Untargeted Molecular Discovery in Primary Metabolism: Collision Cross Section as a Molecular Descriptor in Ion Mobility-Mass Spectrometry
In this work, we established a collision cross section (CCS) library of primary metabolites based on analytical standards in the Mass Spectrometry Metabolite Library of Standards (MSMLS) using a commercially available ion mobility-mass spectrometer (IM-MS). From the 554 unique compounds in the MSMLS...
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| Veröffentlicht in: | Analytical chemistry (Washington) 2018-12, Vol.90 (24), p.14484-14492 |
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| creator | Nichols, Charles M Dodds, James N Rose, Bailey S Picache, Jaqueline A Morris, Caleb B Codreanu, Simona G May, Jody C Sherrod, Stacy D McLean, John A |
| description | In this work, we established a collision cross section (CCS) library of primary metabolites based on analytical standards in the Mass Spectrometry Metabolite Library of Standards (MSMLS) using a commercially available ion mobility-mass spectrometer (IM-MS). From the 554 unique compounds in the MSMLS plate library, we obtained a total of 1246 CCS measurements over a wide range of biochemical classes and adduct types. Resulting data analysis demonstrated that the curated CCS library provides broad molecular coverage of metabolic pathways and highlights intrinsic mass–mobility relationships for specific metabolite superclasses. The separation and characterization of isomeric metabolites were assessed, and all molecular species contained within the plate library, including isomers, were critically evaluated to determine the analytical separation efficiency in both the mass (m/z) and mobility (CCS/ΔCCS) dimension required for untargeted metabolomic analyses. To further demonstrate the analytical utility of CCS as an additional molecular descriptor, a well-characterized biological sample of human plasma serum (NIST SRM 1950) was examined by LC-IM-MS and used to provide a detailed isomeric analysis of carbohydrate constituents by ion mobility. |
| doi_str_mv | 10.1021/acs.analchem.8b04322 |
| format | Article |
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From the 554 unique compounds in the MSMLS plate library, we obtained a total of 1246 CCS measurements over a wide range of biochemical classes and adduct types. Resulting data analysis demonstrated that the curated CCS library provides broad molecular coverage of metabolic pathways and highlights intrinsic mass–mobility relationships for specific metabolite superclasses. The separation and characterization of isomeric metabolites were assessed, and all molecular species contained within the plate library, including isomers, were critically evaluated to determine the analytical separation efficiency in both the mass (m/z) and mobility (CCS/ΔCCS) dimension required for untargeted metabolomic analyses. To further demonstrate the analytical utility of CCS as an additional molecular descriptor, a well-characterized biological sample of human plasma serum (NIST SRM 1950) was examined by LC-IM-MS and used to provide a detailed isomeric analysis of carbohydrate constituents by ion mobility.</description><identifier>ISSN: 0003-2700</identifier><identifier>ISSN: 1520-6882</identifier><identifier>EISSN: 1520-6882</identifier><identifier>DOI: 10.1021/acs.analchem.8b04322</identifier><identifier>PMID: 30449086</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Analytical chemistry ; biochemical pathways ; Blood plasma ; blood serum ; Carbohydrates ; Carbohydrates - analysis ; Carbohydrates - blood ; Chemistry ; Chromatography, High Pressure Liquid ; Cross-sections ; Data analysis ; Data processing ; Humans ; Ion Mobility Spectrometry ; Ionic mobility ; Isomerism ; Isomers ; Libraries ; Mass Spectrometry ; Mass spectroscopy ; Mathematical analysis ; Metabolic pathways ; Metabolism ; Metabolites ; Metabolomics ; Metabolomics - methods ; Mobility ; Plasma ; Separation ; spectrometers ; Spectroscopy</subject><ispartof>Analytical chemistry (Washington), 2018-12, Vol.90 (24), p.14484-14492</ispartof><rights>Copyright American Chemical Society Dec 18, 2018</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a510t-eadf83ba75da73c4b8edad62b5e75dc7058930d4750e3443204b3cb879d8c47a3</citedby><cites>FETCH-LOGICAL-a510t-eadf83ba75da73c4b8edad62b5e75dc7058930d4750e3443204b3cb879d8c47a3</cites><orcidid>0000-0003-4871-5024 ; 0000-0001-8918-6419 ; 0000-0002-5900-7288</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.analchem.8b04322$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.analchem.8b04322$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/30449086$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Nichols, Charles M</creatorcontrib><creatorcontrib>Dodds, James N</creatorcontrib><creatorcontrib>Rose, Bailey S</creatorcontrib><creatorcontrib>Picache, Jaqueline A</creatorcontrib><creatorcontrib>Morris, Caleb B</creatorcontrib><creatorcontrib>Codreanu, Simona G</creatorcontrib><creatorcontrib>May, Jody C</creatorcontrib><creatorcontrib>Sherrod, Stacy D</creatorcontrib><creatorcontrib>McLean, John A</creatorcontrib><title>Untargeted Molecular Discovery in Primary Metabolism: Collision Cross Section as a Molecular Descriptor in Ion Mobility-Mass Spectrometry</title><title>Analytical chemistry (Washington)</title><addtitle>Anal. Chem</addtitle><description>In this work, we established a collision cross section (CCS) library of primary metabolites based on analytical standards in the Mass Spectrometry Metabolite Library of Standards (MSMLS) using a commercially available ion mobility-mass spectrometer (IM-MS). From the 554 unique compounds in the MSMLS plate library, we obtained a total of 1246 CCS measurements over a wide range of biochemical classes and adduct types. Resulting data analysis demonstrated that the curated CCS library provides broad molecular coverage of metabolic pathways and highlights intrinsic mass–mobility relationships for specific metabolite superclasses. The separation and characterization of isomeric metabolites were assessed, and all molecular species contained within the plate library, including isomers, were critically evaluated to determine the analytical separation efficiency in both the mass (m/z) and mobility (CCS/ΔCCS) dimension required for untargeted metabolomic analyses. 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Chem</addtitle><date>2018-12-18</date><risdate>2018</risdate><volume>90</volume><issue>24</issue><spage>14484</spage><epage>14492</epage><pages>14484-14492</pages><issn>0003-2700</issn><issn>1520-6882</issn><eissn>1520-6882</eissn><abstract>In this work, we established a collision cross section (CCS) library of primary metabolites based on analytical standards in the Mass Spectrometry Metabolite Library of Standards (MSMLS) using a commercially available ion mobility-mass spectrometer (IM-MS). From the 554 unique compounds in the MSMLS plate library, we obtained a total of 1246 CCS measurements over a wide range of biochemical classes and adduct types. Resulting data analysis demonstrated that the curated CCS library provides broad molecular coverage of metabolic pathways and highlights intrinsic mass–mobility relationships for specific metabolite superclasses. The separation and characterization of isomeric metabolites were assessed, and all molecular species contained within the plate library, including isomers, were critically evaluated to determine the analytical separation efficiency in both the mass (m/z) and mobility (CCS/ΔCCS) dimension required for untargeted metabolomic analyses. To further demonstrate the analytical utility of CCS as an additional molecular descriptor, a well-characterized biological sample of human plasma serum (NIST SRM 1950) was examined by LC-IM-MS and used to provide a detailed isomeric analysis of carbohydrate constituents by ion mobility.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>30449086</pmid><doi>10.1021/acs.analchem.8b04322</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0003-4871-5024</orcidid><orcidid>https://orcid.org/0000-0001-8918-6419</orcidid><orcidid>https://orcid.org/0000-0002-5900-7288</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | Analytical chemistry biochemical pathways Blood plasma blood serum Carbohydrates Carbohydrates - analysis Carbohydrates - blood Chemistry Chromatography, High Pressure Liquid Cross-sections Data analysis Data processing Humans Ion Mobility Spectrometry Ionic mobility Isomerism Isomers Libraries Mass Spectrometry Mass spectroscopy Mathematical analysis Metabolic pathways Metabolism Metabolites Metabolomics Metabolomics - methods Mobility Plasma Separation spectrometers Spectroscopy |
| title | Untargeted Molecular Discovery in Primary Metabolism: Collision Cross Section as a Molecular Descriptor in Ion Mobility-Mass Spectrometry |
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