Abstract
Fine-grained authigenic magnetite has been recognized increasingly in iron-rich marine environments affected by methane seepage and is a major sedimentary magnetization source. However, it is unknown whether this magnetite forms via microbial or abiotic processes. We report here abundant fine magnetite crystals, in close association with goethite, within coarse-grained sediments from two adjacent methane seepage sites in the South China Sea. The magnetite- and goethite-rich horizons have sharply increased Zr/Ti, Zr/Rb, Ti/Al, and Fe/Al ratios, probably reflecting deposition by turbidity currents. Deeper intervals have elevated pyrite content, positive δ34S excursions of chromium reducible sulfur, and low magnetic susceptibilities, which is consistent with past sulfate-driven anaerobic oxidation of methane in environments with dynamically variable seepage intensity. In magnetically extracted aggregates (>63 μm), magnetite particles are mainly clustered euhedral crystals with 0.2–0.8 μm sizes, which will likely impact sedimentary magnetic signals. The fine, euhedral crystalline nature of the magnetite suggests formation in sulfide-free, ferrous iron-rich sedimentary environments. Based on 16S rRNA gene sequences, anaerobic methanotrophic archaea coincide with pyrite rich horizons. In contrast, two co-occurring methanogenic archaea groups of the Methanomicrobia class (mainly Methanosarcina and Methanocella) are particularly abundant in turbidites but have low abundance in all other horizons. Increased Methanomicrobia abundances suggest that this class of archaea may be involved in microbial iron reduction in turbidites with abundant goethite as a reactive iron source, and that they apparently trigger magnetite formation. Our findings provide new clues to microbial magnetite formation in iron-rich marine sediments.
