<p>Methane (CH <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({}_{4}\)</EquationSource> </InlineEquation>) is common in fluids sourced from low-temperature hydrating (serpentinizing) peridotites, but the carbon sources, rates, and mechanisms of CH <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\({}_{4}\)</EquationSource> </InlineEquation> formation are uncertain. In CH <InlineEquation ID="IEq3"> <EquationSource Format="TEX">\({}_{4}\)</EquationSource> </InlineEquation> dissolved in groundwaters pumped from four wells of up to 400&#xa0;m depth in the Samail Ophiolite, Oman, we observed <InlineEquation ID="IEq4"> <EquationSource Format="TEX">\({}^{14}\)</EquationSource> </InlineEquation> C contents ranging from radiocarbon-dead to <InlineEquation ID="IEq5"> <EquationSource Format="TEX">\(0.3038\pm 0.0015\)</EquationSource> </InlineEquation> fraction modern. Chemical and isotopic analyses of groundwaters and hydrocarbon gases align with microbiological data indicating that methanogens inhabiting H <InlineEquation ID="IEq6"> <EquationSource Format="TEX">\({}_{2}\)</EquationSource> </InlineEquation>-rich <InlineEquation ID="IEq7"> <EquationSource Format="TEX">\((&gt;100 \mu \text{mol }{\text{L}}^{-1}\)</EquationSource> </InlineEquation>), <InlineEquation ID="IEq8"> <EquationSource Format="TEX">\({\text{pH}}&gt;11\)</EquationSource> </InlineEquation> fluids produce the <InlineEquation ID="IEq9"> <EquationSource Format="TEX">\({}^{14}\)</EquationSource> </InlineEquation> C-rich CH <InlineEquation ID="IEq10"> <EquationSource Format="TEX">\({}_{4}\)</EquationSource> </InlineEquation>. This “young” microbial CH <InlineEquation ID="IEq11"> <EquationSource Format="TEX">\({}_{4}\)</EquationSource> </InlineEquation> constitutes a portion of the light hydrocarbons dissolved in the subsurface fluids, which also contain a distinct pool of relatively <sup>13</sup>C- and <sup>2</sup>H-enriched CH <InlineEquation ID="IEq12"> <EquationSource Format="TEX">\({}_{4}\)</EquationSource> </InlineEquation> and C<sub>2+</sub> alkanes that are likely abiotic and older. Our study of groundwaters accessed via wells complements prior studies, which have mostly found <sup>14</sup>C-free, gas-phase CH<sub>4</sub> from natural seeps in ophiolites and interpreted an abiotic source from unsaturated rocks. Most importantly, our radiocarbon data show that transport and localized conversion of atmospheric CO <InlineEquation ID="IEq13"> <EquationSource Format="TEX">\({}_{2}\)</EquationSource> </InlineEquation> to CH <InlineEquation ID="IEq14"> <EquationSource Format="TEX">\({}_{4}\)</EquationSource> </InlineEquation> in peridotites reacting with water at temperatures &lt; 60 ˚C occurs at surprisingly fast rates, within the last <InlineEquation ID="IEq15"> <EquationSource Format="TEX">\(10\hspace{0.17em}000\)</EquationSource> </InlineEquation> years.</p>

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Active conversion of atmospheric carbon dioxide to methane in peridotites of the Samail Ophiolite, Oman

  • Daniel B. Nothaft,
  • Alexis S. Templeton,
  • Peter B. Kelemen,
  • Eric S. Boyd,
  • Juerg M. Matter

摘要

Methane (CH \({}_{4}\) ) is common in fluids sourced from low-temperature hydrating (serpentinizing) peridotites, but the carbon sources, rates, and mechanisms of CH \({}_{4}\) formation are uncertain. In CH \({}_{4}\) dissolved in groundwaters pumped from four wells of up to 400 m depth in the Samail Ophiolite, Oman, we observed \({}^{14}\) C contents ranging from radiocarbon-dead to \(0.3038\pm 0.0015\) fraction modern. Chemical and isotopic analyses of groundwaters and hydrocarbon gases align with microbiological data indicating that methanogens inhabiting H \({}_{2}\) -rich \((>100 \mu \text{mol }{\text{L}}^{-1}\) ), \({\text{pH}}>11\) fluids produce the \({}^{14}\) C-rich CH \({}_{4}\) . This “young” microbial CH \({}_{4}\) constitutes a portion of the light hydrocarbons dissolved in the subsurface fluids, which also contain a distinct pool of relatively 13C- and 2H-enriched CH \({}_{4}\) and C2+ alkanes that are likely abiotic and older. Our study of groundwaters accessed via wells complements prior studies, which have mostly found 14C-free, gas-phase CH4 from natural seeps in ophiolites and interpreted an abiotic source from unsaturated rocks. Most importantly, our radiocarbon data show that transport and localized conversion of atmospheric CO \({}_{2}\) to CH \({}_{4}\) in peridotites reacting with water at temperatures < 60 ˚C occurs at surprisingly fast rates, within the last \(10\hspace{0.17em}000\) years.