Multiple Sulfur Isotopes of Iron Sulfides From Thick Greigite‐Bearing Sediments Indicate Anaerobic Oxidation and Possible Leakages of Coastal Methane

Abstract

Magnetic greigite may be a valuable indicator for methane emissions in the geological past, if its formation pathway and diagenetic environment can be unambiguously defined. Here, we investigate sulfur isotopic compositions of iron sulfides and ferrous iron concentrations of thick greigite‐bearing sediments (TGBSs) in the South Yellow Sea, a shallow marginal sea with strong methane emissions. For the first time, isotopically heavy iron sulfides (up to 28.7‰ in δ34S and 0.19‰ in Δ33S) and enrichments of ferrous iron in the TGBSs are observed. We interpret the data as indicating synchronic occurrences of anaerobic oxidation of methane coupled to sulfate and iron reductions, which occur in coastal methanic zones with limited sulfate availability and therefore probably imply leakages of methane. Consequently, we suggest that greigite is a promising geological indicator for tracing methane liberated from coastal sediments, accounting for ∼60% of the currently rising global marine methane budget.