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Nonequilibrium clumped isotope signals in microbial methane

Author(s)
Wang, David T.; Gruen, Danielle Sarah; Lollar, Barbara Sherwood; Hinrichs, Kai-Uwe; Stewart, Lucy C.; Holden, James F.; Hristov, Alexander N.; Pohlman, John W.; Morrill, Penny L.; Könneke, Martin; Delwiche, Kyle Brook; Reeves, Eoghan; Sutcliffe, Chelsea N.; Ritter, Daniel J.; Seewald, Jeffrey S.; McIntosh, Jennifer C.; Hemond, Harold F.; Kubo, Michael D.; Cardace, Dawn; Hoehler, Tori M.; Ono, Shuhei; ... Show more Show less
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Abstract
Methane is a key component in the global carbon cycle with a wide range of anthropogenic and natural sources. Although isotopic compositions of methane have traditionally aided source identification, the abundance of its multiply-substituted “clumped” isotopologues, e.g., 13CH3D, has recently emerged as a proxy for determining methane-formation temperatures; however, the impact of biological processes on methane’s clumped isotopologue signature is poorly constrained. We show that methanogenesis proceeding at relatively high rates in cattle, surface environments, and laboratory cultures exerts kinetic control on 13CH3D abundances and results in anomalously elevated formation temperature estimates. We demonstrate quantitatively that H2 availability accounts for this effect. Clumped methane thermometry can therefore provide constraints on the generation of methane in diverse settings, including continental serpentinization sites and ancient, deep groundwaters.
Date issued
2015-03
URI
http://hdl.handle.net/1721.1/95903
Department
Massachusetts Institute of Technology. Department of Civil and Environmental Engineering; Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences
Journal
Science Express
Publisher
American Association for the Advancement of Science (AAAS)
Citation
Wang, David T., Danielle S. Gruen, Barbara Sherwood Lollar, Kai-Uwe Hinrichs, Lucy C. Stewart, James F. Holden, Alexander N. Hristo et al. "Nonequilibrium clumped isotope signals in microbial methane." Science Express (5 March 2015). 8 p.
Version: Author's final manuscript
ISSN
0036-8075
1095-9203

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