Shotgun Lipidomics Identifies a Paired Rule for the Presence of Isomeric Ether Phospholipid Molecular Species 英文参考文献.docVIP

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Shotgun Lipidomics Identifies a Paired Rule for the Presence of Isomeric Ether Phospholipid Molecular Species 英文参考文献.doc

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Shotgun Lipidomics Identifies a Paired Rule for the Presence of Isomeric Ether Phospholipid Molecular Species 英文参考文献

ShotgunLipidomicsIdentifiesaPairedRuleforthe PresenceofIsomericEtherPhospholipidMolecular Species KuiYang1,ZhongdanZhao1,RichardW.Gross1,2,XianlinHan1* 1Divisionof Bioorganic ChemistryandMolecularPharmacology, Department ofInternalMedicine,WashingtonUniversitySchoolofMedicine,St. Louis,Missouri,UnitedStatesofAmerica,2DepartmentofChemistry,WashingtonUniversity,St.Louis,Missouri,UnitedStatesofAmerica Background.Etherphospholipidsareabundantmembraneconstituentspresentinelectricallyactivetissues(e.g.,heartand the brain) that play important roles in cellular function. Alterations of ether phospholipid molecular species contents are associatedwithanumberofgeneticdisordersandhumandiseases.Methodology/PrincipalFindings.Herein,thepowerof shotgun lipidomics, in combination withhigh massaccuracy/high resolutionmass spectrometry, wasexplored toidentify a pairedruleforthepresenceofisomericetherphospholipidmolecularspeciesincellularlipidomes.Therulepredictsthatifan etherphospholipidA9-Bispresentinalipidome,itsisomericcounterpartB9-Aisalsopresent(wherethe9representsanether linkage).Thebiochemicalbasisofthisruleresultsfromthefactthattheenzymeswhichparticipateineitherthesequential oxidation of aliphatic alcohols to fatty acids, or the reduction of long chain fatty acids to aliphatic alcohols (metabolic precursors of ether lipid synthesis), are not entirely selective with respect to acyl chain length or degree of unsaturation. Moreover,theenzymaticselectivityfortheincorporationofdifferentaliphaticchainsintotheobligatoryprecursorofether lipids (i.e., 1-O-alkyl-glycero-3-phosphate) is also limited. Conclusions/Significance. This intrinsic amplification of the number of lipid molecular species present in biological membranes predicted by this rule and demonstrated in this study greatly expands the number of ether lipid molecular species present in cellular lipidomes. Application of this rule to mass spectrometricanalysesprovidespredictivecluestothepresenceofspecificmolecularspeciesandg