Quantitative Fragmentation Model for Bottom-Up Shotgun Lipidomics
Quantitative bottom-up shotgun lipidomics relies on molecular species-specific “signature” fragments consistently detectable in tandem mass spectra of analytes and standards. Molecular species of glycerophospholipids are typically quantified using carboxylate fragments of their fatty acid moieties p...
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| Published in | Analytical chemistry (Washington) Vol. 91; no. 18; pp. 12085 - 12093 |
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| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
17.09.2019
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0003-2700 1520-6882 1520-6882 |
| DOI | 10.1021/acs.analchem.9b03270 |
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| Abstract | Quantitative bottom-up shotgun lipidomics relies on molecular species-specific “signature” fragments consistently detectable in tandem mass spectra of analytes and standards. Molecular species of glycerophospholipids are typically quantified using carboxylate fragments of their fatty acid moieties produced by higher-energy collisional dissociation of their molecular anions. However, employing standards whose fatty acids moieties are similar, yet not identical, to the target lipids could severely compromise their quantification. We developed a generic and portable fragmentation model implemented in the open-source LipidXte software that harmonizes the abundances of carboxylate anion fragments originating from fatty acid moieties having different sn-1/2 positions at the glycerol backbone, length of the hydrocarbon chain, and number and location of double bonds. The postacquisition adjustment enables unbiased absolute (molar) quantification of glycerophospholipid species independent of instrument settings, collision energy, and employed internal standards. |
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| AbstractList | Quantitative bottom-up shotgun lipidomics relies on molecular species-specific “signature” fragments consistently detectable in tandem mass spectra of analytes and standards. Molecular species of glycerophospholipids are typically quantified using carboxylate fragments of their fatty acid moieties produced by higher-energy collisional dissociation of their molecular anions. However, employing standards whose fatty acids moieties are similar, yet not identical, to the target lipids could severely compromise their quantification. We developed a generic and portable fragmentation model implemented in the open-source LipidXte software that harmonizes the abundances of carboxylate anion fragments originating from fatty acid moieties having different sn-1/2 positions at the glycerol backbone, length of the hydrocarbon chain, and number and location of double bonds. The postacquisition adjustment enables unbiased absolute (molar) quantification of glycerophospholipid species independent of instrument settings, collision energy, and employed internal standards. Quantitative bottom-up shotgun lipidomics relies on molecular species-specific “signature” fragments consistently detectable in tandem mass spectra of analytes and standards. Molecular species of glycerophospholipids are typically quantified using carboxylate fragments of their fatty acid moieties produced by higher-energy collisional dissociation of their molecular anions. However, employing standards whose fatty acids moieties are similar, yet not identical, to the target lipids could severely compromise their quantification. We developed a generic and portable fragmentation model implemented in the open-source LipidXte software that harmonizes the abundances of carboxylate anion fragments originating from fatty acid moieties having different sn-1/2 positions at the glycerol backbone, length of the hydrocarbon chain, and number and location of double bonds. The postacquisition adjustment enables unbiased absolute (molar) quantification of glycerophospholipid species independent of instrument settings, collision energy, and employed internal standards. Quantitative bottom-up shotgun lipidomics relies on molecular species-specific "signature" fragments consistently detectable in tandem mass spectra of analytes and standards. Molecular species of glycerophospholipids are typically quantified using carboxylate fragments of their fatty acid moieties produced by higher-energy collisional dissociation of their molecular anions. However, employing standards whose fatty acids moieties are similar, yet not identical, to the target lipids could severely compromise their quantification. We developed a generic and portable fragmentation model implemented in the open-source LipidXte software that harmonizes the abundances of carboxylate anion fragments originating from fatty acid moieties having different sn-1/2 positions at the glycerol backbone, length of the hydrocarbon chain, and number and location of double bonds. The postacquisition adjustment enables unbiased absolute (molar) quantification of glycerophospholipid species independent of instrument settings, collision energy, and employed internal standards.Quantitative bottom-up shotgun lipidomics relies on molecular species-specific "signature" fragments consistently detectable in tandem mass spectra of analytes and standards. Molecular species of glycerophospholipids are typically quantified using carboxylate fragments of their fatty acid moieties produced by higher-energy collisional dissociation of their molecular anions. However, employing standards whose fatty acids moieties are similar, yet not identical, to the target lipids could severely compromise their quantification. We developed a generic and portable fragmentation model implemented in the open-source LipidXte software that harmonizes the abundances of carboxylate anion fragments originating from fatty acid moieties having different sn-1/2 positions at the glycerol backbone, length of the hydrocarbon chain, and number and location of double bonds. The postacquisition adjustment enables unbiased absolute (molar) quantification of glycerophospholipid species independent of instrument settings, collision energy, and employed internal standards. |
| Author | Wagner, Nicolai Shevchenko, Andrej Ackerman, Jacobo Miranda Groessl, Michael Nadler, André Schuhmann, Kai Moon, HongKee Thomas, Henrik Kellmann, Markus Henry, Ian |
| AuthorAffiliation | Department of Nephrology and Hypertension Department for BioMedical Research University of Bern Thermo Fisher Scientific |
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| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31441640$$D View this record in MEDLINE/PubMed |
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| Snippet | Quantitative bottom-up shotgun lipidomics relies on molecular species-specific “signature” fragments consistently detectable in tandem mass spectra of analytes... Quantitative bottom-up shotgun lipidomics relies on molecular species-specific "signature" fragments consistently detectable in tandem mass spectra of analytes... Quantitative bottom-up shotgun lipidomics relies on molecular species-specific “signature” fragments consistently detectable in tandem mass spectra of analytes... |
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| SubjectTerms | Analytical chemistry Anions Chemistry Energy of dissociation Fatty acids Fragmentation Fragments Glycerol Ions Lipids Mass spectra Molecular chains Shotguns Source code Species |
| Title | Quantitative Fragmentation Model for Bottom-Up Shotgun Lipidomics |
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