Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS2 Increases Confidence in Both Molecular Identification and Localization

Dušan Veličković; Rosalie K. Chu; Alyssa A. Carrell; Mathew Thomas; Ljiljana Paša-Tolić; David J. Weston; Christopher R. Anderton

doi:10.1021/acs.analchem.7b04319

Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS² Increases Confidence in Both Molecular Identification and Localization

Dušan Veličković, Rosalie K. Chu, Alyssa A. Carrell, Mathew Thomas, Ljiljana Paša-Tolić, David J. Weston, Christopher R. Anderton

Plant Systems Biology

Research output: Contribution to journal › Article › peer-review

32 Scopus citations

Abstract

One critical aspect of mass spectrometry imaging (MSI) is the need to confidently identify detected analytes. While orthogonal tandem MS (e.g., LC-MS²) experiments from sample extracts can assist in annotating ions, the spatial information about these molecules is lost. Accordingly, this could cause mislead conclusions, especially in cases where isobaric species exhibit different distributions within a sample. In this Technical Note, we employed a multimodal imaging approach, using matrix assisted laser desorption/ionization (MALDI)-MSI and liquid extraction surface analysis (LESA)-MS²I, to confidently annotate and localize a broad range of metabolites involved in a tripartite symbiosis system of moss, cyanobacteria, and fungus. We found that the combination of these two imaging modalities generated very congruent ion images, providing the link between highly accurate structural information onfered by LESA and high spatial resolution attainable by MALDI. These results demonstrate how this combined methodology could be very useful in differentiating metabolite routes in complex systems.

Original language	English
Pages (from-to)	702-707
Number of pages	6
Journal	Analytical Chemistry
Volume	90
Issue number	1
DOIs	https://doi.org/10.1021/acs.analchem.7b04319
State	Published - Jan 2 2018

Funding

The authors would like to thank Andrew Palmer and Theodore Alexandrov of the European Molecular Biology Laboratory, as well as Dennis Trede and Jan Kobarg of SCiLS Lab, for their advice and help with processing the MSI data. This work was performed at EMSL, a national scientific user facility sponsored by the Office of Biological and Environmental Research (BER), U.S. Department of Energy (DOE). EMSL is located at PNNL, a multidisciplinary national laboratory operated by Battelle for the U.S. DOE. Preparation of the biological samples was performed at ORNL as part of U.S. DOE-BER, Early Career Research Program. ORNL is managed by UT-Battelle, LLC, DE-AC05-00OR22725.

Funders	Funder number
Office of Biological and Environmental Research
U.S. Department of Energy
Biological and Environmental Research

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title = "Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS2 Increases Confidence in Both Molecular Identification and Localization",

abstract = "One critical aspect of mass spectrometry imaging (MSI) is the need to confidently identify detected analytes. While orthogonal tandem MS (e.g., LC-MS2) experiments from sample extracts can assist in annotating ions, the spatial information about these molecules is lost. Accordingly, this could cause mislead conclusions, especially in cases where isobaric species exhibit different distributions within a sample. In this Technical Note, we employed a multimodal imaging approach, using matrix assisted laser desorption/ionization (MALDI)-MSI and liquid extraction surface analysis (LESA)-MS2I, to confidently annotate and localize a broad range of metabolites involved in a tripartite symbiosis system of moss, cyanobacteria, and fungus. We found that the combination of these two imaging modalities generated very congruent ion images, providing the link between highly accurate structural information onfered by LESA and high spatial resolution attainable by MALDI. These results demonstrate how this combined methodology could be very useful in differentiating metabolite routes in complex systems.",

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AU - Thomas, Mathew

AU - Paša-Tolić, Ljiljana

AU - Weston, David J.

AU - Anderton, Christopher R.

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Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS² Increases Confidence in Both Molecular Identification and Localization

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