TY - JOUR A1 - Taylor, Tristen L. A1 - Tukhmetova, Dariya A1 - Duong, Thi Phuong Thanh A1 - Böwe, Anna-Maria A1 - Meermann, Björn A1 - Gundlach-Graham, Alexander T1 - Comparative study of the vibrating capillary nebulizer (VCN) and commercially available interfaces for on-line coupling of capillary electrophoresis with ICP-MS N2 - Capillary electrophoresis (CE) is a powerful and sensitive tool for speciation analysis when combined with inductively coupled plasma mass spectrometry (ICP-MS); however, the performance of this technique can be limited by the nature of pneumatic nebulizers. This study compares two commercially available pneumatic nebulizers to a newly introduced vibrating capillary nebulizer (VCN) for on-line coupling of CE with ICP-MS. The VCN is a low-cost, non-pneumatic nebulizer that is based on the design of capillary vibrating sharp-edge spray ionization. As a piezoelectrically driven nebulization source, the VCN creates an aerosol independent of gas flows and does not produce a low-pressure region at the nebulizer orifice. To compare the systems, we performed replicate analyses of sulfate in river water with each nebulizer and the same CE and ICP-MS instruments and determined the figures of merit of each setup. With the CE-VCN-ICP-MS setup, we achieved around 2–4 times lower sensitivity compared to the commercial setups. However, the VCN-based setup provided lower noise levels and better linear correlation from the analysis of calibration standards, which resulted in indistinguishable LOD and LOQ values from the in-house-built VCN-based and commercial setups for CE-ICP-MS analysis. The VCN is found to have the highest baseline stability with a standard deviation of 3500 cts s−1, corresponding to an RSD of 2.7%. High reproducibility is found with the VCN with a peak area RSD of 4.1% between 3 replicate measurements. KW - Speciation analysis KW - Analytical chemistry KW - Surface water PY - 2024 DO - https://doi.org/10.1007/s00216-024-05162-7 SN - 1618-2650 SP - 1 EP - 9 PB - Springer CY - Berlin AN - OPUS4-59472 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Busche, Steffen A. A1 - Vigarani, Giulia A1 - Retzmann, Anika A1 - Meermann, Björn A1 - Börner, Hans G. T1 - Heavy metal on stage: Making ion-exchange resin selective by peptide tetrazine-norbornene ligation N2 - The challenge of recycling metal salt-contaminated wastewater is more relevant than ever, and cost-effective materials for specific ion-binding are required. A generic route to functionalize a macroporous polystyrene ion-exchange resin (LR-NH2) via chemoselective inverse electron-demand Diels-Alder (IEDDA) ligation is demonstrated. The resin is modified using accessible endo-/exo-5-norbornene-2-carboxylic acid (Nb-COOH) and a set of tetrazine-functionalized 5mer peptides based on sequence variations of the literature known Cu2+ binding domain HGGGW is employed for the IEDDA ligation. The resulting peptide-functionalized resins (LR-Pz-Peptides) are studied for Cu2+ binding to correlate ion-binding capacity with sequence properties by single bead analysis of metal amounts via inductively-coupled plasma mass spectrometry (ICP-MS). The complexation preferences are demonstrated and utilized for specific binding of Cu2+ versus Ni2+ from 1:1 salt mixture as a model system. Enrichment factors of up to 305 could be realized, which might open the potential for applications in metal recycling or waste water purification. KW - Heavy metals KW - Ion exchange resins KW - Analysis PY - 2024 DO - https://doi.org/10.1016/j.polymer.2023.126608 SN - 0032-3861 VL - 291 SP - 1 EP - 12 PB - Elsevier Ltd. AN - OPUS4-60756 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 - Zweigle, Jonathan A1 - Simon, Fabian A1 - Meermann, Björn A1 - Zwiener, Christian T1 - Can Qualitative Nontarget Data Be Indicative of PFAS Contamination? First Evidence by Correlation with EOF in Environmental Samples N2 - We correlated nontarget screening (NTS) features and extractable organic fluorine (EOF) data for PFAS analysis in environmental samples. Soils, sediments, and ashes from different locations (Germany, France, and Lithuania) (n = 34) were analyzed via liquid chromatography-high-resolution mass spectrometry and high-resolution continuum source-graphite furnace molecular absorption spectrometry. NTS feature prioritization based on mass to carbon (m/C) and mass defect to carbon (MD/C) ratios was applied to discriminate potential PFAS features from common co-extracted organic matrix. Our results show a high correlation between quantitative EOF and the prioritized feature number (R2 = 0.87; rPearson = 0.93) and the total peak area of prioritized features (R2 = 0.97; rPearson = 0.98), while commonly applied MD ranges for filtering showed much weaker correlation with EOF. The observed correlations in PFAS-contaminated samples highlight that MD/C−m/C prioritization is associated with a good indication of the overall PFAS burden as evidenced by EOF. Also, semiquantitative data can be extracted as shown by EOF versus prioritized peak areas. The correlations indicate that weakly fluorinated compounds were negligible and that the EOF was mostly composed of highly fluorinated substances. Our method features the potential to automatically screen large NTS data sets for potential PFAS, determine the contribution of PFAS to EOF, and provide preliminary estimates of the overall PFAS burden. KW - PFAS KW - Non-target Screening KW - Sum parameter PY - 2024 DO - https://doi.org/10.1021/acs.estlett.4c00442 SN - 2328-8930 SP - 1 EP - 6 PB - American Chemical Society (ACS) AN - OPUS4-60754 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 - CONF A1 - Meermann, Björn T1 - Analytical Approaches for PFAS Sum-parameter Analysis – From Materials to Environment N2 - PFAS sind emerging pollutants und sind omnipräsent – sowohl in vielen Produkten als auch in der Umwelt. Aufgrund der Vielzahl an verschiedenen Verbindungen werden dringend neue Analytische Methoden zum Nachweis der PFAS benötigt. Im Rahmen meines eingeladenen Vortrags werden neue elementanalytische Summenparameterverfahren, die in meinem Fachbereich entwickelt wurden, vorgestellt. T2 - Analytisches Seminar Uni Duisburg Essen CY - Duisburg, Germany DA - 26.02.2024 KW - PFAS KW - HR-CS-GFMAS KW - Sum parameter PY - 2024 AN - OPUS4-62240 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Meermann, Björn T1 - Analytical Approaches for PFAS Sum-parameter Analysis – From Materials to Environment N2 - PFAS sind emerging pollutants und sind omnipräsent – sowohl in vielen Produkten als auch in der Umwelt. Aufgrund der Vielzahl an verschiedenen Verbindungen werden dringend neue Analytische Methoden zum Nachweis der PFAS benötigt. Im Rahmen meines eingeladenen Vortrags werden neue elementanalytische Summenparameterverfahren, die in meinem Fachbereich entwickelt wurden, vorgestellt. T2 - GDCh Kolloquium CY - Freiberg, Germany DA - 29.05.2024 KW - PFAS KW - HER-CS-GFMAS KW - Evolution of pollution PY - 2024 AN - OPUS4-62241 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Meermann, Björn T1 - Element Analytical Methods for a Sustainable Transformation of our Society N2 - Ressourcenknappheit benötigt alternative Strategien, um auch nachfolgenden Generationen eine lebenswerte Welt zu erhalten und einen guten Lebensstandard zu gewährleisten. Ein wesentlicher Beitrag hierzu wird die Transformation unserer Gesellschaft hin zu einer Kreislaufwirtschaft (CEco) sein. Bisher ist unsere Wirtschaft nicht dahingehend ausgelegt – ein wesentlicher Beitrag muss seitens der Analytischen Chemie kommen – nur hierüber können Qualitätsstandards und –kontrolle gewährleistet werden Im Rahmen meines eigeladenen Vortrags werden elementanalytisch Methoden, die in meinem Fachbereich entwickelt/angewendet werden, für eine CEco vorgestellt. T2 - Analytica Conference CY - Munich, Germany DA - 11.04.2024 KW - PFAS KW - HR-CS-GFMAS KW - Sum parameter PY - 2024 AN - OPUS4-62242 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Meermann, Björn T1 - Analytical Approaches for PFAS Sum-parameter Analysis – From Materials to Environment N2 - PFAS sind emerging pollutants und sind omnipräsent – sowohl in vielen Produkten als auch in der Umwelt. Aufgrund der Vielzahl an verschiedenen Verbindungen werden dringend neue Analytische Methoden zum Nachweis der PFAS benötigt. Im Rahmen meines eingeladenen Vortrags werden neue elementanalytische Summenparameterverfahren, die in meinem Fachbereich entwickelt wurden, vorgestellt. T2 - Wiley - Free Virtual Event –The Forefront of Environmental Toxicology CY - Online meeting DA - 25.09.2024 KW - HR-CS-GFMAS KW - PFAS KW - Environment PY - 2024 AN - OPUS4-62244 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Meermann, Björn T1 - Discrete element and isotope analytical methods for a sustainable transformation of our society N2 - Ressourcenknappheit benötigt alternative Strategien, um auch nachfolgenden Generationen eine lebenswerte Welt zu erhalten und einen guten Lebensstandard zu gewährleisten. Ein wesentlicher Beitrag hierzu wird die Transformation unserer Gesellschaft hin zu einer Kreislaufwirtschaft (CEco) sein. Bisher ist unsere Wirtschaft nicht dahingehend ausgelegt – ein wesentlicher Beitrag muss seitens der Analytischen Chemie kommen – nur hierüber können Qualitätsstandards und –kontrolle gewährleistet werden. Im Rahmen meines eigeladenen Vortrags werden elementanalytisch Methoden, die in meinem Fachbereich entwickelt/angewendet werden, für eine CEco vorgestellt. T2 - Summer school CY - Poland DA - 31.07.2024 KW - Elemental analysis KW - Division 1.1 KW - Environment - material PY - 2024 AN - OPUS4-62245 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Meermann, Björn T1 - Was macht eigentlich der AK Meermann an der BAM in Berlin? N2 - Der Vortrag wurde im Rahmen des PhD Seminars in Hohenroda de AK Sep. Sciences der GDCh gehalten.Hierin habe ich die Forschungsschwerpunkte meines Fachbereichs vorgestellt und einen Überblick über meine Forschungs-Themenbreite gegeben. T2 - PhD Seminar Hohenroda CY - Hohenroda, Germany DA - 09.01.2024 KW - Umwelt KW - Material KW - Elementanalytik PY - 2024 AN - OPUS4-62246 LA - deu AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Meermann, Björn T1 - Analytical Approaches for PFAS Sum-parameter Analysis N2 - PFAS sind emerging pollutants und sind omnipräsent – sowohl in vielen Produkten als auch in der Umwelt. Aufgrund der Vielzahl an verschiedenen Verbindungen werden dringend neue Analytische Methoden zum Nachweis der PFAS benötigt. Im Rahmen meines eingeladenen Vortrags werden neue elementanalytische Summenparameterverfahren, die in meinem Fachbereich entwickelt wurden, vorgestellt. T2 - PFAS partnership workshop CY - Online meeting DA - 27.03.2024 KW - HR-CS-GFMAS KW - PFAS KW - Environment PY - 2024 AN - OPUS4-62247 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - 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 - Tukhmetova, Dariya A1 - Lisec, Jan A1 - Vogl, Jochen A1 - Meermann, Björn T1 - Development of an Online Isotope Dilution CE/ICP–MS Method for the Quantification of Sulfur in Biological Compounds N2 - We report an analytical methodology for the quantification of sulfur in biological molecules via a speciesunspecific postcolumn isotope dilution (online ID) approach using capillary electrophoresis (CE) coupled online with inductively coupled plasma−mass spectrometry (online ID CE/ICP−MS). The method was optimized using a mixture of standard compounds including sulfate, methionine, cysteine, cystine, and albumin, yielding compound recoveries between 98 and 105%. The quantity of sulfur is further converted to the quantity of the compounds owing to the prior knowledge of the sulfur content in the molecules. The limit of detection and limit of quantification of sulfur in the compounds were 1.3−2.6 and 4.1−8.4 mg L−1, respectively, with a correlation coefficient of 0.99 within the concentration range of sulfur of 5−100 mg L−1. The capability of the method was extended to quantify albumin in its native matrix (i.e., in serum) using experimentally prepared serum spiked with a pure albumin standard for validation. The relative expanded uncertainty of the method for the quantification of albumin was 6.7% (k = 2). Finally, we tested the applicability of the method on real samples by the analysis of albumin in bovine and human sera. For automated data assessment, a software application (IsoCor) which was developed by us in a previous work was developed further for handling of online ID data. The method has several improvements compared to previously published setups: (i) reduced adsorption of proteins onto the capillary wall owing to a special capillary-coating procedure, (ii) baseline separation of the compounds in less than 30 min via CE, (iii) quantification of several sulfur species within one run by means of the online setup, (iv) SI traceability of the quantification results through online ID, and (v) facilitated data processing of the transient signals using the IsoCor application. Our method can be used as an accurate approach for quantification of proteins and other biological molecules via sulfur analysis in complex matrices for various fields, such as environmental, biological, and pharmaceutical studies as well as clinical diagnosis. Sulfur is an essential element in living organisms, where it plays important roles in various biological processes, such as protein synthesis, enzyme activity, and antioxidant defense. However, the biological effects of different sulfur species can vary widely, and imbalances in sulfur speciation have been observed in a range of diseases, including cancer, Alzheimer’s disease, and diabetes.1−3 The accurate quantification of sulfur and its species in biological samples requires sensitive and selective analytical techniques. In recent years, separation techniques coupled online with inductively coupled plasma−mass spectrometry (ICP−MS) have emerged as powerful online analytical tools complementary to molecular spectrometric methods for speciation analysis of biological compounds. External calibration4−9 and isotope dilution (ID)10−15 are common calibration approaches applied for online quantification of sulfur species in complex samples. The ID analysis is advantageous over. KW - Analytical Chemistry KW - CE/MC-ICP-MS KW - species-specific isotope information PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-594736 DO - https://doi.org/10.1021/acs.analchem.3c03553 SN - 0003-2700 SP - 1 EP - 8 PB - American Chemical Society (ACS) AN - OPUS4-59473 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - CONF A1 - Meermann, Björn T1 - Species-specific isotope ratio analysis of proteins via CE/MC-ICP-MS N2 - Klassische Isotopenverhältnisanalyse (stabile IStope) läuft meistens im Rahmen einer bulk Analyse ab. Hierbei geht jedoch die Spezies-Information verloren. Ferner sind bulk Verfahren im Bereich der Probenvorbereitung aufwändig. Im Rahmen meines eingeladenen Vortrags werden neue CE/MC-ICP-MS Verfahren vorgestellt, die in meiner Gruppe entwickelt werden. T2 - 2024 Winter Conference on Plasma Spectrochemistry CY - Tucson, AZ, USA DA - 16.01.2024 KW - CE KW - MC-ICP-MS KW - Species specific isotopes PY - 2024 AN - OPUS4-62239 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER - TY - JOUR A1 - Junge, Florian A1 - Wittwer, Philipp A1 - Sommerfeld, Thomas A1 - Gehrenkemper, Lennart A1 - Zoister, Christian A1 - Nickl, Philip A1 - Koch, Matthias A1 - Meermann, Björn A1 - Haag, Rainer T1 - Adsorber Charge Dominates over Hydrophobic or Fluorophilic Functionalization in Influencing Adsorption of PFCA onto Polystyrene Resins N2 - A systematic series of industrial-relevant polystyrene-based anion exchange resins that are functionalized with hydro- or fluorocarbon chains are compared regarding their adsorption behavior toward perfluorocarboxylic acids (PFCA) in respect to their charge, chain length, and type of chain. The results clearly show the dominance of electrostatic interactions in the adsorption process as uncharged adsorber materials showed no adsorption at all. In contrast, the charged adsorber materials showed in general a PFCA removal of 80% to 30% over the experiment depending on effluent fraction. Unexpectedly, for perfluorobutanoic acid (PFBA) the highest removal rate is found with consistently >90%. Despite observing significant benefits in the adsorption of PFCA for fluoroalkylated adsorbers in comparison to their non-fluorinated counterparts, this effect of fluoroalkylation is comparatively small and can not be clearly attributed to fluorophilic interactions between the fluoroalkyl chains. These findings help clarifying that the introduction of fluorocarbon moieties in adsorber materials is not necessary in order to remove fluorocarbon molecules from the environment. KW - PFAS KW - Remediation KW - Adsorption KW - Fluorophilic interactions PY - 2024 UR - https://nbn-resolving.org/urn:nbn:de:kobv:b43-601883 DO - https://doi.org/10.1002/admi.202400199 SN - 2196-7350 SP - 1 EP - 10 PB - John Wiley & Sons CY - Hoboken, New Jersey, USA AN - OPUS4-60188 LA - eng AD - Bundesanstalt fuer Materialforschung und -pruefung (BAM), Berlin, Germany ER -