Article
Biochemistry & Molecular Biology
Shunji Kato, Yusuke Osuka, Saoussane Khalifa, Takashi Obama, Hiroyuki Itabe, Kiyotaka Nakagawa
Summary: This study developed novel analytical methods using LC-MS/MS to determine the peroxidation mechanisms of plasma lipoproteins in healthy subjects, revealing that PC 16:0/18:2;9OOH, PC 16:0/18:2;13OOH, CE 18:2;9OOH, and CE 18:2;13OOH are the predominant isomers indicating radical and/or enzymatic oxidation. Insights gained from this study could potentially contribute to a more effective suppression of oxidative stress in the human body.
Article
Biochemical Research Methods
Pratima Pathak, Anastasia Sarycheva, Matthew A. Baird, Alexandre A. Shvartsburg
Summary: Mass spectrometry and isotopes have been closely linked in scientific research, with stable isotopes playing a crucial role in identification and quantification. Recent studies have successfully differentiated various halogenated aniline isomers through structurally specific splitting methods.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Biochemical Research Methods
Yang Li, Yujiao Qin, Songchang Wei, Ling Ling, Chuan-Fan Ding
Summary: Steroids are important indicators of health and disease. Differentiating between steroids, especially their isomers, can be challenging due to their structural similarities. This study presents a trapped ion mobility spectrometry-mass spectrometry (TIMS-MS) approach based on steroid analogue adduction for specific identification of isomers. The use of dexamethasone (DEX) as a heterodimer enhancer allowed successful separation of isomer pairs in TIMS.
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
(2023)
Article
Biochemical Research Methods
Qiaohong Lin, Pengyun Li, Ruijun Jian, Yu Xia
Summary: A radical-directed dissociation (RDD) approach was developed for characterizing intrachain modifications within phosphoethanolamines (PEs) in bacterial membranes. This method can generate fragment patterns to locate intrachain modifications and identify the fatty acyl chain composition of PEs.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2022)
Article
Biochemical Research Methods
Jing Zhao, Lipeng Qiao, Yu Xia
Summary: In this study, a MS/MS method based on CID-triggered RDD was developed to characterize sphingoid bases in depth. By applying this method in experiments, the structural diversity of sphingoid bases and novel variations in sphingolipid metabolism were revealed.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Chemistry, Analytical
Chia Yen Liew, Hong-Sheng Luo, Ting-Yi Yang, An-Ti Hung, Bryan John Abel Magoling, Charles Pin-Kuang Lai, Chi-Kung Ni
Summary: This study re-examines high mannose N-glycans in multicellular eukaryotes using a new mass spectrometry method, and identifies many previously unreported isomers. A database is constructed for rapid identification of high mannose N-glycan isomers.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Jian Zhang, Zesen Zhang, Ting Jiang, Zhenyu Zhang, Wenjing Zhang, Wei Xu
Summary: In this paper, a photoepoxidation strategy using benzoin as a reagent under UV light and aerobic conditions was proposed. This method provides a rapid and simple approach for identifying and quantifying isomers of unsaturated lipids in complex biological samples. It has the advantages of high accuracy, high yield of diagnostic ions, and has the potential for large-scale analysis of unsaturated lipids.
Article
Chemistry, Analytical
Rianne E. van Outersterp, Pieter C. Kooijman, Jona Merx, Udo F. H. Engelke, Nematollah Omidikia, Mei-Lan H. Tonneijck, Kas J. Houthuijs, Giel Berden, Tessa M. A. Peters, Dirk J. Lefeber, Michel A. A. P. Willemsen, Jasmin Mecinovic, Jeroen J. Jansen, Karlien L. M. Coene, Ron A. Wevers, Thomas J. Boltje, Jos Oomens, Jonathan Martens
Summary: The room-temperature infrared spectra of ion-complexed saccharides recorded in the far-infrared wavelength range can distinguish isomeric saccharides and have high diagnostic value. This approach, combined with liquid chromatography, can identify saccharide biomarkers in complex sample matrices.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Qingyu Hu, Yuting Sun, Xiyan Mu, Yulan Wang, Huiru Tang
Summary: Direct-infusion tandem mass spectrometry (DI-MS/MS) is valuable for quantitative metabolomics, MS imaging, and single cell studies, but cannot differentiate isomers/isobars with similar MS spectral features. In this study, the fragmentation pathways and characteristics of differential ion-mobility spectrometry (DMS) for four organic compounds were comprehensively investigated. A DI-DMS-MS/MS method was developed to simultaneously quantify these compounds. The method showed high accuracy and low limit-of-quantification, and clear differences between human and mouse urine samples were observed.
Review
Chemistry, Multidisciplinary
Floor ter Braak, Hidde Elferink, Kas J. Houthuijs, Jos Oomens, Jonathan Martens, Thomas J. Boltje
Summary: Understanding the structure and stability of difficult-to-characterize ionic intermediates, such as glycosyl cations, is crucial for studying reaction mechanisms. By combining mass spectrometry with infrared ion spectroscopy, the gas-phase structures of glycosyl cations have been determined, providing valuable insights into their reactivity.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Biochemical Research Methods
Xue Zhao, Yu Xia
Summary: This study demonstrates that almost complete structural information of PC or LPC can be inferred from a single spectrum of the bicarbonate anion adducts, including the identity of the headgroup and composition of fatty acyl chains. Applying this method to analyze LPCs in human plasma revealed the presence of multiple isomers.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Biochemical Research Methods
David L. Williamson, Addison E. Bergman, Gabe Nagy
Summary: High-resolution IMS-MS analysis of D-glucose homopolymers with different metal adducts reveals the presence of multiple IMS peaks with relative areas matching the alpha/beta anomer ratio. A mobility fingerprint trend is identified, with beta anomer showing higher mobility for cellooligosaccharides and alpha anomer showing higher mobility for maltooligosaccharides. The presence of a high mobility fourth peak in maltohexaose suggests a potentially highly compacted conformation.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2021)
Article
Biochemistry & Molecular Biology
Lukas Cudlman, Ales Machara, Vladimir Vrkoslav, Miroslav Polasek, Zuzana Bosakova, Stephen J. Blanksby, Josef Cvacka
Summary: The synthesis and mass spectrometry analysis of triacylglycerol estolides (TG-EST) were conducted to facilitate the identification of these biologically active lipids in biological samples.
Article
Chemistry, Analytical
Zili Guo, Peixi Zhu, Xiaoai He, Tianhe Yan, Xianrui Liang
Summary: A method based on ultra-high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry using electrospray ionization was established to identify chemical constituents in pigeon pea leaves ethanol extract. A total of 58 compounds were detected, with 42 compounds unambiguously identified or tentatively assigned. Eight sets of isomers were differentiated by ion trap mass spectrometry based on fragment ion differences, and energy-resolved mass spectrometry was adopted in the study for relative abundance analysis.
JOURNAL OF SEPARATION SCIENCE
(2021)
Article
Chemistry, Analytical
Peng Che, J. Tyler Davidson, Jeroen Kool, Isabelle Kohler
Summary: A comparison of CID and EAD as fragmentation methods for the characterization and identification of synthetic cathinone positional isomers and their metabolites was conducted. The results highlight the important role of EAD fragmentation in enhancing the confidence in structural elucidation of drug metabolites.
ANALYTICA CHIMICA ACTA
(2023)
Article
Biochemistry & Molecular Biology
Lisa Crozier, Reece Foy, Brandon L. Mouery, Robert H. Whitaker, Andrea Corno, Christos Spanos, Tony Ly, Jeanette Gowen Cook, Adrian T. Saurin
Summary: CDK4/6 inhibitors can induce a prolonged G1 arrest, downregulate replisome components, impair origin licencing, and lead to long-lasting effects on tumor growth. This unexpected ability to induce DNA damage provides a rationale for predicting responsive tumor types and effective combination therapies.
Article
Biochemical Research Methods
Van Kelly, Aymen al-Rawi, David Lewis, Georg Kustatscher, Tony Ly
Summary: This paper presents a method for low cell number proteomics analysis using protease digestion of mildly formaldehyde-fixed cells. The method allows for the quantitative characterization of proteomes from rare cell states, including immune cell subsets and cell cycle subphases. The authors demonstrate the usefulness of the method by characterizing the proteome changes across different cell cycle states and identifying periodic proteins that vary throughout the cell cycle. The dataset generated from this method can be used to classify proteomes into cell cycle states and shows potential for use in single-cell proteomics.
MOLECULAR & CELLULAR PROTEOMICS
(2022)
Article
Chemistry, Analytical
Reuben S. E. Young, Clare L. Flakelar, Venkateswara R. Narreddula, Lachlan J. Jekimovs, Jan P. Menzel, Berwyck L. J. Poad, Stephen J. Blanksby
Summary: Separation and identification of fatty acid isomers in biological samples is a challenging task. Researchers have addressed this challenge by derivatizing fatty acids and using mass spectrometry techniques, successfully determining the structure of fatty acids in complex samples.
ANALYTICAL CHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
Amani M. Batarseh, Fatemeh Vafaee, Elham Hosseini-Beheshti, Azadeh Safarchi, Alex Chen, Amy Cohen, Annette Juillard, Nicholas Henry Hunt, Michael Mariani, Todd Mitchell, Georges Emile Raymond Grau
Summary: It is found that the pathogenesis of cerebral malaria can be understood by studying the specific lipid composition in the plasma. There are significant changes in lipid components in the plasma of cerebral malaria patients compared to non-cerebral malaria patients. This study provides important evidence for studying the pathophysiology of cerebral malaria.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Biochemistry & Molecular Biology
Sarah E. Hancock, Eileen Ding, Emma Johansson Beves, Todd Mitchell, Nigel Turner
Summary: Recent advances in single-cell genomics and transcriptomics have greatly improved our understanding of cellular heterogeneity, but single-cell lipidomics methods have lagged behind. However, we have developed a method combining fluorescence-assisted cell sorting and shotgun lipidomics that allows us to detect and quantify a wide range of phosphatidylcholine and sphingomyelin species from single cells. This method can distinguish between different cell lineages and detect subtle differences in the lipidome between cell lines of the same cancer type. It can also be used in conjunction with other single-cell technologies to provide comprehensive multi-omics data on cells with similar phenotypes, advancing our knowledge on cellular heterogeneity.
JOURNAL OF LIPID RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Oisin J. Shiels, Samuel J. P. Marlton, Adam J. Trevitt
Summary: The gas-phase reaction kinetics of the distonic-radical quinazoline cation's two protonation isomers are independently measured using ion-mobility filtering and laser-equipped quadrupole ion-trap mass spectrometry. The variation in protonation sites significantly affects nearby radical reactivity due to through-space electrostatic effects. Quantum chemical methods, such as double-hybrid density functional theory, are required to explain the experimentally measured difference in reactivity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Biochemical Research Methods
Boris Ucur, Oisin J. Shiels, Stephen J. Blanksby, Adam J. Trevitt
Summary: This study reports on the ion-trap mass spectrometry investigation of methanol-catalyzed proton transfer in para-aminobenzoic acid. The results suggest that single-solvent catalyzed intramolecular proton transfer is possible and must be considered during the late stages of electrospray ionization to predict the protonation site(s) and ion stability in the presence of solvent molecules.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Cell Biology
Aymen al-Rawi, Edward Kaye, Svitlana Korolchuk, Jane A. Endicott, Tony Ly
Summary: Ordered protein phosphorylation by CDKs is a key mechanism for regulating the cell cycle. We show how CDK1 activity and non-catalytic CDK1 subunits contribute to the choice of substrate and site of phosphorylation using a fixed cell kinase assay and phosphoproteomics. Contrary to the model of CDK1 as an exclusively proline-directed kinase, Cyclin A and Cks1 enhance non-proline-directed phosphorylation, preferably on sites with a +3 lysine residue.
Article
Biochemical Research Methods
Britt S. R. Claes, Andrew P. Bowman, Berwyck L. J. Poad, Ron M. A. Heeren, Stephen J. Blanksby, Shane R. Ellis
Summary: The biological functions of lipids highly depend on their molecular structures, specifically even small changes in structure such as different positions of unsaturation serve as critical indicators for changes in metabolism. However, conventional mass spectrometry imaging faces challenges in differentiating lipid isomers with mixture and structural complexity. Recent advances in ozone-induced dissociation coupled with matrix-assisted laser desorption/ionization have shown potential in mapping individual double-bond isomers and visualizing lipid desaturation in adjacent tissue types. This study employs a high-speed gas-phase reaction between ionized lipids and ozone to interrogate anionic glycerophospholipids isomers in biological tissues, providing valuable information on unsaturation and acyl chain composition from a single mass spectrum.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2023)
Article
Chemistry, Analytical
J. C. McKinnon, H. H. Milioli, C. A. Purcell, C. L. Chaffer, B. Wadie, T. Alexandrov, T. W. Mitchell, S. R. Ellis
Summary: Matrix-assisted laser desorption/ionisation mass spectrometry imaging (MALDI-MSI) coupled with laser post-ionisation (MALDI-2) has been used to image low molecular weight (LMW) metabolites, revealing alterations in metabolism throughout heterogeneous tissues.
ANALYTICAL METHODS
(2023)
Article
Chemistry, Multidisciplinary
Tyler Fahrenhorst-Jones, David L. Marshall, Jed. M. Burns, Gregory K. Pierens, Robert E. Hormann, Allison M. Fisher, Paul V. Bernhardt, Stephen J. Blanksby, G. Paul Savage, Philip E. Eaton, Craig M. Williams
Summary: Highly strained cage hydrocarbons have been widely used to explore chemical stability and reactivity, probe physical properties, and as bioactive molecules and in materials discovery. However, the nitrogenous congeners have received less attention. This study presents the synthesis of 1-azahomocubane and its comprehensive characterization, physical property analysis, and chemical reactivity investigation. The findings suggest that nitrogen is well tolerated in a highly strained environment.
Article
Medicine, Research & Experimental
Xiwei Fan, Reuben S. E. Young, Antonia Rujia Sun, Brett R. Hamilton, Udhaya Nedunchezhiyan, Ross Crawford, Stephen J. Blanksby, Indira Prasadam
Summary: This study used mass spectrometry imaging to visualize the distribution of lipase enzymes in bone and cartilage tissue sections and correlated them with immunohistochemistry staining results. The results showed that OA patients exhibited increased expression of PLA(2)G(2)A at the superficial and deep cartilage zones, indicating that tissue-specific inhibition of PLA(2)G(2)A may be a potential therapeutic target for OA.
Article
Chemistry, Analytical
Shane R. Ellis, Jesse A. Michael, Shadrack M. Mutuku, Boris Ucur, Tassiani Sarretto, Alan T. Maccarone, Marcel Niehaus, Adam J. Trevitt
Summary: This study reports the development and optimization of a mass spectrometry imaging platform that combines atmospheric-pressure matrix-assisted laser desorption/ionization (AP-MALDI) with plasma postionization and trapped ion mobility spectrometry (TIMS). The researchers discuss optimal parameters for operating the source and characterize the behavior of different lipid classes. They also show the capabilities of the system for lipid imaging using murine brain tissue.
ANALYTICAL CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
Samuel J. P. Marlton, Adam J. Trevitt
Summary: This article discusses the application of laser photodissociation and ion mobility strategies in the separation and detection of isomers. By using different laser techniques and ion mobility strategies, isomers can be accurately separated and identified, leading to a better understanding of their role in biological processes, physiology, and disease.
CHEMICAL COMMUNICATIONS
(2022)