Enhanced Speciation of Pyrogenic Organic Matter from Wildfires Enabled by 21 T FT-ICR Mass Spectrometry
Wildfires affect soils through the formation of pyrogenic organic matter (pyOM) (e.g., char and soot). While many studies examine the connection between pyOM persistence and carbon (C) composition, nitrogen (N) transformation in wildfire-impacted systems remains poorly understood. Thermal reactions...
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| Veröffentlicht in: | Analytical chemistry (Washington) 2022-02, Vol.94 (6), p.2973-2980 |
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| creator | Roth, Holly K Borch, Thomas Young, Robert B Bahureksa, William Blakney, Greg T Nelson, Amelia R Wilkins, Michael J McKenna, Amy M |
| description | Wildfires affect soils through the formation of pyrogenic organic matter (pyOM) (e.g., char and soot). While many studies examine the connection between pyOM persistence and carbon (C) composition, nitrogen (N) transformation in wildfire-impacted systems remains poorly understood. Thermal reactions in wildfires transform biomass into a highly complex, polyfunctional, and polydisperse organic mixture that challenges most mass analyzers. High-field Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) is the only mass analyzer that achieves resolving powers sufficient to separate species that differ in mass by the mass of an electron across a wide molecular weight range (m/z 150–1500). We report enhanced speciation of organic N by positive-ion electrospray ionization (ESI) that leverages ultrahigh resolving power (m/Δm 50% = 1 800 000 at m/z 400) and mass accuracy ( |
| doi_str_mv | 10.1021/acs.analchem.1c05018 |
| format | Article |
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While many studies examine the connection between pyOM persistence and carbon (C) composition, nitrogen (N) transformation in wildfire-impacted systems remains poorly understood. Thermal reactions in wildfires transform biomass into a highly complex, polyfunctional, and polydisperse organic mixture that challenges most mass analyzers. High-field Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) is the only mass analyzer that achieves resolving powers sufficient to separate species that differ in mass by the mass of an electron across a wide molecular weight range (m/z 150–1500). We report enhanced speciation of organic N by positive-ion electrospray ionization (ESI) that leverages ultrahigh resolving power (m/Δm 50% = 1 800 000 at m/z 400) and mass accuracy (<10–100 ppb) achieved by FT-ICR MS at 21 T. Isobaric overlaps, roughly the mass of an electron (M e– = 548 μDa), are resolved across a wide molecular weight range and are more prevalent in positive ESI than negative ESI. The custom-built 21 T FT-ICR MS instrument identifies previously unresolved mass differences in C c H h N n O o S s formulas and assigns more than 30 000 peaks in a pyOM sample. This is the first molecular catalogue of pyOM by positive-ion ESI 21 T FT-ICR MS and presents a method to provide new insight into terrestrial cycling of organic carbon and nitrogen in wildfire impacted ecosystems.</description><identifier>ISSN: 0003-2700</identifier><identifier>EISSN: 1520-6882</identifier><identifier>DOI: 10.1021/acs.analchem.1c05018</identifier><identifier>PMID: 35107981</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Analytical chemistry ; Analyzers ; Carbon ; Carbon cycle ; Chemistry ; Cyclotron resonance ; Ecosystem ; Fourier transforms ; Ionization ; Ions ; Mass Spectrometry ; Mass spectroscopy ; Molecular weight ; Nitrogen ; Organic carbon ; Organic matter ; Resolution ; Scientific imaging ; Soot ; Speciation ; Spectroscopy ; Terrestrial environments ; Wildfires</subject><ispartof>Analytical chemistry (Washington), 2022-02, Vol.94 (6), p.2973-2980</ispartof><rights>2022 American Chemical Society</rights><rights>Copyright American Chemical Society Feb 15, 2022</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a376t-3b9faa704e0ac1f0cee097c104f9a24f55f9c21f8453209c4d7e6940127a62293</citedby><cites>FETCH-LOGICAL-a376t-3b9faa704e0ac1f0cee097c104f9a24f55f9c21f8453209c4d7e6940127a62293</cites><orcidid>0000-0003-2733-517X ; 0000-0002-4251-1613 ; 0000-0002-4205-9866 ; 0000-0001-7213-521X ; 0000-0001-7485-0604</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.1c05018$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.analchem.1c05018$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,2765,27076,27924,27925,56738,56788</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/35107981$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Roth, Holly K</creatorcontrib><creatorcontrib>Borch, Thomas</creatorcontrib><creatorcontrib>Young, Robert B</creatorcontrib><creatorcontrib>Bahureksa, William</creatorcontrib><creatorcontrib>Blakney, Greg T</creatorcontrib><creatorcontrib>Nelson, Amelia R</creatorcontrib><creatorcontrib>Wilkins, Michael J</creatorcontrib><creatorcontrib>McKenna, Amy M</creatorcontrib><title>Enhanced Speciation of Pyrogenic Organic Matter from Wildfires Enabled by 21 T FT-ICR Mass Spectrometry</title><title>Analytical chemistry (Washington)</title><addtitle>Anal. Chem</addtitle><description>Wildfires affect soils through the formation of pyrogenic organic matter (pyOM) (e.g., char and soot). While many studies examine the connection between pyOM persistence and carbon (C) composition, nitrogen (N) transformation in wildfire-impacted systems remains poorly understood. Thermal reactions in wildfires transform biomass into a highly complex, polyfunctional, and polydisperse organic mixture that challenges most mass analyzers. High-field Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) is the only mass analyzer that achieves resolving powers sufficient to separate species that differ in mass by the mass of an electron across a wide molecular weight range (m/z 150–1500). We report enhanced speciation of organic N by positive-ion electrospray ionization (ESI) that leverages ultrahigh resolving power (m/Δm 50% = 1 800 000 at m/z 400) and mass accuracy (<10–100 ppb) achieved by FT-ICR MS at 21 T. Isobaric overlaps, roughly the mass of an electron (M e– = 548 μDa), are resolved across a wide molecular weight range and are more prevalent in positive ESI than negative ESI. The custom-built 21 T FT-ICR MS instrument identifies previously unresolved mass differences in C c H h N n O o S s formulas and assigns more than 30 000 peaks in a pyOM sample. This is the first molecular catalogue of pyOM by positive-ion ESI 21 T FT-ICR MS and presents a method to provide new insight into terrestrial cycling of organic carbon and nitrogen in wildfire impacted ecosystems.</description><subject>Analytical chemistry</subject><subject>Analyzers</subject><subject>Carbon</subject><subject>Carbon cycle</subject><subject>Chemistry</subject><subject>Cyclotron resonance</subject><subject>Ecosystem</subject><subject>Fourier transforms</subject><subject>Ionization</subject><subject>Ions</subject><subject>Mass Spectrometry</subject><subject>Mass spectroscopy</subject><subject>Molecular weight</subject><subject>Nitrogen</subject><subject>Organic carbon</subject><subject>Organic matter</subject><subject>Resolution</subject><subject>Scientific imaging</subject><subject>Soot</subject><subject>Speciation</subject><subject>Spectroscopy</subject><subject>Terrestrial environments</subject><subject>Wildfires</subject><issn>0003-2700</issn><issn>1520-6882</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNp9kU1PGzEQhq2qqATaf1AhS730smHGu16vjygKLRKIqk3V42rijMOi_Qj25pB_j9MEDhw4zeV5n5HeV4ivCFMEhZfk4pR6at0Dd1N0oAGrD2KCWkFWVpX6KCYAkGfKAJyKsxgfARABy0_iNNcIxlY4Eet5_0C945X8s2HX0NgMvRy8_LULw5r7xsn7sKb9vaNx5CB9GDr5r2lXvgkc5bynZZvSy51UKBfyepHdzH4nOMb_xjHhPIbdZ3HiqY385XjPxd_r-WL2M7u9_3Ezu7rNKDflmOVL64kMFAzk0INjBmscQuEtqcJr7a1T6KtC5wqsK1aGS1sAKkOlUjY_F98P3k0YnrYcx7prouO2pZ6HbaxVqbQqdWorod_eoI_DNqRG91Re6MoaaxJVHCgXhhgD-3oTmo7Crkao90PUaYj6ZYj6OESKXRzl22XHq9fQS_MJgAOwj78-ftf5DBzulWo</recordid><startdate>20220215</startdate><enddate>20220215</enddate><creator>Roth, Holly K</creator><creator>Borch, Thomas</creator><creator>Young, Robert B</creator><creator>Bahureksa, William</creator><creator>Blakney, Greg T</creator><creator>Nelson, Amelia R</creator><creator>Wilkins, Michael J</creator><creator>McKenna, Amy M</creator><general>American Chemical Society</general><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QF</scope><scope>7QO</scope><scope>7QQ</scope><scope>7SC</scope><scope>7SE</scope><scope>7SP</scope><scope>7SR</scope><scope>7TA</scope><scope>7TB</scope><scope>7TM</scope><scope>7U5</scope><scope>7U7</scope><scope>7U9</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>H8G</scope><scope>H94</scope><scope>JG9</scope><scope>JQ2</scope><scope>KR7</scope><scope>L7M</scope><scope>L~C</scope><scope>L~D</scope><scope>P64</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0003-2733-517X</orcidid><orcidid>https://orcid.org/0000-0002-4251-1613</orcidid><orcidid>https://orcid.org/0000-0002-4205-9866</orcidid><orcidid>https://orcid.org/0000-0001-7213-521X</orcidid><orcidid>https://orcid.org/0000-0001-7485-0604</orcidid></search><sort><creationdate>20220215</creationdate><title>Enhanced Speciation of Pyrogenic Organic Matter from Wildfires Enabled by 21 T FT-ICR Mass Spectrometry</title><author>Roth, Holly K ; 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Chem</addtitle><date>2022-02-15</date><risdate>2022</risdate><volume>94</volume><issue>6</issue><spage>2973</spage><epage>2980</epage><pages>2973-2980</pages><issn>0003-2700</issn><eissn>1520-6882</eissn><abstract>Wildfires affect soils through the formation of pyrogenic organic matter (pyOM) (e.g., char and soot). While many studies examine the connection between pyOM persistence and carbon (C) composition, nitrogen (N) transformation in wildfire-impacted systems remains poorly understood. Thermal reactions in wildfires transform biomass into a highly complex, polyfunctional, and polydisperse organic mixture that challenges most mass analyzers. High-field Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) is the only mass analyzer that achieves resolving powers sufficient to separate species that differ in mass by the mass of an electron across a wide molecular weight range (m/z 150–1500). We report enhanced speciation of organic N by positive-ion electrospray ionization (ESI) that leverages ultrahigh resolving power (m/Δm 50% = 1 800 000 at m/z 400) and mass accuracy (<10–100 ppb) achieved by FT-ICR MS at 21 T. Isobaric overlaps, roughly the mass of an electron (M e– = 548 μDa), are resolved across a wide molecular weight range and are more prevalent in positive ESI than negative ESI. The custom-built 21 T FT-ICR MS instrument identifies previously unresolved mass differences in C c H h N n O o S s formulas and assigns more than 30 000 peaks in a pyOM sample. This is the first molecular catalogue of pyOM by positive-ion ESI 21 T FT-ICR MS and presents a method to provide new insight into terrestrial cycling of organic carbon and nitrogen in wildfire impacted ecosystems.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>35107981</pmid><doi>10.1021/acs.analchem.1c05018</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0003-2733-517X</orcidid><orcidid>https://orcid.org/0000-0002-4251-1613</orcidid><orcidid>https://orcid.org/0000-0002-4205-9866</orcidid><orcidid>https://orcid.org/0000-0001-7213-521X</orcidid><orcidid>https://orcid.org/0000-0001-7485-0604</orcidid></addata></record> |
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| subjects | Analytical chemistry Analyzers Carbon Carbon cycle Chemistry Cyclotron resonance Ecosystem Fourier transforms Ionization Ions Mass Spectrometry Mass spectroscopy Molecular weight Nitrogen Organic carbon Organic matter Resolution Scientific imaging Soot Speciation Spectroscopy Terrestrial environments Wildfires |
| title | Enhanced Speciation of Pyrogenic Organic Matter from Wildfires Enabled by 21 T FT-ICR Mass Spectrometry |
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