 DO - https://doi.org/10.3389/falgy.2023.1303943 VL - 4 SP - 1 EP - 8 PB - Frontiers Media CY - Switzerland AN - OPUS4-59145 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Garrido, E. A1 - Hernández-Sigüenza, G. A1 - Climent, Estela A1 - Marcos, M. D. A1 - Rurack, Knut A1 - Gaviña, P. A1 - Parra, M. A1 - Sancenón, F. A1 - Martí-Centelles, V. A1 - Martínez-Máñez, R. T1 - Strip-based lateral flow-type indicator displacement assay for γ-hydroxybutyric acid (GHB) detection in beverages N2 - The use of gamma-hydroxybutyric acid (GHB) in drug-facilitated sexual assault has increased due to its availability and high solubility in aqueous solutions and alcoholic beverages, necessitating the development of rapid methods for GHB detection. In this respect, portable testing methods for use in the field, based on lateral flow assays (LFAs) and capable of detecting trace concentrations of target analytes, are particularly attractive and hold enormous potential for the detection of illicit drugs. Using this strategy, here we report a rapid, low cost, easy-to-handle strip-based LFA for GHB analysis employing a smartphone for fluorescence readout. At molecular signalling level, the ensemble is based on a Cu2+ complex with a tetradentate ligand and the fluorescent dye coumarin 343, which indicate GHB through an indicator displacement assay (IDA) in aqueous solution. When incorporated in a LFA-based strip test this system shows a detection limit as low as 0.03 μM for GHB in MES buffer solution and is able to detect GHB at concentrations of 0.1 μM in soft drinks and alcoholic beverages in only 1 min. KW - Indicator displacement assay KW - Gamma-hydroxybutyric acid KW - Lateral flow assay KW - Test strip KW - Fluorescent dyes KW - Smartphone readout PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-564631 DO - https://doi.org/10.1016/j.snb.2022.133043 SN - 0925-4005 VL - 377 SP - 1 EP - 7 PB - Elsevier B.V. CY - Amsterdam AN - OPUS4-56463 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Gehrenkemper, Lennart A1 - Rühl, Isabel A1 - Westphalen, Tanja A1 - Simon, Fabian A1 - von der Au, Marcus A1 - Cossmer, Antje A1 - Meermann, Björn T1 - Investigating the uptake and fate of per- and polyfluoroalkylated substances (PFAS) in bean plants (Phaseolus vulgaris): comparison between target MS and sum parameter analysis via HR-CS-GFMAS N2 - AbstractIn this study, we present a screening method based on molecular absorption spectrometry to study PFAS uptake and fate in plants. To evaluate the suitability of this method we analyzed plant extracts with molecular absorption spectrometry (MAS) as well as liquid chromatography–tandem mass spectrometry (LC–MS/MS) for mass balance studies (w(F)). French bean plants (Phaseolus vulgaris) were grown on soil spiked using eight PFAS substances that vary in chain length and functional group composition. Specifically, these include three short-chained (C4–C5), five long-chained (C7–C10) carboxylic acids, one sulfonic acid and one sulfonic amide moieties. To investigate substance-specific PFAS uptake systematically, PFAS were spiked as single substance spike. Additionally, we studied one mixture of the investigated substances in equal proportions regarding w(F) and four PFAS mixtures of unknown composition. After 6 weeks, the plants were separated into four compartments. We analyzed the four compartments as well as the soil for extractable organically bound fluorine (EOF) by high resolution-continuum source-graphite furnace-molecular absorption spectrometry (HR-CS-GFMAS) as well as for sum of ten target-PFAS by LC–MS/MS. All three short-chained PFAS perfluorobutanoic acid (PFBA), perfluorobutanoic sulfonic acid (PFBS) and perfluoropentanoic acid (PFPeA) were determined in high concentrations mainly in the fruits of the investigated plants while long-chained PFAS perfluorononanoic acid (PFNA) and perfluorodecanoic acid (PFDA) were mainly determined in roots. PFBS was determined in remarkably high concentrations in leaves compartment by both quantification methods. Overall, comprehensive results of single substance spikes were in good agreement for both methods except for a few cases. Hence, two phenomena were identified: for mixed PFAS spikes of unknown composition huge differences between EOF and sum of target PFAS were observed with systematically higher EOF values. Overall, both methods indicate comparable results with MS being more reliable for known PFAS contamination and MAS being more valuable to identify PFAS exposure of unknown composition. Graphical Abstract KW - Pollution PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-589394 DO - https://doi.org/10.1186/s12302-023-00811-7 VL - 35 IS - 104 SP - 1 EP - 13 PB - Springer Science and Business Media LLC AN - OPUS4-58939 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Gehrenkemper, Lennart A1 - Simon, Fabian A1 - Roesch, Philipp A1 - Fischer, E. A1 - von der Au, Marcus A1 - Pfeifer, Jens A1 - Cossmer, Antje A1 - Wittwer, Philipp A1 - Vogel, Christian A1 - Simon, Franz-Georg A1 - Meermann, Björn T1 - Determination of organically bound fluorine sum parameters in river water samples - Comparison of combustion ion chromatography (CIC) and high resolution-continuum source-graphite furnace molecular absorption spectrometry (HR-CS-GFMAS) N2 - In this study, we compare combustion ion chromatography (CIC) and high resolution-continuum source-graphite furnace molecular absorption spectrometry (HR-CS-GFMAS) with respect to their applicability for determining organically Bound fluorine sum parameters. Extractable (EOF) and adsorbable (AOF) organically bound fluorine as well as total fluorine (TF) were measured in samples fromriver Spree in Berlin, Germany, to reveal the advantages and disadvantages of the two techniques used as well as the two established fluorine sum Parameters AOF and EOF. TF concentrations determined via HR-CS-GFMAS and CIC were comparable between 148 and 270 μg/L. On average, AOF concentrations were higher than EOF concentrations, with AOF making up 0.14–0.81% of TF (determined using CIC) and EOF 0.04–0.28% of TF (determined using HR-CSGFMAS). The results obtained by the two independent methods were in good agreement. It turned out that HR-CS-GFMAS is a more sensitive and precise method for fluorine analysis compared to CIC. EOF and AOF are comparable tools in Risk evaluation for the emerging pollutants per- and polyfluorinated alkyl substances; however, EOF is much faster to conduct. KW - High resolution-continuum source-graphite furnace molecular absorption spectrometry (HR-CS-GFMAS) KW - Combustion ion chromatography (CIC) KW - Per- and polyfluorinated alkyl substances (PFASs) KW - Adsorbable organically bound fluorine (AOF) KW - Extractable organically bound fluorine (EOF) KW - Surface waters PY - 2020 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-515351 DO - https://doi.org/10.1007/s00216-020-03010-y SN - 1618-2650 VL - 413 IS - 28 SP - 103 EP - 115 PB - Springer CY - Berlin AN - OPUS4-51535 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Geißler, Daniel A1 - Nirmalananthan-Budau, Nithiya A1 - Scholtz, Lena A1 - Tavernaro, Isabella A1 - Resch-Genger, Ute T1 - Analyzing the surface of functional nanomaterials — how to quantify the total and derivatizable number of functional groups and ligands N2 - Functional nanomaterials (NM) of different size, shape, chemical composition, and surface chemistry are of increasing relevance for many key technologies of the twenty-first century. This includes polymer and silica or silica-coated nanoparticles (NP) with covalently bound surface groups, semiconductor quantum dots (QD), metal and metal oxide NP, and lanthanide-based NP with coordinatively or electrostatically bound ligands, as well as surface-coated nanostructures like micellar encapsulated NP. The surface chemistry can significantly affect the physicochemical properties of NM, their charge, their processability and performance, as well as their impact on human health and the environment. Thus, analytical methods for the characterization of NM surface chemistry regarding chemical identification, quantification, and accessibility of functional groups (FG) and surface ligands bearing such FG are of increasing importance for quality control of NM synthesis up to nanosafety. Here, we provide an overview of analytical methods for FG analysis and quantification with special emphasis on bioanalytically relevant FG broadly utilized for the covalent attachment of biomolecules like proteins, peptides, and oligonucleotides and address methodand material-related challenges and limitations. Analytical techniques reviewed include electrochemical titration methods, optical assays, nuclear magnetic resonance and vibrational spectroscopy, as well as X-ray based and thermal analysis methods, covering the last 5–10 years. Criteria for method classification and evaluation include the need for a signal-generating label, provision of either the total or derivatizable number of FG, need for expensive instrumentation, and suitability for process and production control during NM synthesis and functionalization. KW - Functional group quantification KW - Surface ligand KW - Nanomaterial KW - Optical detection KW - Electrochemical titration KW - Nanosafety (Safe-by-design) PY - 2021 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-533597 DO - https://doi.org/10.1007/s00604-021-04960-5 VL - 188 IS - 10 SP - 1 EP - 28 PB - Springer Nature AN - OPUS4-53359 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -