4.7 Article

Quantification of the sources of sedimentary organic carbon at methane seeps: A case study from the South China Sea

Journal

CHEMICAL GEOLOGY
Volume 627, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.chemgeo.2023.121463

Keywords

Methane seepage; Anaerobic oxidation of methane; Organic carbon; Carbon stable isotopes; Radiocarbon; South China Sea

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Large amounts of methane stored as methane hydrate along continental margins can release substantial quantities of methane when destabilized. Microorganisms in the marine subsurface convert methane into organic matter, which acts as a long-term carbon sink and mitigates the effect of methane as a greenhouse gas. However, the controls on the formation and consumption of sedimentary organic matter at marine seeps are poorly understood, hindering the accurate quantification of carbon burial and its role in the marine carbon cycle.
Large amounts of methane are stored along continental margins in the form of methane hydrate. Methane hy-drate is sensitive to environmental change, resulting in the release of substantial quantities of methane upon its destabilization. In the marine subsurface, microorganisms consume most of the methane in the sulfate-methane transition zone and convert a certain amount of methane into organic matter. Burial of such organic matter deriving from methane oxidation represents a long-term carbon sink, therefore mitigating the effect of a prominent greenhouse gas on global warming. However, the controls on the formation and consumption of sedimentary organic matter at marine seeps remain poorly constrained, impeding accurate quantification of carbon burial at seeps and its role in the marine carbon cycle. To gain new insight on the effect of seeps on carbon burial, sediments from two seep sites of the South China Sea (Site F, Haiyang 4) and a nearby reference site (Jiulong canyon) were analyzed for total organic carbon contents (TOC), 813CTOC and A14C values, total inor-ganic carbon contents (TIC) and 813CTIC values, as well as organic nitrogen (N) contents. Depth distributions reveal that the TOC at seeps (Site F, 0.55% +/- 0.08%, Haiyang 4, 0.67% +/- 0.11%) is higher than in sediments not affected by seepage (Jiulong canyon, 0.50% +/- 0.10%). The enrichment of total sulfur, high TIC, and negative 813CTIC values in sediments from Site F and Haiyang 4 agrees with locally prominent sulfate-driven anaerobic oxidation of methane (AOM) and resultant precipitation of authigenic carbonate. At the two seep sites, the sediments are characterized by more negative 813CTOC and A14C values and a lower TOC/N ratio, indicating a contribution of the microbial fixation of 13C-depleted methane to the local pool of sedimentary organic matter. A linear increase in 14C ages of organic carbon with sediment depth at the reference site indicates steady depo-sitional conditions, whereas the 14C age of organic carbon at seeps is typified by contributions of methanotrophy-derived carbon. A Delta 14C mass balance approach shows that carbon derived from fossil methane accounts for at least 10 to 20% of the organic carbon preserved in the sediments. By comparing seeps, hydrate-bearing sedi-ments, modern coastal sediments, and Archaean rocks, it becomes apparent that the carbon stable isotope composition of organic carbon in seep sediments is mainly controlled by the rate of methane oxidation and marine primary productivity.

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