Extreme (13)C depletion of carbonates formed during oxidation of biogenic methane in fractured granite

Nat Commun. 2015 May 7:6:7020. doi: 10.1038/ncomms8020.

Abstract

Precipitation of exceptionally 13C-depleted authigenic carbonate is a result of, and thus a tracer for, sulphate-dependent anaerobic methane oxidation, particularly in marine sediments. Although these carbonates typically are less depleted in 13C than in the source methane, because of incorporation of C also from other sources, they are far more depleted in 13C (δ13C as light as -69‰ V-PDB) than in carbonates formed where no methane is involved. Here we show that oxidation of biogenic methane in carbon-poor deep groundwater in fractured granitoid rocks has resulted in fracture-wall precipitation of the most extremely 13C-depleted carbonates ever reported, δ13C down to -125‰ V-PDB. A microbial consortium of sulphate reducers and methane oxidizers has been involved, as revealed by biomarker signatures in the carbonates and S-isotope compositions of co-genetic sulphide. Methane formed at shallow depths has been oxidized at several hundred metres depth at the transition to a deep-seated sulphate-rich saline water. This process is so far an unrecognized terrestrial sink of methane.

MeSH terms

  • Calcium Carbonate / chemistry*
  • Carbon Isotopes
  • Crystallization
  • Geologic Sediments
  • Groundwater / chemistry
  • Iron / chemistry
  • Isotope Labeling
  • Methane / analysis*
  • Oxidation-Reduction
  • Silicon Dioxide / chemistry*
  • Sulfides / chemistry
  • Time Factors

Substances

  • Carbon Isotopes
  • Sulfides
  • granite
  • pyrite
  • Silicon Dioxide
  • Iron
  • Calcium Carbonate
  • Methane