He, Ar, N and C isotope compositions in Tatun Volcanic Group (TVG), Taiwan: Evidence for an important contribution of pelagic carbonates in the magmatic source
“…4 is not so much different compared to the one of the Okinawa Trough samples 64 . This distribution is also similar to the one observed for the Tatun Volcanic Group in North Taiwan 65 . Figure 4 Correlation diagram between δ 15 N values and N 2 / 36 Ar ratios of methane-rich natural gases at the West Pacific convergent plate boundary.…”
Methane emission from the geosphere is generally characterized by a radiocarbon-free signature and might preserve information on the deep carbon cycle on Earth. Here we report a clear relationship between the origin of methane-rich natural gases and the geodynamic setting of the West Pacific convergent plate boundary. Natural gases in the frontal arc basin (South Kanto gas fields, Northeast Japan) show a typical microbial signature with light carbon isotopes, high CH4/C2H6 and CH4/3He ratios. In the Akita-Niigata region – which corresponds to the slope stretching from the volcanic-arc to the back-arc –a thermogenic signature characterize the gases, with prevalence of heavy carbon isotopes, low CH4/C2H6 and CH4/3He ratios. Natural gases from mud volcanoes in South Taiwan at the collision zone show heavy carbon isotopes, middle CH4/C2H6 ratios and low CH4/3He ratios. On the other hand, those from the Tokara Islands situated on the volcanic front of Southwest Japan show the heaviest carbon isotopes, middle CH4/C2H6 ratios and the lowest CH4/3He ratios. The observed geochemical signatures of natural gases are clearly explained by a mixing of microbial, thermogenic and abiotic methane. An increasing contribution of abiotic methane towards more tectonically active regions of the plate boundary is suggested.
“…4 is not so much different compared to the one of the Okinawa Trough samples 64 . This distribution is also similar to the one observed for the Tatun Volcanic Group in North Taiwan 65 . Figure 4 Correlation diagram between δ 15 N values and N 2 / 36 Ar ratios of methane-rich natural gases at the West Pacific convergent plate boundary.…”
Methane emission from the geosphere is generally characterized by a radiocarbon-free signature and might preserve information on the deep carbon cycle on Earth. Here we report a clear relationship between the origin of methane-rich natural gases and the geodynamic setting of the West Pacific convergent plate boundary. Natural gases in the frontal arc basin (South Kanto gas fields, Northeast Japan) show a typical microbial signature with light carbon isotopes, high CH4/C2H6 and CH4/3He ratios. In the Akita-Niigata region – which corresponds to the slope stretching from the volcanic-arc to the back-arc –a thermogenic signature characterize the gases, with prevalence of heavy carbon isotopes, low CH4/C2H6 and CH4/3He ratios. Natural gases from mud volcanoes in South Taiwan at the collision zone show heavy carbon isotopes, middle CH4/C2H6 ratios and low CH4/3He ratios. On the other hand, those from the Tokara Islands situated on the volcanic front of Southwest Japan show the heaviest carbon isotopes, middle CH4/C2H6 ratios and the lowest CH4/3He ratios. The observed geochemical signatures of natural gases are clearly explained by a mixing of microbial, thermogenic and abiotic methane. An increasing contribution of abiotic methane towards more tectonically active regions of the plate boundary is suggested.
“…This likely reflects marginal (<10%) air contributions. Their δ 15 N values were +3.6‰, a pattern consistent with the signature associated with subducted nitrogen, which is later accumulated in sub‐arc mantle sources worldwide (Busigny et al., 2011; Epstein et al., 2021; Labidi et al., 2021), and previously hypothesized to contribute nitrogen to surface vents in Taiwan (Roulleau et al., 2015). Together with mantle‐derived helium, the recycled nitrogen must have been remobilized toward the surface via volcanism followed by hydrothermal interactions.…”
Identification of methane origins remains a challenging work as current diagnostic signals are often not sufficient to resolve individual formation and post‐formation processes. To address such a knowledge gap in a tectonically active and fragmented terrain, samples from mud volcanoes, gas seeps, and springs distributed along structural features onshore and offshore of Taiwan were analyzed for their isotopic compositions of methane, nitrogen, helium, dissolved inorganic carbon, CO2, and water. Our analyses yielded Δ13CH3D and Δ12CH2D2 values ranging between +1.9‰ and +7.8‰ and between +3.0‰ and +19.9‰, respectively. A portion of the samples were characterized by values that represent the thermodynamic equilibrium at temperatures of 99°–260°C. These temperature estimates, together with the bulk isotopic compositions and local geothermal gradients (25°–30°C/km), suggest that methane was formed by thermal maturation of organic matter at depths of 2–9 km below the land surface and channeled upward along faults. Other samples were found to deviate from equilibrium by varying degrees. Considering the geological background, helium isotopic ratios, and nitrogen isotopologue compositions, and methanogens detected at some sites, these gases are either abiotic in origin or a mixture of microbial and thermogenic sources. Regardless of whether the equilibrium of methane isotopologues was reached, few sites hosted by sedimentary formations were characterized by mantle‐like helium signatures, indicating decoupled origins and potential degassing of helium from the relic igneous source. Overall, these results suggest the extraction of methane and other gases from multiple depths from strata fragmented by fault displacement in an active orogenic belt.
“…SCLM = subcontinental lithospheric mantle. plausible process to produce the carbon isotopic signature and the CO 2 / 3 He of the studied fluids (Figure 7; Holland & Gilfillan, 2013;Roulleau et al, 2015). However, the 13 C CO2 values of most of the samples fall in the narrow range of −2‰ and −5‰, which is a typical signature for mantle-derived carbon.…”
Section: Sources and Origin Of Carbon Dioxidementioning
Ciomadul is the youngest volcano in the Carpathian‐Pannonian Region, Eastern‐Central Europe, which last erupted 30 ka. This volcano is considered to be inactive, however, combined evidence from petrologic and magnetotelluric data, as well as seismic tomography studies, suggests the existence of a subvolcanic crystal mush with variable melt content. The volcanic area is characterized by high CO2 gas output rate, with a minimum of 8.7 × 103 t/year. We investigated 31 gas emissions at Ciomadul to constrain the origin of the volatiles. The δ13C–CO2 and 3He/4He compositions suggest the outgassing of a significant component of mantle‐derived fluids. The He isotope signature in the outgassing fluids (up to 3.10 Ra) is lower than the values in the peridotite xenoliths of the nearby alkaline basalt volcanic field (R/Ra 5.95 Ra ± 0.01), which are representative of a continental lithospheric mantle and significantly lower than MORB values. Considering the chemical characteristics of the Ciomadul dacite, including trace element and Sr–Nd and O isotope compositions, an upper crustal contamination is less probable, whereas the primary magmas could have been derived from an enriched mantle source. The low He isotopic ratios could indicate a strongly metasomatized mantle lithosphere. This could be due to infiltration of subduction‐related fluids and postmetasomatic ingrowth of radiogenic He. The metasomatic fluids are inferred to have contained subducted carbonate material resulting in a heavier carbon isotope composition (δ13C is in the range of −1.4‰ to −4.6‰) and an increase of CO2/3He ratio. Our study shows the magmatic contribution to the emitted gases.
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