Article
Chemistry, Multidisciplinary
David S. Roberts, Morgan Mann, Brad H. Li, Donguk Kim, Allan R. Braiser, Song Jin, Ying Ge
Summary: The SARS-CoV-2 Omicron variant has multiple spike mutations that enhance transmissibility and evasion of neutralizing antibodies. By using high-resolution mass spectrometry, researchers have identified novel glycosite and glycoform changes in the Omicron variant, which can provide insights for the rational design of vaccines and therapeutics.
Article
Chemistry, Analytical
Hany A. Majeed, Tijmen S. Bos, Robert L. C. Voeten, Ruben F. Kranenburg, Arian C. van Asten, Govert W. Somsen, Isabelle Kohler
Summary: A method using trapped ion mobility spectrometry and time-of-flight mass spectrometry was developed to identify different ring-positional isomers in synthetic cathinones. The method allows for accurate ion mobility assessment and high-confidence isomer identification through narrow ion-trapping regions, internal reference mobility calibration, and a dedicated data analysis tool. The method was successfully applied to the unambiguous assignment of isomers in confiscated street samples.
ANALYTICA CHIMICA ACTA
(2023)
Article
Biochemical Research Methods
Robert P. Pellegrinelli, Lei Yue, Eduardo Carrascosa, Ahmed Ben Faleh, Stephan Warnke, Priyanka Bansal, Thomas R. Rizzo
Summary: This article presents a systematic method of identifying reducing-end anomers of glycans using ultrahigh-resolution ion mobility, collision-induced dissociation, and cryogenic infrared spectroscopy. The results confirm that the infrared spectra can rapidly identify precursor glycans with a single anomer.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2022)
Article
Engineering, Chemical
Fateme Banihashemi, Jerry Y. S. Lin
Summary: This study investigates the influence of xylene activity on the vapor and liquid permeation/separation performance of b-oriented MFI zeolite membranes. The results showed that the permeance and separation factor increase with temperature, but decrease with increasing xylene activity. B-oriented MFI zeolite membranes exhibit better vapor permeation/separation performance compared to randomly oriented membranes, and show less negative effect of xylene activity on separation factor. However, both types of membranes show poor separation factor when operated in the pervaporation mode.
JOURNAL OF MEMBRANE SCIENCE
(2022)
Article
Biology
Hao Yan, Julia Lockhauserbaeumer, Gergo Peter Szekeres, Alvaro Mallagaray, Robert Creutznacher, Stefan Taube, Thomas Peters, Kevin Pagel, Charlotte Uetrecht
Summary: Research indicates that the determination of specific glycan binding affinities from native mass spectrometry (MS) must be interpreted cautiously, as the degree of glycan clustering during electrospray ionization depends on the physicochemical properties of the protein studied. The mass fraction of beta-sheets in the protein has a strong influence on the glycan clustering, highlighting the importance of selecting a suitable reference protein for analysis.
Article
Biochemical Research Methods
Raquel Gonzalez de Vega, Alex Cameron, David Clases, Tyren M. Dodgen, Philip A. Doble, David P. Bishop
Summary: PFAS, a large group of synthetic organic compounds widely used in consumer and industrial products, have become widespread in the environment. Global regulations requiring monitoring of PFAS have been implemented due to their potential health and eco-toxicological effects. Targeted methods monitor a small fraction of PFAS compounds, while there is growing interest in complementary non-targeted methods to screen and identify unknown PFAS compounds.
JOURNAL OF CHROMATOGRAPHY A
(2021)
Article
Engineering, Environmental
Hongxin Mu, Jiawei Wang, Ling Chen, Haidong Hu, Jinfeng Wang, Cheng Gu, Hongqiang Ren, Bing Wu
Summary: This study identified and characterized 38 branched isomers of 14 typical PFASs in wastewater samples from 148 municipal WWTPs in China. Linear PFASs had higher detection rates than branched isomers, and the proportion of branched isomers increased in the effluents compared to the influents. Conventional biological treatment processes had poor removal efficiency for both linear PFASs and branched isomers. The isomer composition in the WWTPs showed differences among regions, with the usage of short-chain PFASs being a key factor.
Article
Chemistry, Analytical
Guinevere S. M. Lageveen-Kammeijer, Sander Wagt, Noortje de Haan, Wenjun Wang, Tao Zhang, Manfred Wuhrer
Summary: This study established a zero flow approach using capillary electrophoresis and (tandem) mass spectrometry to characterize isomeric N-glycans at high sensitivity. Diagnostic fragment ion ratios were also identified to indicate the antenna carrying specifically linked sialic acids. In total, 208 N-glycans were characterized in human plasma, with 57 compositions showing multiple isomers.
ANALYTICAL CHEMISTRY
(2022)
Article
Pharmacology & Pharmacy
Zhigang Liang, Huanhuan Wang, Fangling Wu, Longfei Wang, Chenwei Li, Chuan-Fan Ding
Summary: Drug adulteration and contamination pose serious threats to human health, making accurate monitoring crucial. In this study, the drug isomers of Alp/Hyt and Thp/Thm were mixed with cyclodextrins (CD) and metal ions, and separated using trapped ion mobility spectrometry-mass spectrometry (TIMS-MS). The results showed successful separation of the isomers through the formation of binary or ternary complexes with CD and metal ions. The proposed method offers an effective strategy for the detection of isomer adulteration in drugs, with advantages of fast speed, simple operation, high sensitivity, and no chromatographic separation required.
JOURNAL OF PHARMACEUTICAL ANALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Michael C. Pfrunder, David L. Marshall, Berwyck L. J. Poad, Therese M. Fulloon, Jack K. Clegg, Stephen J. Blanksby, John C. McMurtrie, Kathleen M. Mullen
Summary: Ultra-high-resolution cyclic ion-mobility mass spectrometry (cIM-MS) is used to resolve stereoisomers of coordination cages, and complementary NMR experiments can assign the point groups. This method allows for the identification and interrogation of individual isomers in complex mixtures that cannot be performed in solution. Additionally, the stability of individual isomers within the mixture can be probed, with T-symmetric isomers found to be more stable than C-3 and S-4 analogues.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemical Research Methods
Christian Manz, Michael Goetze, Clemens Frank, Andreas Zappe, Kevin Pagel
Summary: LC-MS is an important tool for the comprehensive characterization of N-glycans. However, the measurement times of HILIC chromatography remain a bottleneck in glycan analysis. This study demonstrates the use of an internal calibration strategy to speed up glycan analysis by reducing the number of utilized calibrant. The minimized calibrant shows accurate calibration and can be applied in HPLC runs without modification.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2022)
Review
Chemistry, Analytical
Daniel G. Delafield, Gaoyuan Lu, Cameron J. Kaminsky, Lingjun Li
Summary: Mass spectrometry-based biomolecular analyses have become popular in research settings. Gas phase ion separation techniques provide a fourth dimension of analysis, enabling rapid characterization and high throughput profiling. This review highlights the latest developments and applications of high-end ion-mobility enabled instruments and their advantages for biomolecular research.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2022)
Article
Nanoscience & Nanotechnology
Jiyang Wu, Haolin Wu, Bin Wang, Rongfei Zhou, Weihong Xing
Summary: This study presents the scalable fabrication of high-performance zeolite MFI membranes by single-step secondary growth on alumina monoliths. The monolithic membranes show higher packing density and mechanical strength compared to tubular ones. The separation performance of the monolithic membranes in butane isomer mixtures was evaluated and shows great potential.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Analytical
Lidia Belova, Alberto Celma, Glenn Van Haesendonck, Filip Lemiere, Juan Vicente Sancho, Adrian Covaci, Alexander L. N. van Nuijs, Lubertus Bijlsma
Summary: The number of open access databases containing experimental and predicted collision cross section (CCS) values is increasing, which is important for compound identification. However, the reproducibility of reference values with different instrumental designs and the comparison between predicted and experimental CCS values is still being evaluated. This study compared experimental CCS values of 56 small molecules acquired by both drift tube (DT) and travelling wave (TW) ion mobility mass spectrometry (IM-MS). The results showed good correlation between the datasets of the two methods. Prediction models based on artificial neural networks (ANN) and multivariate adaptive regression splines (MARS) were also found to be applicable for the prediction of CCS values. Recommendations for database transfer and applications of prediction models are provided for future studies.
ANALYTICA CHIMICA ACTA
(2022)
Article
Chemistry, Multidisciplinary
Yi Liu, Mingrun Li, Zhigang Chen, Yi Cui, Jinming Lu, Yi Liu
Summary: Introducing hierarchy enables concurrent thickness reduction and orientation control of zeolite membranes, leading to enhanced performance. Hollow-structured MFI nanoseeds and single-mode microwave heating are crucial for preparing superior butane isomer separation performance of MFI zeolite membranes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Biochemical Research Methods
Ellen D. Inutan, Dean R. Jarois, Christopher B. Lietz, Tarick J. El-Baba, Efstathios A. Elia, Santosh Karki, Andjoe A. S. Sampat, Casey D. Foley, David E. Clemmer, Sarah Trimpin
Summary: By studying ubiquitin using IMS-MS with new ionization processes and different ion sources, researchers were able to compare mass-to-charge and drift time measurements for ubiquitin ions obtained through different ionization methods and found both similarities and differences in the structural features within the elongated distribution of structures. This suggests that the protein structures observed with ESI- or MAI-generated ions may not necessarily reflect the solution structures of the protein prior to ionization.
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
(2021)
Article
Biochemical Research Methods
Calvin A. Austin, Ellen D. Inutan, Brian C. Bohrer, Jing Li, Joshua L. Fischer, Kanchana Wijerathne, Casey D. Foley, Christopher B. Lietz, Daniel W. Woodall, Lorelie F. Imperial, David E. Clemmer, Sarah Trimpin, Barbara S. Larsen
Summary: Ion mobility spectrometry mass spectrometry is able to separate differently branched multiply charged ions of star-branched poly(ethylene glycol) oligomers regardless of the ionization method used. The detailed structural characterization of isomers of the star-branched compositions was achieved using a home-built high-resolution ESI IMS-MS instrument. This approach allows for improved gas-phase separations and potential spatially resolved measurements compared to traditional ionization methods.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Biochemical Research Methods
Daniel W. Woodall, Lucas W. Henderson, Shannon A. Raab, Kenji Honma, David E. Clemmer
Summary: The thermal denaturation of holomyoglobin in solution was characterized using ion mobility spectrometry and mass spectrometry techniques to investigate stability and structural changes. Two experimental approaches were utilized to induce thermal denaturation, highlighting the stabilizing effects of heme binding on the protein's stability.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Chemistry, Multidisciplinary
Shannon A. Raab, Tarick J. El-, Daniel W. Woodall, Wen Liu, Yang Liu, Zane Baird, David A. Hales, Arthur Laganowsky, David H. Russell, David E. Clemmer
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Editorial Material
Biochemical Research Methods
David H. Russell, David E. Clemmer
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Biochemical Research Methods
Mirela Sarbu, Ligia Petrica, David E. Clemmer, Zeljka Vukelic, Alina D. Zamfir
Summary: GBM is a malignant and highly aggressive brain tumor with aberrant cell-surface glycosylation patterns in nearly all tumor cells. Profiling of ganglioside mixtures from GBM specimens revealed over 160 distinct components, dominated by GD3 and GT1 forms. The presence of GT1c(d18:1/24:1) was identified as a potential GBM marker for the first time using high performance ion mobility separation mass spectrometry.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Biochemical Research Methods
Shannon A. Raab, Tarick J. El-Baba, Arthur Laganowsky, David H. Russell, Stephen J. Valentine, David E. Clemmer
Summary: The article discusses the impact of differences in time scales between protons and proteins on the conformation trapping during the electrospray process. It highlights the mechanisms of conformational changes and proton exchange at different time scales, as well as the immobilization of protons specific to protein conformations in the vacuum of the mass spectrometer.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Biochemistry & Molecular Biology
Mirela Sarbu, Dragana Fabris, Zeljka Vukelic, David E. Clemmer, Alina D. Zamfir
Summary: Gangliosides play an important role in the central nervous system and can be used as diagnostic markers and potential therapeutic agents. Ion mobility separation mass spectrometry and IMS tandem mass spectrometry were used to study gangliosides in human central nervous system and cerebrospinal fluid. The results demonstrate the potential of IMS MS/MS in biomarker discovery and characterization, and its application in early diagnosis of CNS diseases through molecular fingerprints.
Article
Biochemical Research Methods
Zhi-chao Zhang, David A. Hales, David E. Clemmer
Summary: Diketopiperazine (DKP) formation is an important degradation pathway for peptides and proteins. The kinetics of peptide cleavage through DKP formation have been analyzed for different model peptides at multiple elevated temperatures. The results show that the degradation rate is influenced by the properties of the amino acid residues, with charged or polar side chains leading to faster degradation and nonpolar alkyl side chains providing stability. The stability of the peptides is influenced by various factors, including the presence of bulky groups on the alpha carbon and the preference for cis proline bond favored by the aromatic N-terminus.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2022)
Article
Biochemistry & Molecular Biology
Mirela Sarbu, Raluca Ica, Edie Sharon, David E. Clemmer, Alina D. Zamfir
Summary: CS/DS play crucial roles in the extracellular matrix, and the structural analysis of their domains is essential; IMS MS technique can identify novel CS/DS species and provide important diagnostic fragment ions.
Article
Biochemical Research Methods
Mirela Sarbu, Raluca Ica, Edie Sharon, David E. Clemmer, Alina D. Zamfir
Summary: In this study, an advanced glycomics method based on ion mobility separation mass spectrometry and tandem mass spectrometry was used to characterize the chondroitin sulfate disaccharide domains in BGN. Five distinct disaccharide motifs were identified in BGN, with four showing irregular sulfation patterns. Trisulfated unsaturated and bisulfated saturated disaccharides were found, the latter indicating the non-reducing end of the chains. Structural investigation revealed a rare bisulfated motif, 3-O-sulfated GlcA-4-O-sulfated GalNAc, at the non-reducing end of one or both CS/DS chains in BGN. The influence of these newly identified sequences on cancer cell spreading will be investigated in future studies.
JOURNAL OF MASS SPECTROMETRY
(2023)
Meeting Abstract
Biochemical Research Methods
Jonathan C. Trinidad, Xuyao Zeng, David E. Clemmer
MOLECULAR & CELLULAR PROTEOMICS
(2022)
Article
Biochemistry & Molecular Biology
Xuyao Zeng, Milos Novotny, David E. Clemmer, Jonathan C. Trinidad
Summary: A substantial shortcoming of large-scale datasets is the difficulty in representing and visualizing key features, particularly in the study of glycopeptides and glycans. This paper presents a simple and concise graphical representation method to capture the microheterogeneity of glycan modification at specific sites, and provides visual illustrations of glycans and glycopeptides from various species.
Meeting Abstract
Biochemistry & Molecular Biology
M. Sarbu, Z. Vukelic, D. E. Clemmer, A. D. Zamfir
Article
Chemistry, Multidisciplinary
Santu Bera, Xuewei Dong, Bankala Krishnarjuna, Shannon A. Raab, David A. Hales, Wei Ji, Yiming Tang, Linda J. W. Shimon, Ayyalusamy Ramamoorthy, David E. Clemmer, Guanghong Wei, Ehud Gazit
Summary: This study explores the molecular basis behind the high solubility of the tripeptide Ala-Phe-Ala, demonstrating its unexpectedly high water solubility and unique structure. The research provides insight into the structural basis of solubility and offers a simple and feasible tool for estimation, with implications for peptide drug design, peptide materials, and advancing peptide nanotechnology.
CELL REPORTS PHYSICAL SCIENCE
(2021)