Resolving the Complexity of Spatial Lipidomics Using MALDI TIMS Imaging Mass Spectrometry

Lipids are a structurally diverse class of molecules with important biological functions including cellular signaling and energy storage. Matrix-assisted laser desorption/ionization (MALDI) imaging mass spectrometry (IMS) allows for direct mapping of biomolecules in tissues. Fully characterizing the...

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Bibliographic Details
Published in:Analytical chemistry (Washington) 2020-10, Vol.92 (19), p.13290-13297
Main Authors: Djambazova, Katerina V, Klein, Dustin R, Migas, Lukasz G, Neumann, Elizabeth K, Rivera, Emilio S, Van de Plas, Raf, Caprioli, Richard M, Spraggins, Jeffrey M
Format: Article
Language:English
Subjects:
Animals
Biomolecules
Cellular structure
Chemistry
Complexity
Data interpretation
Energy storage
Imaging
Ion Mobility Spectrometry
Ionic mobility
Ionization
Ions
Isomers
Lipidomics
Lipids
Lipids - analysis
Mapping
Mass spectrometry
Mass spectroscopy
Mice
Mice, Inbred C57BL
Mobility
Quadrupoles
Scientific imaging
Separation
Spatial distribution
Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization
Spectroscopy
Stereoisomerism
Stereoisomers
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Summary:Lipids are a structurally diverse class of molecules with important biological functions including cellular signaling and energy storage. Matrix-assisted laser desorption/ionization (MALDI) imaging mass spectrometry (IMS) allows for direct mapping of biomolecules in tissues. Fully characterizing the structural diversity of lipids remains a challenge due to the presence of isobaric and isomeric species, which greatly complicates data interpretation when only m/z information is available. Integrating ion mobility separations aids in deconvoluting these complex mixtures and addressing the challenges of lipid IMS. Here, we demonstrate that a MALDI quadrupole time-of-flight (Q-TOF) mass spectrometer with trapped ion mobility spectrometry (TIMS) enables a >250% increase in the peak capacity during IMS experiments. MALDI TIMS-MS separation of lipid isomer standards, including sn backbone isomers, acyl chain isomers, and double-bond position and stereoisomers, is demonstrated. As a proof of concept, in situ separation and imaging of lipid isomers with distinct spatial distributions were performed using tissue sections from a whole-body mouse pup.
ISSN:0003-2700
1520-6882
DOI:10.1021/acs.analchem.0c02520