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

preprint
revised on 17.08.2020 and posted on 18.08.2020 by Katerina Djambazova, Dustin R. Klein, Lukasz Migas, Elizabeth Neumann, Emilio Rivera, Raf Van de Plas, Richard M. Caprioli, Jeffrey Spraggins

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 map-ping of biomolecules in tissue. 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 approximately a ~270% increase in the peak capacity during IMS experiments. MALDI TIMS-MS separation of lipid isomer standards, including sn-backbone isomers, acyl chain isomers, as well as double bond positional and geometric isomers are demonstrated. As a proof-of-concept, in situ separation and imaging of lipid isomers with distinct spatial distributions was performed using tissue sections from a whole-body mouse pup.

Funding

MRI: Development of a next-generation MALDI ion mobility mass spectrometry platform for molecular imaging and training

Directorate for Engineering

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Imaging Mass Spectrometry Research Resource at Vanderbilt University

National Institute of General Medical Sciences

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15 Tesla Bruker SolariX FT-ICR mass spectrometer

Office of the Director

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Training Program in Environmental Toxicology

National Institute of Environmental Health Sciences

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History

Email Address of Submitting Author

jeff.spraggins@vanderbilt.edu

Institution

Vanderbilt University

Country

USA

ORCID For Submitting Author

0000-0001-9198-5498

Declaration of Conflict of Interest

The authors have no conflicts of interest.

Version Notes

Version 2.

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