Elemental sulfur in northern South China Sea sediments and its significance

Elemental sulfur (ES) is one of the intermediates in the inorganic sulfur cycle and thus plays a key role in the fractionation of stable sulfur isotopes in different reservoirs and the marine environment. In this study, solid ES is discovered in sediments near the Jiulong Methane Reef in the northern South China Sea by scanning electron microscopy and Raman spectroscopy. Combining the morphology and distribution of ES, pyrite concentrations, and sulfur isotopes, we conclude that: (1) solid ES coexists with pyrite microcrystals and sulfide (oxyhydr)oxides as well as clay minerals, and they are mainly distributed on the surface of mineral aggregates; (2) ES mainly occurs within and near the sulfate-methane transition zone (SMTZ) despite little morphological diversity; (3) ES formation might be related to hydrogen sulfide oxidation and is therefore linked with fluctuations in the SMTZ. Within the SMTZ, hydrogen sulfide is produced and pyrite precipitates because of enhanced anaerobic oxidation of methane coupled with dissimilatory sulfate reduction. This enhances the efficiency of the inorganic sulfur cycle and provides favorable conditions for ES formation. The discovery of solid ES in sediments near the Jiulong Methane Reef suggests an important relationship with SMTZ fluctuations that could have implications for the evolution of methane hydrate in the South China Sea.