Structural characterization of glycerophospholipids by combinations of ozone- and collision-induced dissociation mass spectrometry: The next step towards "top-down" lipidomics

Pham, H. T., Maccarone, A. T., Thomas, M. C., Campbell, J. L., Mitchell, T. W., & Blanksby, S. J. (2013) Structural characterization of glycerophospholipids by combinations of ozone- and collision-induced dissociation mass spectrometry: The next step towards "top-down" lipidomics. Analyst, 139(1), pp. 204-214.

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The complete structural elucidation of complex lipids, including glycerophospholipids, using only mass spectrometry represents a major challenge to contemporary analytical technologies. Here, we demonstrate that product ions arising from the collision-induced dissociation (CID) of the [M + Na] + adduct ions of phospholipids can be isolated and subjected to subsequent gas-phase ozonolysis-known as ozone-induced dissociation (OzID)-in a linear ion-trap mass spectrometer. The resulting CID/OzID experiment yields abundant product ions that are characteristic of the acyl substitution on the glycerol backbone (i.e., sn-position). This approach is shown to differentiate sn-positional isomers, such as the regioisomeric phosphatidylcholine pair of PC 16:0/18:1 and PC 18:1/16:0. Importantly, CID/OzID provides a sensitive diagnostic for the existence of an isomeric mixture in a given sample. This is of very high value for the analysis of tissue extracts since CID/OzID analyses can reveal changes in the relative abundance of isomeric constituents even within different tissues from the same animal. Finally, we demonstrate the ability to assign carbon-carbon double bond positions to individual acyl chains at specific backbone positions by adding subsequent CID and/or OzID steps to the workflow and that this can be achieved in a single step using a hybrid triple quadrupole-linear ion trap mass spectrometer. This unique approach represents the most complete and specific structural analysis of lipids by mass spectrometry demonstrated to date and is a significant step towards comprehensive top-down lipidomics. This journal is © The Royal Society of Chemistry 2014.

Grant Number

ARC/DP0986628, ARC/FT110100249, ARC/LP110200648

Impact and interest:

20 citations in Scopus
20 citations in Web of Science®
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ID Code: 68928
Item Type: Journal Article
Refereed: Yes
Keywords: ARC
DOI: 10.1039/c3an01712e
ISSN: 00032654 (ISSN)
Subjects: Australian and New Zealand Standard Research Classification > CHEMICAL SCIENCE (030000) > ANALYTICAL CHEMISTRY (030100) > Analytical Chemistry not elsewhere classified (030199)
Divisions: Current > QUT Faculties and Divisions > Science & Engineering Faculty
Copyright Owner: RSC
Deposited On: 20 Mar 2014 04:10
Last Modified: 09 Apr 2014 12:21

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