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Large Hydrogen Isotope Fractionation Distinguishes Nitrogenase-Derived Methane from Other Methane Sources

Author(s): Zhang, Xinning; Luxem, Katja E; Leavitt, William D

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dc.contributor.authorZhang, Xinning-
dc.contributor.authorLuxem, Katja E-
dc.contributor.authorLeavitt, William D-
dc.date.accessioned2022-01-25T14:51:54Z-
dc.date.available2022-01-25T14:51:54Z-
dc.date.issued2020-09-17en_US
dc.identifier.citationLuxem, Katja E., William D. Leavitt, and Xinning Zhang. "Large hydrogen isotope fractionations distinguish nitrogenase-derived methane from other sources." Applied and Environmental Microbiology 86 (2020). doi:10.1128/AEM.00849-20.en_US
dc.identifier.issn0099-2240-
dc.identifier.urihttp://arks.princeton.edu/ark:/88435/pr11g0ht6s-
dc.description.abstractBiological nitrogen fixation is catalyzed by the enzyme nitrogenase. Two forms of this metalloenzyme, the vanadium (V)- and iron (Fe)-only nitrogenases, were recently found to reduce small amounts of carbon dioxide (CO2) into the potent greenhouse gas methane (CH4). Here, we report carbon (13C/12C) and hydrogen (2H/1H) stable isotopic compositions and fractionations of methane generated by V- and Fe-only nitrogenases in the metabolically versatile nitrogen fixer Rhodopseudomonas palustris. The stable carbon isotope fractionation imparted by both forms of alternative nitrogenase are within the range observed for hydrogenotrophic methanogenesis (13αCO2/CH4 = 1.051 ± 0.002 for V-nitrogenase and 1.055 ± 0.001 for Fe-only nitrogenase; values are means ± standard errors). In contrast, the hydrogen isotope fractionations (2αH2O/CH4 = 2.071 ± 0.014 for V-nitrogenase and 2.078 ± 0.018 for Fe-only nitrogenase) are the largest of any known biogenic or geogenic pathway. The large 2αH2O/CH4 shows that the reaction pathway nitrogenases use to form methane strongly discriminates against 2H, and that 2αH2O/CH4 distinguishes nitrogenase-derived methane from all other known biotic and abiotic sources. These findings on nitrogenase-derived methane will help constrain carbon and nitrogen flows in microbial communities and the role of the alternative nitrogenases in global biogeochemical cycles.en_US
dc.language.isoen_USen_US
dc.relation.ispartofApplied and Environmental Microbiologyen_US
dc.rightsFinal published version. This is an open access article.en_US
dc.titleLarge Hydrogen Isotope Fractionation Distinguishes Nitrogenase-Derived Methane from Other Methane Sourcesen_US
dc.typeJournal Articleen_US
dc.identifier.doidoi:10.1128/AEM.00849-20-
dc.identifier.eissn1098-5336-
pu.type.symplectichttp://www.symplectic.co.uk/publications/atom-terms/1.0/journal-articleen_US

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