Relative Quantification of Lipid Isomers in Imaging Mass Spectrometry Using Gas-Phase Charge Inversion Ion/Ion Reactions and Infrared Multiphoton Dissociation

Accurate structural identification of lipids in imaging mass spectrometry is critical to properly contextualizing spatial distributions with tissue biochemistry. Gas-phase charge inversion ion/ion reactions alter the ion type prior to dissociation to allow for more structurally informative fragmenta...

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Bibliographic Details
Published in:Analytical chemistry (Washington) 2023-12, Vol.95 (48), p.17766-17775
Main Authors: Bonney, Julia R, Kang, Woo-Young, Specker, Jonathan T, Liang, Zhongling, Scoggins, 4th, Troy R, Prentice, Boone M
Format: Article
Language:English
Subjects:
Animal tissues
Animals
Anions
Brain
Carbon
Composition
Dissociation
Fragmentation
Infrared lasers
Ion charge
Ionization
Isomers
Lecithin
Lipids
Mass spectrometry
Mass spectroscopy
Medical imaging
Neuroimaging
Phosphatidylcholine
Phosphatidylcholines - chemistry
Rats
Reaction products
Reagents
Scientific imaging
Spatial distribution
Spectrometry, Mass, Electrospray Ionization - methods
Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization
Workflow
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Summary:Accurate structural identification of lipids in imaging mass spectrometry is critical to properly contextualizing spatial distributions with tissue biochemistry. Gas-phase charge inversion ion/ion reactions alter the ion type prior to dissociation to allow for more structurally informative fragmentation and improve lipid identification at the isomeric level. In this work, infrared multiphoton dissociation (IRMPD) was interfaced with a commercial hybrid Qh-FT-ICR mass spectrometer to enable the rapid fragmentation of gas-phase charge inversion ion/ion reaction products at every pixel in imaging mass spectrometry experiments. An ion/ion reaction between phosphatidylcholine (PC) monocations generated from rat brain tissue via matrix-assisted laser desorption/ionization (MALDI) and 1,4-phenylenediproprionic acid reagent dianions generated via electrospray ionization (ESI) followed by IRMPD of the resulting product ion complex produces selective fatty acyl chain cleavages indicative of fatty acyl carbon compositions in the lipid. Ion/ion reaction images using this workflow allow for mapping of the relative spatial distribution of multiple PC isomers under a single sum composition lipid identification. Lipid isomers display significantly different relative spatial distributions within rat brain tissue, highlighting the importance of resolving isomers in imaging mass spectrometry experiments.
ISSN:0003-2700
1520-6882
1520-6882
DOI:10.1021/acs.analchem.3c03804