Nonequilibrium clumped isotope signals in microbial methane

David T. Wang, Danielle S. Gruen, Barbara Sherwood Lollar, Kai Uwe Hinrichs, Lucy C. Stewart, James F. Holden, Alexander N. Hristov, John W. Pohlman, Penny L. Morrill, Martin Könneke, Kyle B. Delwiche, Eoghan P. Reeves, Chelsea N. Sutcliffe, Daniel J. Ritter, Jeffrey S. Seewald, Jennifer C. McIntosh, Harold F. Hemond, Michael D. Kubo, Dawn Cardace, Tori M. HoehlerShuhei Ono

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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 (for example, 13CH3D) has recently emerged as a proxy for determining methane-formation temperatures. However, the effect 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.

Original languageEnglish (US)
Pages (from-to)428-431
Number of pages4
JournalScience
Volume348
Issue number6233
DOIs
StatePublished - Apr 24 2015

All Science Journal Classification (ASJC) codes

  • General

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    Wang, D. T., Gruen, D. S., Sherwood Lollar, B., Hinrichs, K. U., Stewart, L. C., Holden, J. F., Hristov, A. N., Pohlman, J. W., Morrill, P. L., Könneke, M., Delwiche, K. B., Reeves, E. P., Sutcliffe, C. N., Ritter, D. J., Seewald, J. S., McIntosh, J. C., Hemond, H. F., Kubo, M. D., Cardace, D., ... Ono, S. (2015). Nonequilibrium clumped isotope signals in microbial methane. Science, 348(6233), 428-431. https://doi.org/10.1126/science.aaa4326