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dc.contributor.authorPaglia, Giuseppe
dc.contributor.authorAngel, Peggi
dc.contributor.authorWilliams, Jonathan P
dc.contributor.authorRichardson, Keith
dc.contributor.authorOlivos, Hernando J
dc.contributor.authorThompson, J Will
dc.contributor.authorMenikarachchi, Lochana
dc.contributor.authorLai, Steven
dc.contributor.authorWalsh, Callee
dc.contributor.authorMoseley, Arthur
dc.contributor.authorPlumb, Robert S
dc.contributor.authorGrant, David F
dc.contributor.authorPalsson, Bernhard O
dc.contributor.authorLangridge, James
dc.contributor.authorGeromanos, Scott
dc.contributor.authorAstarita, Giuseppe
dc.date.accessioned2016-03-07T16:12:20Zen
dc.date.available2016-03-07T16:12:20Zen
dc.date.issued2015-01-20en
dc.date.submitted2016en
dc.identifier.citationAnal. Chem. 2015, 87 (2):1137-44en
dc.identifier.issn1520-6882en
dc.identifier.pmid25495617en
dc.identifier.doi10.1021/ac503715ven
dc.identifier.urihttp://hdl.handle.net/2336/600753en
dc.descriptionTo access publisher's full text version of this article, please click on the hyperlink in Additional Links field or click on the hyperlink at the top of the page marked Files. This article is open access.en
dc.description.abstractDespite recent advances in analytical and computational chemistry, lipid identification remains a significant challenge in lipidomics. Ion-mobility spectrometry provides an accurate measure of the molecules' rotationally averaged collision cross-section (CCS) in the gas phase and is thus related to ionic shape. Here, we investigate the use of CCS as a highly specific molecular descriptor for identifying lipids in biological samples. Using traveling wave ion mobility mass spectrometry (MS), we measured the CCS values of over 200 lipids within multiple chemical classes. CCS values derived from ion mobility were not affected by instrument settings or chromatographic conditions, and they were highly reproducible on instruments located in independent laboratories (interlaboratory RSD < 3% for 98% of molecules). CCS values were used as additional molecular descriptors to identify brain lipids using a variety of traditional lipidomic approaches. The addition of CCS improved the reproducibility of analysis in a liquid chromatography-MS workflow and maximized the separation of isobaric species and the signal-to-noise ratio in direct-MS analyses (e.g., "shotgun" lipidomics and MS imaging). These results indicate that adding CCS to databases and lipidomics workflows increases the specificity and selectivity of analysis, thus improving the confidence in lipid identification compared to traditional analytical approaches. The CCS/accurate-mass database described here is made publicly available.
dc.description.sponsorshipNIH/GM087714 eu-repo/grantAgreement/EC/FP7/232816 Alzheimer's Association/NIRG-11-203674en
dc.language.isoenen
dc.publisherAmer Chemical Socen
dc.relationinfo:eu-repo/grantAgreement/EC/FP7/232816en
dc.relation.urlhttp://dx.doi.org/10.1021/ac503715ven
dc.relation.urlhttp://www.ncbi.nlm.nih.gov/pmc/articles/PMC4302848/en
dc.relation.urlhttp://pubs.acs.org/doi/pdf/10.1021/ac503715ven
dc.rightsopenAccessen
dc.subjectAldraðiren
dc.subject.meshAgeden
dc.subject.meshBrainen
dc.subject.meshChromatography, Liquiden
dc.subject.meshHumansen
dc.subject.meshLipidsen
dc.subject.meshSignal-To-Noise Ratioen
dc.subject.meshSpectrometry, Mass, Secondary Ionen
dc.titleIon mobility-derived collision cross section as an additional measure for lipid fingerprinting and identification.en
dc.typearticleen
dc.contributor.department[ 1 ] Ist Zooprofilatt Sperimentale Puglia & Basilicata, Foggia, Italy [ 2 ] Univ Iceland, Ctr Syst Biol, Reykjavik, Iceland [ 3 ] Protea Biosci Grp Inc, Morgantown, WV 26505 USA [ 4 ] Waters Corp, Milford, MA 01757 USA [ 5 ] Duke Prote Core Facil, Durham, NC 27708 USA [ 6 ] Univ Connecticut, Dept Pharmaceut Sci, Storrs, CT 06268 USA [ 7 ] Univ London Imperial Coll Sci Technol & Med, Fac Med, Dept Surg & Canc, London, England [ 8 ] Georgetown Univ, Dept Biochem & Mol & Cellular Biol, Washington, DC 20057 USAen
dc.identifier.journalAnalytical chemistryen
dc.rights.accessOpen Accessen
refterms.dateFOA2018-09-12T15:48:16Z
html.description.abstractDespite recent advances in analytical and computational chemistry, lipid identification remains a significant challenge in lipidomics. Ion-mobility spectrometry provides an accurate measure of the molecules' rotationally averaged collision cross-section (CCS) in the gas phase and is thus related to ionic shape. Here, we investigate the use of CCS as a highly specific molecular descriptor for identifying lipids in biological samples. Using traveling wave ion mobility mass spectrometry (MS), we measured the CCS values of over 200 lipids within multiple chemical classes. CCS values derived from ion mobility were not affected by instrument settings or chromatographic conditions, and they were highly reproducible on instruments located in independent laboratories (interlaboratory RSD < 3% for 98% of molecules). CCS values were used as additional molecular descriptors to identify brain lipids using a variety of traditional lipidomic approaches. The addition of CCS improved the reproducibility of analysis in a liquid chromatography-MS workflow and maximized the separation of isobaric species and the signal-to-noise ratio in direct-MS analyses (e.g., "shotgun" lipidomics and MS imaging). These results indicate that adding CCS to databases and lipidomics workflows increases the specificity and selectivity of analysis, thus improving the confidence in lipid identification compared to traditional analytical approaches. The CCS/accurate-mass database described here is made publicly available.


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