DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Toward Mass Spectrometry Imaging in the Metabolomics Scale: Increasing Metabolic Coverage Through Multiple On-Tissue Chemical Modifications

Abstract

Exploring the metabolic differences directly on tissues is essential for the comprehensive understanding of how multicellular organisms function. Mass spectrometry imaging (MSI) is an attractive technique toward this goal; however, MSI in metabolomics scale has been hindered by multiple limitations. This is most notable for single cell level high-spatial resolution imaging because of the limited number of molecules in small sampling size and the low ionization yields of many metabolites. Several on-tissue chemical derivatization approaches have been reported to increase MSI signals of targeted compounds, especially in matrix-assisted laser desorption/ionization (MALDI)- MSI. Herein, we adopt a combination of chemical derivatization reactions, to selectively enhance metabolite signals of a specific functional group for each consecutive tissue section. Three well-known on-tissue derivatization methods were used as a proof of concept experiment: coniferyl aldehyde for primary amines, Girard’s reagent T for carbonyl groups, and 2-picolylamine for carboxylic acids. This strategy was applied to the cross-sections of leaves and roots from two different maize genotypes (B73 and Mo17), and enabled the detection of over six hundred new unique metabolite features compared to without modification. Statistical analysis indicated quantitative variation between metabolites in the tissue sections, while MS images revealed differences in localization of thesemore » metabolites. Combined, this untargeted approach facilitated the visualization of various classes of compounds, demonstrating the potential for untargeted MSI in the metabolomics scale.« less

Authors:
; ;
Publication Date:
Research Org.:
Iowa State Univ., Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); American Chemical Society (ACS); Society for Analytical Chemists of Pittsburgh (SACP)
OSTI Identifier:
1542477
Alternate Identifier(s):
OSTI ID: 1903827
Resource Type:
Published Article
Journal Name:
Frontiers in Plant Science
Additional Journal Information:
Journal Name: Frontiers in Plant Science Journal Volume: 10; Journal ID: ISSN 1664-462X
Publisher:
Frontiers Media SA
Country of Publication:
Switzerland
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; mass spectrometry imaging; metabolomics; on-tissue derivatization; high-spatial resolution; maize; single cell

Citation Formats

Dueñas, Maria Emilia, Larson, Evan A., and Lee, Young Jin. Toward Mass Spectrometry Imaging in the Metabolomics Scale: Increasing Metabolic Coverage Through Multiple On-Tissue Chemical Modifications. Switzerland: N. p., 2019. Web. doi:10.3389/fpls.2019.00860.
Dueñas, Maria Emilia, Larson, Evan A., & Lee, Young Jin. Toward Mass Spectrometry Imaging in the Metabolomics Scale: Increasing Metabolic Coverage Through Multiple On-Tissue Chemical Modifications. Switzerland. https://doi.org/10.3389/fpls.2019.00860
Dueñas, Maria Emilia, Larson, Evan A., and Lee, Young Jin. Fri . "Toward Mass Spectrometry Imaging in the Metabolomics Scale: Increasing Metabolic Coverage Through Multiple On-Tissue Chemical Modifications". Switzerland. https://doi.org/10.3389/fpls.2019.00860.
@article{osti_1542477,
title = {Toward Mass Spectrometry Imaging in the Metabolomics Scale: Increasing Metabolic Coverage Through Multiple On-Tissue Chemical Modifications},
author = {Dueñas, Maria Emilia and Larson, Evan A. and Lee, Young Jin},
abstractNote = {Exploring the metabolic differences directly on tissues is essential for the comprehensive understanding of how multicellular organisms function. Mass spectrometry imaging (MSI) is an attractive technique toward this goal; however, MSI in metabolomics scale has been hindered by multiple limitations. This is most notable for single cell level high-spatial resolution imaging because of the limited number of molecules in small sampling size and the low ionization yields of many metabolites. Several on-tissue chemical derivatization approaches have been reported to increase MSI signals of targeted compounds, especially in matrix-assisted laser desorption/ionization (MALDI)- MSI. Herein, we adopt a combination of chemical derivatization reactions, to selectively enhance metabolite signals of a specific functional group for each consecutive tissue section. Three well-known on-tissue derivatization methods were used as a proof of concept experiment: coniferyl aldehyde for primary amines, Girard’s reagent T for carbonyl groups, and 2-picolylamine for carboxylic acids. This strategy was applied to the cross-sections of leaves and roots from two different maize genotypes (B73 and Mo17), and enabled the detection of over six hundred new unique metabolite features compared to without modification. Statistical analysis indicated quantitative variation between metabolites in the tissue sections, while MS images revealed differences in localization of these metabolites. Combined, this untargeted approach facilitated the visualization of various classes of compounds, demonstrating the potential for untargeted MSI in the metabolomics scale.},
doi = {10.3389/fpls.2019.00860},
journal = {Frontiers in Plant Science},
number = ,
volume = 10,
place = {Switzerland},
year = {Fri Jul 12 00:00:00 EDT 2019},
month = {Fri Jul 12 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.3389/fpls.2019.00860

Citation Metrics:
Cited by: 37 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Variations in Anatomy, Associations, and Origins of Kranz Tissue
journal, April 1975


Amino Acid Export in Plants: A Missing Link in Nitrogen Cycling
journal, May 2011

  • Okumoto, Sakiko; Pilot, Guillaume
  • Molecular Plant, Vol. 4, Issue 3
  • DOI: 10.1093/mp/ssr003

Metabolomic Profiling of the Nectars of Aquilegia pubescens and A. Canadensis
journal, May 2015


MetaboAnalyst 4.0: towards more transparent and integrative metabolomics analysis
journal, May 2018

  • Chong, Jasmine; Soufan, Othman; Li, Carin
  • Nucleic Acids Research, Vol. 46, Issue W1
  • DOI: 10.1093/nar/gky310

Genome-wide association study for kernel composition and flour pasting behavior in wholemeal maize flour
journal, April 2019


Implementation of a Gaussian Beam Laser and Aspheric Optics for High Spatial Resolution MALDI Imaging MS
journal, April 2014

  • Zavalin, Andre; Yang, Junhai; Haase, Andreas
  • Journal of The American Society for Mass Spectrometry, Vol. 25, Issue 6
  • DOI: 10.1007/s13361-014-0872-5

Spatial Mapping and Profiling of Metabolite Distributions during Germination
journal, June 2017

  • Feenstra, Adam D.; Alexander, Liza E.; Song, Zhihong
  • Plant Physiology, Vol. 174, Issue 4
  • DOI: 10.1104/pp.17.00652

Microscopic visualization of testosterone in mouse testis by use of imaging mass spectrometry
journal, May 2016

  • Shimma, Shuichi; Kumada, Henri-Obadja; Taniguchi, Hisanori
  • Analytical and Bioanalytical Chemistry, Vol. 408, Issue 27
  • DOI: 10.1007/s00216-016-9594-9

Sputter-Coated Metal Screening for Small Molecule Analysis and High-Spatial Resolution Imaging in Laser Desorption Ionization Mass Spectrometry
journal, October 2018

  • Hansen, Rebecca L.; Dueñas, Maria Emilia; Lee, Young Jin
  • Journal of The American Society for Mass Spectrometry, Vol. 30, Issue 2
  • DOI: 10.1007/s13361-018-2081-0

Targeted Multiplex Imaging Mass Spectrometry in Transmission Geometry for Subcellular Spatial Resolution
journal, February 2013

  • Thiery-Lavenant, Gwendoline; Zavalin, Andre I.; Caprioli, Richard M.
  • Journal of The American Society for Mass Spectrometry, Vol. 24, Issue 4
  • DOI: 10.1007/s13361-012-0563-z

Maize 9-Lipoxygenase ZmLOX3 Controls Development, Root-Specific Expression of Defense Genes, and Resistance to Root-Knot Nematodes
journal, January 2008

  • Gao, Xiquan; Starr, James; Göbel, Cornelia
  • Molecular Plant-Microbe Interactions, Vol. 21, Issue 1
  • DOI: 10.1094/mpmi-21-1-0098

Spatial Localization and Quantitation of Androgens in Mouse Testis by Mass Spectrometry Imaging
journal, October 2016


Optimization and Comparison of Multiple MALDI Matrix Application Methods for Small Molecule Mass Spectrometric Imaging
journal, October 2014

  • Gemperline, Erin; Rawson, Stephanie; Li, Lingjun
  • Analytical Chemistry, Vol. 86, Issue 20
  • DOI: 10.1021/ac5028534

In Situ Analysis of Small Populations of Adherent Mammalian Cells Using Laser Ablation Electrospray Ionization Mass Spectrometry in Transmission Geometry
journal, November 2015


Subcellular-level resolution MALDI-MS imaging of maize leaf metabolites by MALDI-linear ion trap-Orbitrap mass spectrometer
journal, January 2015

  • Korte, Andrew R.; Yandeau-Nelson, Marna D.; Nikolau, Basil J.
  • Analytical and Bioanalytical Chemistry, Vol. 407, Issue 8
  • DOI: 10.1007/s00216-015-8460-5

Efficient Total Synthesis of 12-oxo-PDA and OPC-8:0
journal, October 2003

  • Ainai, Takayuki; Matsuumi, Michitaka; Kobayashi, Yuichi
  • The Journal of Organic Chemistry, Vol. 68, Issue 20
  • DOI: 10.1021/jo0348571

Five Micron High Resolution MALDI Mass Spectrometry Imaging with Simple, Interchangeable, Multi-Resolution Optical System
journal, January 2017

  • Feenstra, Adam D.; Dueñas, Maria Emilia; Lee, Young Jin
  • Journal of The American Society for Mass Spectrometry, Vol. 28, Issue 3
  • DOI: 10.1007/s13361-016-1577-8

High-resolution AP-SMALDI mass spectrometry imaging of Drosophila melanogaster
journal, May 2017


Direct imaging of single cells and tissue at sub-cellular spatial resolution using transmission geometry MALDI MS
journal, November 2012

  • Zavalin, Andre; Todd, Erik M.; Rawhouser, Patrick D.
  • Journal of Mass Spectrometry, Vol. 47, Issue 11
  • DOI: 10.1002/jms.3132

Matrix Recrystallization for MALDI-MS Imaging of Maize Lipids at High-Spatial Resolution
journal, June 2016

  • Dueñas, Maria Emilia; Carlucci, Laura; Lee, Young Jin
  • Journal of The American Society for Mass Spectrometry, Vol. 27, Issue 9
  • DOI: 10.1007/s13361-016-1422-0

Pyrylium Salts as Reactive Matrices for MALDI-MS Imaging of Biologically Active Primary Amines
journal, March 2015

  • Shariatgorji, Mohammadreza; Nilsson, Anna; Källback, Patrik
  • Journal of The American Society for Mass Spectrometry, Vol. 26, Issue 6
  • DOI: 10.1007/s13361-015-1119-9

High Spatial Resolution Imaging of Mouse Pancreatic Islets Using Nanospray Desorption Electrospray Ionization Mass Spectrometry
journal, April 2018


Modern analytical techniques in metabolomics analysis
journal, January 2012

  • Zhang, Aihua; Sun, Hui; Wang, Ping
  • The Analyst, Vol. 137, Issue 2
  • DOI: 10.1039/c1an15605e

Heterotic patterns of sugar and amino acid components in developing maize kernels
journal, November 2009

  • Römisch-Margl, Lilla; Spielbauer, Gertraud; Schützenmeister, Andre
  • Theoretical and Applied Genetics, Vol. 120, Issue 2
  • DOI: 10.1007/s00122-009-1190-3

Atmospheric pressure MALDI mass spectrometry imaging of tissues and cells at 1.4-μm lateral resolution
journal, November 2016

  • Kompauer, Mario; Heiles, Sven; Spengler, Bernhard
  • Nature Methods, Vol. 14, Issue 1
  • DOI: 10.1038/nmeth.4071

Laser Beam Filtration for High Spatial Resolution MALDI Imaging Mass Spectrometry
journal, May 2013

  • Zavalin, Andre; Yang, Junhai; Caprioli, Richard
  • Journal of The American Society for Mass Spectrometry, Vol. 24, Issue 7
  • DOI: 10.1007/s13361-013-0638-5

The Metabolism of Acetaldehyde by Plant Tissues
journal, January 1968


Sodium-Doped Gold-Assisted Laser Desorption Ionization for Enhanced Imaging Mass Spectrometry of Triacylglycerols from Thin Tissue Sections
journal, May 2016


FERONIA mutation induces high levels of chloroplast-localized Arabidopsides which are involved in root growth
journal, November 2018

  • Hansen, Rebecca L.; Guo, Hongqing; Yin, Yanhai
  • The Plant Journal, Vol. 97, Issue 2
  • DOI: 10.1111/tpj.14123

Changes in Polar Lipid Composition in Maize Seedlings Induced by Cadmium Stress
journal, February 2007

  • ., Radhouane Chaffai; ., Mohamed Anis Elhammadi; ., Tini Nouhou Seybou
  • International Journal of Agricultural Research, Vol. 2, Issue 2
  • DOI: 10.3923/ijar.2007.126.135

MSiReader: An Open-Source Interface to View and Analyze High Resolving Power MS Imaging Files on Matlab Platform
journal, March 2013

  • Robichaud, Guillaume; Garrard, Kenneth P.; Barry, Jeremy A.
  • Journal of The American Society for Mass Spectrometry, Vol. 24, Issue 5
  • DOI: 10.1007/s13361-013-0607-z

Derivatization Strategies for the Detection of Triamcinolone Acetonide in Cartilage by Using Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry Imaging
journal, December 2016


Synthesis and Functions of Jasmonates in Maize
journal, November 2016


Reactions of Microsolvated Organic Compounds at Ambient Surfaces: Droplet Velocity, Charge State, and Solvent Effects
journal, March 2012

  • Badu-Tawiah, Abraham K.; Campbell, Dahlia I.; Cooks, R. Graham
  • Journal of The American Society for Mass Spectrometry, Vol. 23, Issue 6, p. 1077-1084
  • DOI: 10.1007/s13361-012-0365-3