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Elsevier, Chemical Geology, (382), p. 24-31, 2014

DOI: 10.1016/j.chemgeo.2014.05.024

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Methane sources and sinks in the subtropical South Pacific along 17°S as traced by stable isotope ratios

This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

We analyzed the concentration and stable carbon isotopic ratio (δ13C-CH4) of methane in the atmosphere and in dissolved methane in the water column along 17°S in the subtropical South Pacific. Additionally, the hydrogen isotopic ratios (δD-CH4) of some water samples were analyzed. The sea-air CH4 flux is high in the eastern region and off the west coast of Australia, which is related to the high concentrations of dissolved CH4 and high wind speeds. Moreover, there is a positive correlation between the CH4 and chlorophyll a concentrations at the surface. This consistency suggested that active CH4 productions related to the primary production cause surface CH4 accumulation. CH4 shows a decrease in concentration and an increase in δ13C-CH4 and δD-CH4 values from the surface to the depth of about 1000 m. The relationship between δ13C-CH4 values and CH4 concentration indicates that the isotopic enrichment of CH4 reflects microbial oxidation of CH4 with isotopic fractionation during vertical transport via vertical sinking and/or zooplankton migration. East of 120°W, δ13C-CH4 values at around 1000 m exceed -30.0‰. The relationships among the δ13C-CH4 values, CH4 concentrations, and oxygen concentrations indicate that the 13C-enriched CH4 originates not only from in situ CH4 production and oxidation but also from CH4 transported from the eastern margin off Peru. Furthermore, at a site near the Central Lau Spreading Centers in the Lau Basin, high δ13C-CH4 values (up to -21.4‰) are observed in the benthic water, suggesting a hydrothermal field source.