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

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

doi:10.1021/acs.analchem.7b04319

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

Journal Article · Wed Dec 06 00:00:00 EST 2017 · Analytical Chemistry

DOI:https://doi.org/10.1021/acs.analchem.7b04319· OSTI ID:1425337

Veličković, Dušan ^[1]; Chu, Rosalie K. ^[1]; Carrell, Alyssa A. ^[2]; Thomas, Mathew ^[3]; Paša-Tolić, Ljiljana ^[1];

^[2];

^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biosciences Division
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical Sciences Division

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.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1425337

Journal Information:: Analytical Chemistry, Vol. 90, Issue 1; ISSN 0003-2700

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 24 works

Citation information provided by
Web of Science

References (26)

Ultra-High Mass Resolution MALDI Imaging Mass Spectrometry of Proteins and Metabolites in a Mouse Model of Glioblastoma Dilillo, M.; Ait-Belkacem, R.; Esteve, C. Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-00703-w	journal	April 2017
Mannitol in Plants, Fungi, and Plant–Fungal Interactions Patel, Takshay K.; Williamson, John D. Trends in Plant Science, Vol. 21, Issue 6 https://doi.org/10.1016/j.tplants.2016.01.006	journal	June 2016
Overlapping MALDI-Mass Spectrometry Imaging for In-Parallel MS and MS/MS Data Acquisition without Sacrificing Spatial Resolution Hansen, Rebecca L.; Lee, Young Jin Journal of The American Society for Mass Spectrometry, Vol. 28, Issue 9 https://doi.org/10.1007/s13361-017-1699-7	journal	May 2017
Imaging mass spectrometry and MS/MS molecular networking reveals chemical interactions among cuticular bacteria and pathogenic fungi associated with fungus-growing ants Boya P., Cristopher A.; Fernández-Marín, Hermógenes; Mejía, Luis C. Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-05515-6	journal	July 2017
Proposed minimum reporting standards for chemical analysis: Chemical Analysis Working Group (CAWG) Metabolomics Standards Initiative (MSI) Sumner, Lloyd W.; Amberg, Alexander; Barrett, Dave Metabolomics, Vol. 3, Issue 3 https://doi.org/10.1007/s11306-007-0082-2	journal	September 2007
Where imaging mass spectrometry stands: here are the numbers Palmer, Andrew; Trede, Dennis; Alexandrov, Theodore Metabolomics, Vol. 12, Issue 6 https://doi.org/10.1007/s11306-016-1047-0	journal	May 2016
Mass spectrometry imaging: Towards mapping the elemental and molecular composition of the rhizosphere Veličković, Dušan; Anderton, Christopher R. Rhizosphere, Vol. 3 https://doi.org/10.1016/j.rhisph.2017.03.003	journal	June 2017
High-resolution AP-SMALDI mass spectrometry imaging of Drosophila melanogaster Khalil, S. M.; Pretzel, J.; Becker, K. International Journal of Mass Spectrometry, Vol. 416 https://doi.org/10.1016/j.ijms.2017.04.001	journal	May 2017
Imaging MS Methodology for More Chemical Information in Less Data Acquisition Time Utilizing a Hybrid Linear Ion Trap−Orbitrap Mass Spectrometer Perdian, D. C.; Lee, Young Jin Analytical Chemistry, Vol. 82, Issue 22 https://doi.org/10.1021/ac102017q	journal	November 2010
Direct Matrix-Assisted Laser Desorption/Ionization Mass Spectrometric Imaging of Cellulose and Hemicellulose in Populus Tissue Lunsford, Kyle Ann; Peter, Gary F.; Yost, Richard A. Analytical Chemistry, Vol. 83, Issue 17 https://doi.org/10.1021/ac2013527	journal	September 2011
Liquid extraction surface analysis mass spectrometry (LESA-MS) as a novel profiling tool for drug distribution and metabolism analysis: the terfenadine example: LESA-MS distribution analysis of terfenadine Eikel, Daniel; Vavrek, Marissa; Smith, Sheri Rapid Communications in Mass Spectrometry, Vol. 25, Issue 23 https://doi.org/10.1002/rcm.5274	journal	November 2011
Development of liquid microjunction extraction strategy for improving protein identification from tissue sections Quanico, Jusal; Franck, Julien; Dauly, Claire Journal of Proteomics, Vol. 79 https://doi.org/10.1016/j.jprot.2012.11.025	journal	February 2013
MALDI Imaging of Liquid Extraction Surface Analysis Sampled Tissue Randall, Elizabeth C.; Race, Alan M.; Cooper, Helen J. Analytical Chemistry, Vol. 88, Issue 17 https://doi.org/10.1021/acs.analchem.5b04281	journal	August 2016
Induction of budding on chloronemata and caulonemata of the moss, Physcomitrella patens, using isopentenyladenine Reski, R.; Abel, W. O. Planta, Vol. 165, Issue 3 https://doi.org/10.1007/BF00392232	journal	January 1985
Homogeneous Matrix Deposition on Dried Agar for MALDI Imaging Mass Spectrometry of Microbial Cultures Hoffmann, Thomas; Dorrestein, Pieter C. Journal of The American Society for Mass Spectrometry, Vol. 26, Issue 11 https://doi.org/10.1007/s13361-015-1241-8	journal	August 2015
Utilizing a Robotic Sprayer for High Lateral and Mass Resolution MALDI FT-ICR MSI of Microbial Cultures Anderton, Christopher R.; Chu, Rosalie K.; Tolić, Nikola Journal of The American Society for Mass Spectrometry, Vol. 27, Issue 3 https://doi.org/10.1007/s13361-015-1324-6	journal	January 2016
Primer on Agar-Based Microbial Imaging Mass Spectrometry Yang, J. Y.; Phelan, V. V.; Simkovsky, R. Journal of Bacteriology, Vol. 194, Issue 22 https://doi.org/10.1128/JB.00823-12	journal	July 2012
Automated Platform for High-Resolution Tissue Imaging Using Nanospray Desorption Electrospray Ionization Mass Spectrometry Lanekoff, Ingela; Heath, Brandi S.; Liyu, Andrey Analytical Chemistry, Vol. 84, Issue 19 https://doi.org/10.1021/ac301909a	journal	September 2012
Adenine nucleotide levels in and nitrogen fixation by the cyanobacterium Anabaena sp. strain 7120 Privalle, L. S.; Burris, R. H. Journal of Bacteriology, Vol. 154, Issue 1 https://doi.org/10.1128/JB.154.1.351-355.1983	journal	April 1983
Combining Metabolomics and Gene Expression Analysis Reveals that Propionyl- and Butyryl-Carnitines Are Involved in Late Stages of Arbuscular Mycorrhizal Symbiosis Laparre, Jérôme; Malbreil, Mathilde; Letisse, Fabien Molecular Plant, Vol. 7, Issue 3 https://doi.org/10.1093/mp/sst136	journal	March 2014
Choline-O-Sulfate Biosynthesis in Plants (Identification and Partial Characterization of a Salinity-Inducible Choline Sulfotransferase from Species of Limonium (Plumbaginaceae) Rivoal, J.; Hanson, A. D. Plant Physiology, Vol. 106, Issue 3 https://doi.org/10.1104/pp.106.3.1187	journal	November 1994
Metabolites of 2,3-diketogulonate delay peroxidase action and induce non-enzymic H 2 O 2 generation: Potential roles in the plant cell wall Kärkönen, Anna; Dewhirst, Rebecca A.; Mackay, C. Logan Archives of Biochemistry and Biophysics, Vol. 620 https://doi.org/10.1016/j.abb.2017.03.006	journal	April 2017
Reconstruction of the carnitine biosynthesis pathway from Neurospora crassa in the yeast Saccharomyces cerevisiae Franken, Jaco; Burger, Anita; Swiegers, Jan H. Applied Microbiology and Biotechnology, Vol. 99, Issue 15 https://doi.org/10.1007/s00253-015-6561-x	journal	April 2015
Using the pimeloyl-CoA synthetase adenylation fold to synthesize fatty acid thioesters Wang, Menglu; Moynié, Lucile; Harrison, Peter J. Nature Chemical Biology, Vol. 13, Issue 6 https://doi.org/10.1038/nchembio.2361	journal	April 2017
Analyzing a mixture of disaccharides by IMS-VUVPD-MS Lee, Sunyoung; Valentine, Stephen J.; Reilly, James P. International Journal of Mass Spectrometry, Vol. 309 https://doi.org/10.1016/j.ijms.2011.09.013	journal	January 2012
Microbial metabolism of mandelate: a microcosm of diversity Fewson, Charles A. FEMS Microbiology Letters, Vol. 54, Issue 2 https://doi.org/10.1111/j.1574-6968.1988.tb02737.x	journal	April 1988

Cited By (4)

Optimization of a minimal sample preparation protocol for imaging mass spectrometry of unsectioned juvenile invertebrates Zink, Katherine E.; Tarnowski, Denise A.; Mandel, Mark J. Journal of Mass Spectrometry, Vol. 55, Issue 4 https://doi.org/10.1002/jms.4458	journal	November 2019
An approach for visualizing the spatial metabolome of an entire plant root system inspired by the Swiss-rolling technique Veličković, Dušan; Chu, Rosalie K.; Myers, Gabriel L. Journal of Mass Spectrometry, Vol. 55, Issue 4 https://doi.org/10.1002/jms.4363	journal	May 2019
Three dimensional secondary ion mass spectrometry imaging (3D-SIMS) of Aedes aegypti ovarian follicles Castellanos, Anthony; Ramirez, Cesar E.; Michalkova, Veronika Journal of Analytical Atomic Spectrometry, Vol. 34, Issue 5 https://doi.org/10.1039/c8ja00425k	journal	January 2019
Imaging mass spectrometry for natural products discovery: a review of ionization methods Spraker, Joseph E.; Luu, Gordon T.; Sanchez, Laura M. Natural Product Reports, Vol. 37, Issue 2 https://doi.org/10.1039/c9np00038k	journal	January 2020

Similar Records

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

Journal Article · Mon Dec 18 00:00:00 EST 2017 · Analytical Chemistry · OSTI ID:1425337

Veličković, Dušan; Chu, Rosalie K.; Carrell, Alyssa A.; +4 more

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

Journal Article · Tue Jan 02 00:00:00 EST 2018 · Analytical Chemistry · OSTI ID:1425337

Velickovic, Dusan; Chu, Rosalie K.; Carrell, Alyssa A.; +4 more

Towards Resolving the Spatial Metabolome with Unambiguous Molecular Annotations in Complex Biological Systems by Coupling Mass Spectrometry Imaging with Structures for Lossless Ion Manipulations

Journal Article · Tue Jan 01 00:00:00 EST 2019 · ChemComm · OSTI ID:1425337

Nagy, Gabe; Veličković, Dusan; Chu, Rosalie K.; +5 more

Related Subjects

59 BASIC BIOLOGICAL SCIENCES

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

Citation Formats

References (26)

Cited By (4)

Similar Records

Related Subjects

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