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

Nagy, Gabe; Veličković, Dusan; Chu, Rosalie K.; Carrell, Alyssa A.; Weston, David J.; Ibrahim, Yehia M.; Anderton, Christopher R.; Smith, Richard D.

doi:10.1039/C8CC07482H

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 · Mon Dec 31 23:00:00 EST 2018 · ChemComm

DOI:https://doi.org/10.1039/C8CC07482H· OSTI ID:1496826

Nagy, Gabe ^[1]; Veličković, Dusan ^[1]; Chu, Rosalie K. ^[2]; Carrell, Alyssa A. ^[3]; Weston, David J. ^[3]; ^[1]; ^[2]; ^[1]

Biological Sciences Division, Pacific Northwest National Laboratory; Richland; USA
Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory; Richland; USA
Biosciences Division; Oak Ridge National Laboratory; Oak Ridge; USA

We demonstrate the coupling of liquid extraction surface analysis (LESA) to structures for lossless ion manipulations in conjunction with serpentine ultralong path with extending routing (SLIM SUPER) ion mobility-mass spectrometry (IM-MS) for the unambiguous annotation of important isomeric glycoforms in carbon-fixing communities. A major bottleneck of current mass spectrometry imaging (MSI) methods is their inability to accurately and confidently delineate amongst isomers within a single probing area. Our methodology provides gains in both sensitivity and IM resolution, while simultaneously gaining insight on the spatial distribution of these biological isomers in a mixed organism composed of moss, cyanobacteria and fungus. We envision this methodology will be broadly applicable to other mass spectrometry imaging modalities and invaluable in multiplexed, untargeted, analyses of a single probing location.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1496826

Report Number(s):: PNNL-SA-138045

Journal Information:: ChemComm, Journal Name: ChemComm Journal Issue: 3 Vol. 55; ISSN CHCOFS; ISSN 1359-7345

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

References (40)

Ion Mobility Separations of Isomers based upon Long Path Length Structures for Lossless Ion Manipulations Combined with Mass Spectrometry Deng, Liulin; Ibrahim, Yehia M.; Baker, Erin S. ChemistrySelect, Vol. 1, Issue 10 https://doi.org/10.1002/slct.201600460	journal	July 2016
Separation of sodiated isobaric disaccharides and trisaccharides using electrospray ionization-atmospheric pressure ion mobility-time of flight mass spectrometry Clowers, Brian H.; Dwivedi, Prabha; Steiner, Wes E. Journal of the American Society for Mass Spectrometry, Vol. 16, Issue 5 https://doi.org/10.1016/j.jasms.2005.01.010	journal	May 2005
Compression Ratio Ion Mobility Programming (CRIMP) Accumulation and Compression of Billions of Ions for Ion Mobility-Mass Spectrometry Using Traveling Waves in Structures for Lossless Ion Manipulations (SLIM) Deng, Liulin; Garimella, Sandilya V. B.; Hamid, Ahmed M. Analytical Chemistry, Vol. 89, Issue 12 https://doi.org/10.1021/acs.analchem.7b00189	journal	May 2017
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
Laser-ablation electrospray ionization mass spectrometry with ion mobility separation reveals metabolites in the symbiotic interactions of soybean roots and rhizobia Stopka, Sylwia A.; Agtuca, Beverly J.; Koppenaal, David W. The Plant Journal, Vol. 91, Issue 2 https://doi.org/10.1111/tpj.13569	journal	May 2017
Rapid resolution of carbohydrate isomers by electrospray ionization ambient pressure ion mobility spectrometry-time-of-flight mass spectrometry (ESI-APIMS-TOFMS) Dwivedi, Prabha; Bendiak, Brad; Clowers, Brian H. Journal of the American Society for Mass Spectrometry, Vol. 18, Issue 7 https://doi.org/10.1016/j.jasms.2007.04.007	journal	July 2007
New insights on trehalose: a multifunctional molecule Elbein, A. D. Glycobiology, Vol. 13, Issue 4 https://doi.org/10.1093/glycob/cwg047	journal	January 2003
Automated, parallel mass spectrometry imaging and structural identification of lipids Ellis, Shane R.; Paine, Martin R. L.; Eijkel, Gert B. Nature Methods, Vol. 15, Issue 7 https://doi.org/10.1038/s41592-018-0010-6	journal	May 2018
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
Serpentine Ultralong Path with Extended Routing (SUPER) High Resolution Traveling Wave Ion Mobility-MS using Structures for Lossless Ion Manipulations Deng, Liulin; Webb, Ian K.; Garimella, Sandilya V. B. Analytical Chemistry, Vol. 89, Issue 8 https://doi.org/10.1021/acs.analchem.7b00185	journal	April 2017
Naturally Occurring Structural Isomers in Serum IgA1 O -Glycosylation Takahashi, Kazuo; Smith, Archer D.; Poulsen, Knud Journal of Proteome Research, Vol. 11, Issue 2 https://doi.org/10.1021/pr200608q	journal	December 2011
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
Profiling and imaging of tissues by imaging ion mobility-mass spectrometry McLean, John A.; Ridenour, Whitney B.; Caprioli, Richard M. Journal of Mass Spectrometry, Vol. 42, Issue 8 https://doi.org/10.1002/jms.1254	journal	January 2007
Separation of isomeric disaccharides by traveling wave ion mobility mass spectrometry using CO ₂ as drift gas : Increasing ion mobility Synapt resolution with CO2 Fasciotti, Maíra; Sanvido, Gustavo B.; Santos, Vanessa G. Journal of Mass Spectrometry, Vol. 47, Issue 12 https://doi.org/10.1002/jms.3089	journal	December 2012
Observed metabolic asymmetry within soybean root nodules reflects unexpected complexity in rhizobacteria-legume metabolite exchange Veličković, Dušan; Agtuca, Beverly J.; Stopka, Sylwia A. The ISME Journal, Vol. 12, Issue 9 https://doi.org/10.1038/s41396-018-0188-8	journal	June 2018
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
Differentiating N-linked glycan structural isomers in metastatic and nonmetastatic tumor cells using sequential mass spectrometry Prien, J. M.; Huysentruyt, L. C.; Ashline, D. J. Glycobiology, Vol. 18, Issue 5 https://doi.org/10.1093/glycob/cwn010	journal	February 2008
Multimodal MSI in Conjunction with Broad Coverage Spatially Resolved MS ² Increases Confidence in Both Molecular Identification and Localization Veličković, Dušan; Chu, Rosalie K.; Carrell, Alyssa A. Analytical Chemistry, Vol. 90, Issue 1 https://doi.org/10.1021/acs.analchem.7b04319	journal	December 2017
Glycan analysis by ion mobility-mass spectrometry and gas-phase spectroscopy Manz, Christian; Pagel, Kevin Current Opinion in Chemical Biology, Vol. 42 https://doi.org/10.1016/j.cbpa.2017.10.021	journal	February 2018
Rapid and sensitive differentiation of anomers, linkage, and position isomers of disaccharides using High-Field Asymmetric Waveform Ion Mobility Spectrometry (FAIMS) Gabryelski, Wojciech; Froese, Kenneth L. Journal of the American Society for Mass Spectrometry, Vol. 14, Issue 3 https://doi.org/10.1016/S1044-0305(03)00002-3	journal	March 2003
Recombinant " IMS TAG" proteins - A new method for validating bottom-up matrix-assisted laser desorption/ionisation ion mobility separation mass spectrometry imaging: Recombinant " IMS TAG" proteins Cole, Laura M.; Mahmoud, Khaled; Haywood-Small, Sarah Rapid Communications in Mass Spectrometry, Vol. 27, Issue 21 https://doi.org/10.1002/rcm.6693	journal	October 2013
Ion mobility mass spectrometry analysis of isomeric disaccharide precursor, product and cluster ions: Analysis of isomeric disaccharide precursor, product and cluster ions Li, Hongli; Bendiak, Brad; Siems, William F. Rapid Communications in Mass Spectrometry, Vol. 27, Issue 23 https://doi.org/10.1002/rcm.6720	journal	October 2013
Glycan Analysis by Ion Mobility-Mass Spectrometry Hofmann, Johanna; Pagel, Kevin Angewandte Chemie International Edition, Vol. 56, Issue 29 https://doi.org/10.1002/anie.201701309	journal	June 2017
Improved Sensitivity and Separations for Phosphopeptides using Online Liquid Chromotography Coupled with Structures for Lossless Ion Manipulations Ion Mobility–Mass Spectrometry Chouinard, Christopher D.; Nagy, Gabe; Webb, Ian K. Analytical Chemistry, Vol. 90, Issue 18 https://doi.org/10.1021/acs.analchem.8b02397	journal	August 2018
Ion Mobility Studies of Carbohydrates as Group I Adducts: Isomer Specific Collisional Cross Section Dependence on Metal Ion Radius Huang, Yuting; Dodds, Eric D. Analytical Chemistry, Vol. 85, Issue 20 https://doi.org/10.1021/ac402133f	journal	September 2013
MALDI Mass Spectrometry Imaging: A Novel Tool for the Identification and Classification of Amyloidosis Winter, Martin; Tholey, Andreas; Kristen, Arnt PROTEOMICS, Vol. 17, Issue 22 https://doi.org/10.1002/pmic.201700236	journal	November 2017
Advances in mass spectrometry imaging coupled to ion mobility spectrometry for enhanced imaging of biological tissues Sans, Marta; Feider, Clara L.; Eberlin, Livia S. Current Opinion in Chemical Biology, Vol. 42 https://doi.org/10.1016/j.cbpa.2017.12.005	journal	February 2018
Ambient Ionization and FAIMS Mass Spectrometry for Enhanced Imaging of Multiply Charged Molecular Ions in Biological Tissues Feider, Clara L.; Elizondo, Natalia; Eberlin, Livia S. Analytical Chemistry, Vol. 88, Issue 23 https://doi.org/10.1021/acs.analchem.6b02798	journal	November 2016
Identification of carbohydrate anomers using ion mobility–mass spectrometry Hofmann, J.; Hahm, H. S.; Seeberger, P. H. Nature, Vol. 526, Issue 7572 https://doi.org/10.1038/nature15388	journal	September 2015
Enhancing glycan isomer separations with metal ions and positive and negative polarity ion mobility spectrometry-mass spectrometry analyses Zheng, Xueyun; Zhang, Xing; Schocker, Nathaniel S. Analytical and Bioanalytical Chemistry, Vol. 409, Issue 2 https://doi.org/10.1007/s00216-016-9866-4	journal	September 2016
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
The specificity of α-glucosidase from Saccharomyces cerevisiae differs depending on the type of reaction: hydrolysis versus transglucosylation Dušan, Veličković; Nenad, Milosavić; Dejan, Bezbradica Applied Microbiology and Biotechnology, Vol. 98, Issue 14 https://doi.org/10.1007/s00253-014-5587-9	journal	February 2014
Purification and Properties of Glycogen Isolated from a Blue-Green Alga, Nostoc muscorum Chao, Lee; Bowen, C. C. Journal of Bacteriology, Vol. 105, Issue 1 https://doi.org/10.1128/JB.105.1.331-338.1971	journal	January 1971
Conjugated linoleic acid isomers: Differences in metabolism and biological effects Churruca, Itziar; Fernández-Quintela, Alfredo; Portillo, Maria Puy BioFactors, Vol. 35, Issue 1 https://doi.org/10.1002/biof.13	journal	January 2009
Imaging mass spectrometry: Molecular microscopy for the new age of biology and medicine Caprioli, Richard M. PROTEOMICS, Vol. 16, Issue 11-12 https://doi.org/10.1002/pmic.201600133	journal	May 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
Squeezing of Ion Populations and Peaks in Traveling Wave Ion Mobility Separations and Structures for Lossless Ion Manipulations Using Compression Ratio Ion Mobility Programming Garimella, Sandilya V. B.; Hamid, Ahmed M.; Deng, Liulin Analytical Chemistry, Vol. 88, Issue 23 https://doi.org/10.1021/acs.analchem.6b03660	journal	November 2016
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
LESA FAIMS Mass Spectrometry for the Spatial Profiling of Proteins from Tissue Griffiths, Rian L.; Creese, Andrew J.; Race, Alan M. Analytical Chemistry, Vol. 88, Issue 13 https://doi.org/10.1021/acs.analchem.6b01060	journal	June 2016
Ultra-High Resolution Ion Mobility Separations Utilizing Traveling Waves in a 13 m Serpentine Path Length Structures for Lossless Ion Manipulations Module Deng, Liulin; Ibrahim, Yehia M.; Hamid, Ahmed M. Analytical Chemistry, Vol. 88, Issue 18 https://doi.org/10.1021/acs.analchem.6b01915	journal	August 2016

Cited By (1)

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

Similar Records

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 · Thu Dec 06 23:00:00 EST 2018 · ChemComm · OSTI ID:1560416

Implementation of Ion Mobility Spectrometry-Based Separations in Structures for Lossless Ion Manipulations (SLIM)

Book · Fri Dec 31 23:00:00 EST 2021 · OSTI ID:1855404

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

Citation Formats

References (40)

Cited By (1)

Similar Records

Related Subjects