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Fractionation of the Methane Isotopologues ¹³CH₄, ¹²CH₃D, and ¹³CH₃D During Aerobic Oxidation of Methane by Methylococcus Capsulatus (Bath)

Author(s)
Wang, David T.; Welander, Paula V.; Ono, Shuhei
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Abstract
Aerobic oxidation of methane plays a major role in reducing the amount of methane emitted to the atmosphere from freshwater and marine settings. We cultured an aerobic methanotroph, Methylococcus capsulatus (Bath) at 30 and 37 °C, and determined the relative abundance of ¹²CH₄, ¹³CH₄, ¹²CH₃D, and ¹³CH₃D (a doubly-substituted, or “clumped” isotopologue of methane) to characterize the clumped isotopologue effect associated with aerobic methane oxidation. In batch culture, the residual methane became enriched in ¹³C and D relative to starting methane, with D/H fractionation a factor of 9.14 (Dε/13ε) larger than that of ¹³C/¹²C. As oxidation progressed, the Δ¹³CH₃D value (a measure of the excess in abundance of ¹³CH₃D relative to a random distribution of isotopes among isotopologues) of residual methane decreased. The isotopologue fractionation factor for ¹³CH₃D/¹²CH₄ was found to closely approximate the product of the measured fractionation factors for ¹³CH₄/¹²CH₄ and ¹²CH₃D/¹²CH₄ (i.e., ¹³C/¹²C and D/H). The results give insight into enzymatic reversibility in the aerobic methane oxidation pathway. Based on the experimental data, a mathematical model was developed to predict isotopologue signatures expected for methane in the environment that has been partially-oxidized by aerobic methanotrophy. Measurement of methane clumped isotopologue abundances can be used to distinguish between aerobic methane oxidation and alternative methane-cycling processes. Keywords: Methane; Clumped isotopologues; Aerobic methane oxidation; Methanotrophic cultures; Isotopic fractionation
Date issued
2016-08
URI
http://hdl.handle.net/1721.1/118880
Department
Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences
Journal
Geochimica et Cosmochimica Acta
Publisher
Elsevier
Citation
Wang, David T. et al. “Fractionation of the Methane Isotopologues ¹³CH₄, ¹²CH₃D, and ¹³CH₃D During Aerobic Oxidation of Methane by Methylococcus Capsulatus (Bath).” Geochimica et Cosmochimica Acta 192 (November 2016): 186–202 © 2016 Elsevier
Version: Author's final manuscript
ISSN
0016-7037
0016-7037

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