Mapping Unsaturation in Human Plasma Lipids by Data-Independent Ozone-Induced Dissociation

Marshall, David L.; Criscuolo, Angela; Young, Reuben S. E.; Poad, Berwyck L. J.; Zeller, Martin; Reid, Gavin E.; Mitchell, Todd W.; Blanksby, Stephen J.

doi:10.1007/s13361-019-02261-z

Cited by 60 publications

(58 citation statements)

References 64 publications

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“…The number of reported PCs from a given lipidome, however, is typically less than 50, e.g., 41 PCs from human plasma 9 and 14 PCs from yeast, 10 much less than that has been predicted. 11 One reason accounting for the small numbers of detected PCs arises from the fact that current lipid analysis methods do not differentiate structural isomers.…”

Section: Introductionmentioning

confidence: 99%

“…These include electron impact excitation of ions from organics (EIEIO), 23 ozone-induced dissociation (OzID), [24][25][26] and ultraviolet photodissociation (UVPD). 27,28 All these developments greatly expand the toolbox for lipid analysis; more importantly, they not only provide rst-time analysis of lipidomes at the isomer level 11,19,[28][29][30] but also demonstrate the link between altered isomer compositions with disease quantitatively and spatially. [31][32][33][34] Radical-directed fragmentation has attracted increasing attention in MS/MS method development due to its unique capabilities in differentiating structural isomers of biomolecules, which otherwise cannot be obtained from chargedirected fragmentations typically seen from CID.…”

Section: Introductionmentioning

confidence: 99%

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A lipidomic workflow capable of resolving sn- and CC location isomers of phosphatidylcholines

Zhao

Zhang

et al. 2019

Chem. Sci.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

A lipidomic workflow capable of resolving sn- and CC location isomers of phosphatidylcholines

Zhao

Zhang

et al. 2019

Chem. Sci.

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“…Various methods have been explored for differentiating the lipid C=C location and sn-position isomers. Ozone-induced dissociation (OzID) [31][32][33] and ultraviolet photodissociation (UVPD) 28 have been used to determine both sn-positions and C=C locations in GPs. By coupling photochemical (Paternò-Bǜchi, PB) reaction with tandem MS (MS/MS), we have systematically demonstrated the qualitative and quantitative analysis of lipids with C=C specificity from complex biological samples [25][26][27]34,35 .…”

mentioning

confidence: 99%

Large-scale lipid analysis with C=C location and sn-position isomer resolving power

Cao¹,

Cheng²,

Yang³

et al. 2020

Nat Commun

144

183

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Lipids play a pivotal role in biological processes and lipid analysis by mass spectrometry (MS) has significantly advanced lipidomic studies. While the structure specificity of lipid analysis proves to be critical for studying the biological functions of lipids, current mainstream methods for large-scale lipid analysis can only identify the lipid classes and fatty acyl chains, leaving the C=C location and sn-position unidentified. In this study, combining photochemistry and tandem MS we develop a simple but effective workflow to enable large-scale and near-complete lipid structure characterization with a powerful capability of identifying C=C location(s) and sn-position(s) simultaneously. Quantitation of lipid structure isomers at multiple levels of specificity is achieved and different subtypes of human breast cancer cells are successfully discriminated. Remarkably, human lung cancer tissues can only be distinguished from adjacent normal tissues using quantitative results of both lipid C=C location and sn-position isomers.

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“…Subsequent OzID preferentially dissociated the newly formed ring-adjacent DB revealing neighboring FAs. Combined with the ability to identify DBs in OzID MS 2 experiments, this powerful analytic platform has been utilized to structurally characterize SLs [95], GLs [93,95], FAs [96], and GPs [95]. However, ion/molecule reaction yields are often limited by the partial pressure of the regent gas or can contaminate the mass spectrometer if reactions are not carefully optimized.…”

Section: Ion/molecule and Ion/ion Reactionsmentioning

confidence: 99%

Advanced tandem mass spectrometry in metabolomics and lipidomics—methods and applications

Heiles

2021

Anal Bioanal Chem

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Metabolomics and lipidomics are new drivers of the omics era as molecular signatures and selected analytes allow phenotypic characterization and serve as biomarkers, respectively. The growing capabilities of untargeted and targeted workflows, which primarily rely on mass spectrometric platforms, enable extensive charting or identification of bioactive metabolites and lipids. Structural annotation of these compounds is key in order to link specific molecular entities to defined biochemical functions or phenotypes. Tandem mass spectrometry (MS), first and foremost collision-induced dissociation (CID), is the method of choice to unveil structural details of metabolites and lipids. But CID fragment ions are often not sufficient to fully characterize analytes. Therefore, recent years have seen a surge in alternative tandem MS methodologies that aim to offer full structural characterization of metabolites and lipids. In this article, principles, capabilities, drawbacks, and first applications of these “advanced tandem mass spectrometry” strategies will be critically reviewed. This includes tandem MS methods that are based on electrons, photons, and ion/molecule, as well as ion/ion reactions, combining tandem MS with concepts from optical spectroscopy and making use of derivatization strategies. In the final sections of this review, the first applications of these methodologies in combination with liquid chromatography or mass spectrometry imaging are highlighted and future perspectives for research in metabolomics and lipidomics are discussed. Graphical abstract

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Mapping Unsaturation in Human Plasma Lipids by Data-Independent Ozone-Induced Dissociation

Cited by 60 publications

References 64 publications

A lipidomic workflow capable of resolving sn- and CC location isomers of phosphatidylcholines

A lipidomic workflow capable of resolving sn- and CC location isomers of phosphatidylcholines

Large-scale lipid analysis with C=C location and sn-position isomer resolving power

Advanced tandem mass spectrometry in metabolomics and lipidomics—methods and applications

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