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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. In conclusion, 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.

Authors:
 [1];  [1];  [2];  [3];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biosciences Division
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1425337
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Analytical Chemistry
Additional Journal Information:
Journal Volume: 90; Journal Issue: 1; Journal ID: ISSN 0003-2700
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Veličković, Dušan, Chu, Rosalie K., Carrell, Alyssa A., Thomas, Mathew, Paša-Tolić, Ljiljana, Weston, David J., and Anderton, Christopher R. Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS2 Increases Confidence in Both Molecular Identification and Localization. United States: N. p., 2017. Web. doi:10.1021/acs.analchem.7b04319.
Veličković, Dušan, Chu, Rosalie K., Carrell, Alyssa A., Thomas, Mathew, Paša-Tolić, Ljiljana, Weston, David J., & Anderton, Christopher R. Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS2 Increases Confidence in Both Molecular Identification and Localization. United States. https://doi.org/10.1021/acs.analchem.7b04319
Veličković, Dušan, Chu, Rosalie K., Carrell, Alyssa A., Thomas, Mathew, Paša-Tolić, Ljiljana, Weston, David J., and Anderton, Christopher R. Wed . "Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS2 Increases Confidence in Both Molecular Identification and Localization". United States. https://doi.org/10.1021/acs.analchem.7b04319. https://www.osti.gov/servlets/purl/1425337.
@article{osti_1425337,
title = {Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS2 Increases Confidence in Both Molecular Identification and Localization},
author = {Veličković, Dušan and Chu, Rosalie K. and Carrell, Alyssa A. and Thomas, Mathew and Paša-Tolić, Ljiljana and Weston, David J. and Anderton, Christopher R.},
abstractNote = {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. In conclusion, 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.},
doi = {10.1021/acs.analchem.7b04319},
journal = {Analytical Chemistry},
number = 1,
volume = 90,
place = {United States},
year = {2017},
month = {12}
}

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