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dc.contributor.authorBerthias, Francis
dc.contributor.authorPoad, Berwyck L.J.
dc.contributor.authorThurman, Hayden A.
dc.contributor.authorBowman, Andrew P.
dc.contributor.authorBlanksby, Stephen J.
dc.contributor.authorShvartsburg, Alexandre A.
dc.identifier.citationBerthias, F., Poad, B. L. J., Thurman, H. A., Bowman, A. P., Blanksby, S. J., & Shvartsburg, A. A. (2021). Disentangling lipid isomers by high-resolution differential ion mobility Spectrometry/Ozone-induced dissociation of metalated species. Journal of the American Society for Mass Spectrometry, doi:10.1021/jasms.1c00251en_US
dc.descriptionClick on the DOI link to access the article (may not be free).en_US
dc.description.abstractThe preponderance and functional importance of isomeric biomolecules have become topical in biochemistry. Therefore, one must distinguish and identify all such forms across compound classes, over a wide dynamic range as minor species often have critical activities. With all the power of modern mass spectrometry for compositional assignments by accurate mass, the identical precursor and often fragment ion masses render this task a steep challenge. This is recognized in proteomics and epigenetics, where proteoforms are disentangled and characterized employing novel separations and non-ergodic dissociation mechanisms. This issue is equally pertinent to lipidomics, where the lack of isomeric depth has thwarted the deciphering of functional networks. Here we introduce a new platform, where the isomeric lipids separated by high-resolution differential ion mobility spectrometry (FAIMS) are identified using ozone-induced dissociation (OzID). Cationization by metals (here K+, Ag+, and especially Cu+) broadly improves the FAIMS resolution of isomers with alternative C═C double bond (DB) positions or stereochemistry, presumably via metal attaching to the DB and reshaping the ion around it. However, the OzID yield diminishes for Ag+ and vanishes for Cu+ adducts. Argentination still strikes the best compromise between efficient separation and diagnostic fragmentation for optimal FAIMS/OzID performance.en_US
dc.description.sponsorshipThe work at WSU was funded by the NSF CAREER Award (CHE-1552640). S.J.B. acknowledges support from the Australian Research Council Discovery Program (DP190101486). We thank Matthew A. Baird and Gordon A. Anderson for experimental help.en_US
dc.publisherAmerican Chemical Societyen_US
dc.relation.ispartofseriesJournal of The American Society for Mass Spectrometry;
dc.subjectIon mobility spectrometryen_US
dc.subjectDifferential IMSen_US
dc.subjectTandem MSen_US
dc.subjectOzone-induced dissociationen_US
dc.titleDisentangling lipid isomers by high-resolution differential ion mobility spectrometry/ozone-induced dissociation of metalated speciesen_US
dc.rights.holder© 2021 American Society for Mass Spectrometry. Published by American Chemical Society. All rights reserved.en_US

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