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In this study, we used pore water dissolved inorganic carbon (DIC), SO 4 2− , Ca 2+ and Mg 2+ gradients at the sulfate-methane transition zone (SMTZ) to estimate biogeochemical fluxes for cored sediments collected offshore SW Taiwan. Net DIC flux changes (Δ DIC-Prod ) were applied to determine the proportion of sulfate consumption by organic matter oxidation (heterotrophic sulfate reduction) and anaerobic oxidation of methane (AOM), and to determine reliable CH 4 fluxes at the SMTZ. Our results show that SO 4 2− profiles are mainly controlled by AOM rather than heterotrophic sulfate reduction. Refinement of CH 4 flux estimates enhance our understanding of methane abundance from deep carbon reservoirs to the SMTZ. Concentrations of chloride (Cl − ), bromide (Br − ) and iodide (I − ) dissolved in pore water were used to identify potential sources that control fluid compositions and the behavior of dissolved ions. Constant Cl − concentrations throughout ∼30 m sediment suggest no influence of gas hydrates for the compositions within the core. Bromide (Br − ) and Iodine (I − ) concentrations increase with sediment depth. The I − /Br − ratio appears to reflect organic matter degradation. SO 4 2− concentrations decrease with sediment depth at a constant rate, and sediment depth profiles of Br − and I − concentrations suggests diffusion as the main transport mechanism. Therefore diffusive flux calculations are reasonable. Coring sites with high CH 4 fluxes are more common in the accretionary wedge, amongst thrust faults and fractures, than in the passive continental margin offshore southwestern Taiwan. AOM reactions are a major sink for CH 4 passing upward through the SMTZ and prevent high methane fluxes in the water column and to the atmosphere.

Geochemical data (CH4, SO42−, I−, Cl−, particulate organic carbon (POC), δ13C-CH4, and δ13C-CO2) are presented from the upper 30 m of marine sediment on a tectonic submarine accretionary wedge offshore southwest Taiwan. The sampling stations covered three ridges (Tai-Nan, Yung-An, and Good Weather), each characterized by bottom simulating reflectors, acoustic turbidity, and different types of faulting and anticlines. Sulfate and iodide concentrations varied little from seawater-like values in the upper 1–3 m of sediment at all stations; a feature that is consistent with irrigation of seawater by gas bubbles rising through the soft surface sediments. Below this depth, sulfate was rapidly consumed within 5–10 m by anaerobic oxidation of methane (AOM) at the sulfate-methane transition. Carbon isotopic data imply a mainly biogenic methane source. A numerical transport-reaction model was used to identify the supply pathways of methane and estimate depth-integrated turnover rates at the three ridges. Methane gas ascending from deep layers, facilitated by thrusts and faults, was by far the dominant term in the methane budget at all sites. Differences in the proximity of the sampling sites to the faults and anticlines mainly accounted for the variability in gas fluxes and depth-integrated AOM rates. By comparison, methane produced in situ by POC degradation within the modeled sediment column was unimportant. This study demonstrates that the geochemical trends in the continental margins offshore SW Taiwan are closely related to the different geological settings.

Source at https://doi.org/10.1002/2017GC006798 To systematically quantify the production, consumption, and migration of methane, 210 sediment cores were collected from offshore southwestern Taiwan and analyzed for their gas and aqueous geochemistry. These data, combined with published results, were used to calculate the diffusive methane fluxes across different geochemical transitions and to develop scenarios of mass balance and constrain deep microbial and thermogenic methane production rates within the accretionary prism. The results showed that methane diffusive fluxes ranged from 2.71 × 10−3 to 2.78 × 10−1 and from –1.88 × 10−1 to 3.97 mmol m−2 d−1 at the sulfate‐methane‐transition‐zone (SMTZ) and sediment‐seawater interfaces, respectively. High methane fluxes tend to be associated with structural features, suggesting a strong structural control on the methane transport. A significant portion of ascending methane (>50%) is consumed by anaerobic oxidation of methane at the SMTZ at most sites, indicating effective biological filtration. Gas compositions and isotopes revealed a transition from the predominance of microbial methane in the passive margin to thermogenic methane at the upper slope of the active margin and onshore mud volcanoes. Methane production and consumption at shallow depths were nearly offset with a small fraction of residual methane discharged into seawater. The flux imbalance arose primarily due to the larger production of methane through deep microbial and thermogenic processes at a magnitude of 1512–43,096 Tg Myr−1 and could be likely accounted for by the sequestration of methane into hydrate forms, and clay absorption.

Widely distributed bottom simulating reflectors (BSRs) imply the potential existence of gas hydrates offshore southwestern Taiwan. To compare the distribution of methane concentrations along passive and active margins in the region, bottom waters and cored sediments were collected during four cruises from 2005 to 2006. The results reveal that sites with high methane concentrations are predominantly distributed in the active margin and site GS5 is the only site that contains very high methane concentrations in the passive margin of studied area. Anomalously high methane fluxes still can be obtained from the calculation of diffusive methane flux, although there might be some gas leakage during or after sampling procedures. The profiles of methane and sulfate concentration reveal very shallow depths of the sulfate–methane interface (SMI) at some sites. There is evidence that sulfate reduction is mainly driven by the process of anaerobic methane oxidation. Thus, sulfate fluxes can be used as a proxy for methane fluxes through the use of diffusion equations; and the results show that the fluxes are very high in offshore southwestern Taiwan. The depths of the SMI are different at sites GH6 and C; however, both methane profiles reveal parallel methane gradients below the SMI. This might be because of methane migration to surface sediments from the same reservoir with the same diffusion rates. Although BSRs are widely distributed both in the active margin and in the passive margin, most sites with high methane concentrations have been found in the active margin. Therefore, the specific tectonic settings in offshore SW Taiwan might strongly control the stability of gas hydrates, and thus affect the methane concentrations and fluxes of the sediments and sea waters. Furthermore, the carbon isotopic composition of methane shows that a biogenic gas source is dominant at shallower depth; however, some thermogenic gases might be introduced through the fracture/fault zones from deeper source in the active region of studied area.

Water column samples were collected systematically in several potential gas hydrate areas offshore of SW Taiwan for analysis of dissolved gases. Some these samples show unusually high dissolved methane concentrations at sites A, B, C, and H of cruise ORI-765. The profiles of helium concentrations in the dissolved gases of the water column also exhibit consistent results with an increasing trend toward the seafloor. The 3He/4He ratios range from 0.2 to 0.4 times that of the atmospheric air ratio after air correction, which fall in the range of typical crustal gas composition and are similar to those of on-shore mud volcanoes in SW Taiwan. This indicates that gases are venting actively from the seafloor in the region and may share similar gas sources to on-shore mud volcanoes. The venting gases are considered to have originated from dissociation of gas hydrates and/or a deeper gas reservoir.