TY - JOUR A1 - Tukhmetova, Dariya A1 - Langhammer, Nicole A1 - Vogl, Jochen A1 - Meermann, Björn T1 - Online Isotope Analysis of Sulfur in Proteins via Capillary Electrophoresis Coupled With Multicollector ICP‐MS (CE/MC‐ICP‐MS): A Proof of Concept Study N2 - Isotope ratio analysis of sulfur in biological samples using inductively coupled plasma-mass spectrometry (ICP-MS) has gained significant interest for applications in quantitative proteomics. Advancements like coupling separation techniques with multicollector ICP-MS (MC-ICP-MS) enhance the throughput of species-specific sulfur isotope ratio measurements, fostering new avenues for studying sulfur metabolism in complex biological matrices. This proof-of-concept study investigates the feasibility of online CE/MC-ICP-MS for directly analyzing sulfur isotope ratios in proteins (albumin). Leveraging our previous work on the applicability of CE/ICP-MS for quantifying sulfur-containing biological molecules, we explore its potential for sulfur isotope analysis. Our results demonstrate that direct analysis of sulfur isotopes in albumin protein using online capillary electrophoresis MC-ICP-MS (CE/MC-ICP-MS) eliminates the need for laborious pretreatment steps, while yielding isotope ratios comparable to the reference values. Although initial precision can be improved through further system optimization and protein injection techniques, this approach paves the way for future analysis of mixtures of various biological compounds in, for example, clinical diagnosis studies. KW - Isotope analysis KW - Sulfur KW - CE/MC-ICP-MS PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-612439 DO - https://doi.org/10.1002/elps.202400128 SN - 0173-0835 SP - 1 EP - 6 PB - Wiley-Blackwell CY - Weinheim AN - OPUS4-61243 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Duddi, M. A1 - Kocherla, Amarteja A1 - Subramaniam, K. V. L. T1 - Evaluation of boundary and material influences on the dynamic electromechanical impedance response of the embedded PZT sensor in concrete N2 - The article explores the material and structural size effects on the electrical impedance response of the embedded PZT sensors which are used as an sensors/actuator in the smart sensing concrete. An embedded sensor for use in concrete monitoring is developed using Lead Zirconate Titanate (PZT). The electrical impedance (EI) response of the sensor placed inside concrete cubes of varying sizes are recorded for an applied electrical input of varying frequency. The dynamic response of the embedded PZT sensor to the applied electrical input is determined by the mechanical impedance offered by the surrounding medium. In specimens of finite size, the mechanical impedance to the motion of the PZT is influenced by the combination of dynamic material resistance and structural stiffness (size of the structure). The current study examined the effects of material resistance and size of structure on the EI response of the PZT sensor embedded in concrete medium. The influence of the size of the medium from small-sized specimens is seen in the form of secondary peaks, identified as structural peaks, on the resonance spectrum of the embedded PZT sensor. The structural peaks on the EI response are very dominant in the concrete cube of small sizes. Magnitude and intensity of these structural peaks attenuate with an increase in the size of the concrete cube. Also, the EI response from the smaller-sized specimens registered a significant leftward shift in the spectrum. The observations from the numerical simulations also showed the mechanical impedance of the surrounding concrete medium to the motion of the PZT also increases and converges at 150 mm. At sizes below 150 mm, the structural effects that are influenced by the specimen boundary must be separated to access the material properties of the concrete medium from the measured EI response of an embedded PZT sensor. At sizes, larger than 150 mm, the dynamic motion of the PZT patch and the measured EI response of the PZT patch depend only on the dynamic material properties of the concrete medium around the sensor. The zone of influence and its importance in standardization of PZT sensor for SHM of concrete structures is discussed. KW - PZT KW - Concrete sensor KW - Embedded KW - Electrical impedance KW - Mechanical impedance KW - Zone of influence PY - 2023 DO - https://doi.org/10.1016/j.sna.2023.114575 SN - 0924-4247 SN - 1873-3069 VL - 361 SP - 1 EP - 12 PB - Elsevier CY - Amsterdam AN - OPUS4-61791 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Dhull, N. A1 - Kaur, Gurpreet A1 - Jindal, K. A1 - Verma, M. A1 - Tomar, M. T1 - Microfluidics integrated NiO based electrolyte-gated FETs for the detection of cortisol N2 - A microfluidics integrated EGFET has been devised using NiO for the detection of cortisol. A low detection limit of 0.5 fg mL−1 has been achieved and human salivary cortisol has been successfully assessed. KW - Microfluidic system KW - Field effect transistor (FET) KW - Electrolyte gating PY - 2022 DO - https://doi.org/10.1039/d2tb01652d SN - 2050-7518 VL - 10 IS - 44 SP - 9226 EP - 9234 PB - Royal Society of Chemistry (RSC) CY - London AN - OPUS4-61772 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Li, Yue A1 - Colnaghi, Timoteo A1 - Gong, Yilun A1 - Zhang, Huaide A1 - Yu, Yuan A1 - Wei, Ye A1 - Gan, Bin A1 - Song, Min A1 - Marek, Andreas A1 - Rampp, Markus A1 - Zhang, Siyuan A1 - Pei, Zongrui A1 - Wuttig, Matthias A1 - Ghosh, Sheuly A1 - Körmann, Fritz A1 - Neugebauer, Jörg A1 - Wang, Zhangwei A1 - Gault, Baptiste T1 - Machine learning‐enabled tomographic imaging of chemical short‐range atomic ordering N2 - In solids, chemical short‐range order (CSRO) refers to the self‐organization of atoms of certain species occupying specific crystal sites. CSRO is increasingly being envisaged as a lever to tailor the mechanical and functional properties of materials. Yet quantitative relationships between properties and the morphology, number density, and atomic configurations of CSRO domains remain elusive. Herein, it is showcased how machine learning‐enhanced atom probe tomography (APT) can mine the near‐atomically resolved APT data and jointly exploit the technique's high elemental sensitivity to provide a 3D quantitative analysis of CSRO in a CoCrNi medium‐entropy alloy. Multiple CSRO configurations are revealed, with their formation supported by state‐of‐the‐art Monte‐Carlo simulations. Quantitative analysis of these CSROs allows establishing relationships between processing parameters and physical properties. The unambiguous characterization of CSRO will help refine strategies for designing advanced materials by manipulating atomic‐scale architectures. KW - Chemical short-range order (CSRO) KW - Atom probe tomography (APT) KW - Machine learning PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-623777 DO - https://doi.org/10.1002/adma.202407564 SN - 1521-4095 VL - 36 IS - 44 SP - 1 EP - 9 PB - Wiley-VCH CY - Weinheim AN - OPUS4-62377 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Arıkan, Muzaffer A1 - Demir, Tuğçe Kahraman A1 - Yıldız, Zeynep A1 - Nalbantoğlu, Özkan Ufuk A1 - Korkmaz, Nur Damla A1 - Yılmaz, Nesrin H. A1 - Şen, Aysu A1 - Özcan, Mutlu A1 - Muth, Thilo A1 - Hanoğlu, Lütfü A1 - Yıldırım, Süleyman T1 - Metaproteogenomic analysis of saliva samples from Parkinson's disease patients with cognitive impairment N2 - Cognitive impairment (CI) is very common in patients with Parkinson’s Disease (PD) and progressively develops on a spectrum from mild cognitive impairment (PD-MCI) to full dementia (PDD). Identification of PD patients at risk of developing cognitive decline, therefore, is unmet need in the clinic to manage the disease. Previous studies reported that oral microbiota of PD patients was altered even at early stages and poor oral hygiene is associated with dementia. However, data from single modalities are often unable to explain complex chronic diseases in the brain and cannot reliably predict the risk of disease progression. Here, we performed integrative metaproteogenomic characterization of salivary microbiota and tested the hypothesis that biological molecules of saliva and saliva microbiota dynamically shift in association with the progression of cognitive decline and harbor discriminatory key signatures across the spectrum of CI in PD. We recruited a cohort of 115 participants in a multi-center study and employed multi-omics factor analysis (MOFA) to integrate amplicon sequencing and metaproteomic analysis to identify signature taxa and proteins in saliva. Our baseline analyses revealed contrasting interplay between the genus Neisseria and Lactobacillus and Ligilactobacillus genera across the spectrum of CI. The group specific signature profiles enabled us to identify bacterial genera and protein groups associated with CI stages in PD. Our study describes compositional dynamics of saliva across the spectrum of CI in PD and paves the way for developing non-invasive biomarker strategies to predict the risk of CI progression in PD. KW - Cognitive impairment (CI) KW - Parkinson’s disease (PD) KW - Metaproteogenomic analysis KW - Saliva sample PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-624228 DO - https://doi.org/10.1038/s41522-023-00452-x SN - 2055-5008 VL - 9 IS - 1 SP - 1 EP - 10 PB - Nature Publ. Group CY - London AN - OPUS4-62422 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 - Völker, Tobias A1 - Mensing, Friedrich A1 - Kruschwitz, Sabine T1 - Estimation of cement content in concrete by spatially resolved laser induced breakdown spectroscopy N2 - The cement content in concrete significantly influences critical properties such as durability, permeability, strength, and workability. Traditional methods for estimating the cement content face limitations. These include the need for comprehensive chemical and solubility knowledge, extensive sample preparation, and their time-consuming and destructive nature. This study investigates the application of laser-induced breakdown spectroscopy (LIBS) as an alternative method. It involves probing concrete samples with high spatial resolution and analyzing the resultant spectra. The methodology is first tested on mesoscale concrete models to assess limitations and inherent errors. Subsequently, the methodology is applied to actual concrete samples with varying cement content and aggregate size distributions. The results demonstrate a promising accuracy, with an average relative error of approximately 8%. This paper offers a comprehensive evaluation of the method's advantages, limitations, and factors influencing its practical applicability in field conditions. KW - LIBS KW - Spectroscopy KW - Cement content KW - Elemental mapping PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-620112 DO - https://doi.org/10.1016/j.cemconres.2024.107714 SN - 1873-3948 VL - 189 SP - 1 EP - 10 PB - Elsevier Ltd. AN - OPUS4-62011 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Saeidfirozeh, H. A1 - Kubelík, P. A1 - Laitl, V. A1 - Krivkova, A. A1 - Vrabel, J. A1 - Rammelkamp, K. A1 - Schroder, S. A1 - Gornushkin, Igor B. A1 - Kepes, E. A1 - Zabka, J. A1 - Ferus, M. A1 - Porízka, P. A1 - Kaiser, J. T1 - Laser-induced breakdown spectroscopy in space applications: Review and prospects N2 - This review describes the principles and summarizes the challenges of analytical methods based on optical emission spectroscopy (OES) in space applications, with a particular focus on Laser-Induced Breakdown Spectroscopy (LIBS). Over the past decade, LIBS has emerged as a powerful analytical technique for space exploration and In-Situ Resource Utilization (ISRU) of celestial bodies. Its implementation has been suggested for various segments of the Space Resources Value Chain, including prospecting, mining, and beneficiation. Current missions to Mars, including the ChemCam instrument on the Curiosity rover, the SuperCam on the Perseverance rover, and the MarSCoDe on the Zhurong rover, are considered flagship applications of LIBS. Despite neither the Pragyan rover nor the Vikram lander waking from the lunar night, the success of the Chandrayaan-3 mission marks another milestone in the development of LIBS instruments, with further missions, including commercial ones, anticipated. This paper reviews the deployment of LIBS payloads on Mars rovers, upcoming missions prospecting the Moon and asteroids, and LIBS analysis of meteorites. Additionally, it highlights the importance of data processing specific to space applications, emphasizing recent trends in transfer learning. Furthermore, LIBS combined with other spectroscopic techniques (e.g., Raman Spectroscopy, Mass Spectrometry, and Fourier-Transform Infrared Spectroscopy) represents an intriguing platform with comprehensive analytical capabilities. The review concludes by emphasizing the significance of LIBS-based contributions in advancing our understanding of celestial bodies and paving the way for future space exploration endeavors KW - Laser-induced breakdown spectroscopy KW - Mars KW - Moon KW - Asteroids KW - Meteorites KW - Machine learning KW - Transfer learning KW - Raman spectroscopy KW - Mass spectrometry KW - Fourier-transform infrared spectroscopy PY - 2024 DO - https://doi.org/10.1016/j.trac.2024.117991 VL - 181 SP - 1 EP - 22 PB - Elsevier B.V. AN - OPUS4-62142 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Westwood, Steven A1 - Lippa, Katrice A1 - Shimuzu, Yoshitaka A1 - Lalerle, Beatrice A1 - Saito, Takeshi A1 - Duewer, David A1 - Dai, Xinhua A1 - Davies, Stephen A1 - Ricci, Marina A1 - Baldan, Annarita A1 - Lang, Brian A1 - Sarge, Stefan A1 - Wang, Haifeng A1 - Pratt, Ken A1 - Josephs, Ralf A1 - Mariassy, Mikael A1 - Pfeifer, Dietmar A1 - Warren, John A1 - Bremser, Wolfram A1 - Ellison, Stephen A1 - Toman, Blaza A1 - Nelson, Michael A1 - Huang, Ting A1 - Fajgelj, Ales A1 - Gören, Ahmet A1 - Mackay, Lindsey A1 - Wielgosz, Robert T1 - Methods for the SI-traceable value assignment of the purity of organic compounds (IUPAC Technical Report) N2 - The “purity” of an organic compound typically refers, in practice, to an assignment of the mass fraction content of the primary organic component present in the material. The “purity” value of an organic primary calibrator material is the ultimate source of metrological traceability of any quantitative measurement of the content of that compound in a given matrix. The primary calibrator may consist of a Certified Reference Material (CRM) whose purity has been assigned by the CRM producer or a laboratory may choose to value-assign a material to the extent necessary for their intended application by using appropriately valid methods. This report provides an overview of the approach, performance and applicability of the principal methods used to determine organic purity including mass balance, quantitative NMR, thermal methods and direct-assay techniques. A statistical section reviews best practice for combination of data, value assignment as the upper limit values corresponding to 100 % purity are approached and how to report and propagate the standard uncertainty associated with the assigned values. KW - Calibration hierarchy KW - Certified reference materials KW - Mass balance KW - Measurement uncertainty KW - Organic purity KW - Primary calibrators KW - Primary reference materials KW - qNMR KW - Related-structure impurities KW - Thermal analysis KW - Titrimetry KW - Traceability KW - Uncertainty propagation KW - Volatile organic compounds KW - Water content PY - 2023 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-627932 DO - https://doi.org/10.1515/pac-2020-0804 SN - 0033-4545 SN - 1365-3075 VL - 95 IS - 1 SP - 1 EP - 77 PB - de Gruyter CY - Berlin AN - OPUS4-62793 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Sparber‐Sauer, Monika A1 - Ferrari, Andrea A1 - Kosztyla, Daniel A1 - Ladenstein, Ruth A1 - Cecchetto, Giovanni A1 - Kazanowska, Bernarda A1 - Scarzello, Giovanni A1 - Ljungman, Gustaf A1 - Milano, Giuseppe Maria A1 - Niggli, Felix A1 - Alaggio, Rita A1 - Vokuhl, Christian A1 - Casanova, Michela A1 - Klingebiel, Thomas A1 - Zin, Angelica A1 - Koscielniak, Ewa A1 - Bisogno, Gianni T1 - Long‐term results from the multicentric European randomized phase 3 trial CWS/RMS‐96 for localized high‐risk soft tissue sarcoma in children, adolescents, and young adults N2 - Background: CWS/RMS‐96 was an international multicenter trial with randomization between two therapy arms of the standard four‐drug therapy (vincristine, ifosfamide, adriamycin, dactinomycin [VAIA]) versus an intensified six‐drug regimen (carboplatin, epirubicin, vincristine, dactinomycin, ifosfamide, and etoposide [CEVAIE]) for high‐risk rhabdomyosarcoma (RMS), extraskeletal Ewing sarcoma (EES), and undifferentiated sarcoma (UDS) in children, adolescents, and young adults aiming to improve their survival. Intensified chemotherapy with CEVAIE did not improve outcome. Methods: Patients younger than 21 years with a previously untreated localized HR‐RMS, EES, and UDS were enrolled from Cooperative Weichteilsarkom Studiengruppe (CWS) centers in Germany, Austria, Poland, Switzerland, and from Italian Soft Tissue Sarcoma Committee (STSC) centers. Randomization (1:1) to receive either 9 × 21 days cycles of VAIA or CEVAIE was performed separately in CWS and STSC. Hyperfractionated accelerated radiotherapy (32–44.8 Gy) was added at week 9–12 according to histology and response to chemotherapy. A secondary microscopically complete nonmutilating resection was performed if possible. Primary endpoints were response to chemotherapy, event‐free (EFS) and overall survival (OS). Results: Five hundred fifty‐seven patients (HR‐RMS:n = 416, EES and UDS:n = 141) underwent randomization: VAIA (n = 273) or CEVAIE (n = 284). Radiotherapy was given to 70% of patients in both groups. A secondary resection was performed in 47% and 48% patients, respectively. The 5‐year EFS and OS for the VAIA and CEVAIE treatment arms were 59.8% and 60.8% (p = .89), and 74.2% and 68.3% (p = .16), respectively. No differences in response, toxicity, or second malignancies emerged in the two groups. Conclusion: The use of an intensified regimen failed to show a significant improvement in tumor response and outcome of patients with localized HR‐RMS, EES, and UDS. KW - CEVAIE KW - CWS-96 KW - High-risk soft tissue sarcoma KW - Randomization KW - Rhabdomyosarcoma KW - RMS-96 KW - VAIA PY - 2022 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-629373 DO - https://doi.org/10.1002/pbc.29691 SN - 1545-5017 VL - 69 IS - 9 SP - 1 EP - 11 PB - Wiley CY - New York, NY AN - OPUS4-62937 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -