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Research on the origin and source of hydrate-bound gas and its relationship to deep conventional oil and gas accumulation in a basin is critical to understanding the accumulation mechanism of gas hydrates and to resource evaluation of gas hydrate accumulation. In this study, the hydrate-bound gas obtained via pressure coring and the production gas recovered during a production test on a gas hydrate reservoir in the Shenhu area offshore of Southern China were tested and discussed. The geochemical analysis results indicate that methane is the predominant gas, and heavier hydrocarbons (C2+) are also present but in low concentrations. The molecular compositions of the hydrate gas recovered from two production test sites are similar to those of the hydrate-bound gas acquired via pressure coring. In addition to the isotopic composition of the methane, the carbon and hydrogen isotopes of the C2+ hydrocarbons were obtained for the first time. The δ13C isotopes of the methane range from −66.6‰ to −46.2‰, indicating that the hydrate-bound gases have a mixed origin, containing both biogenic and thermogenic gases. The plot of δ13C 1 versus δ13C 2 suggests that the biogenic and thermogenic hydrocarbons were derived from marine organic matter and terrestrial organic matter, respectively. The isotopic characterization of the hydrate-bound gas reveals that the thermogenic hydrate gas contains both humic-type gas and sapropel-type gas, but the sapropel-type gas is predominant. The source rocks of the thermogenic hydrate gas are interpreted to be both the gas-prone coal measure strata of the Enping Formation and the oil-prone medium-deep lacustrine strata of the Wenchang Formation, the latter of which contributed more to the hydrocarbon supply of the gas hydrates. In addition, the maturity of the source rocks of the thermogenic hydrate gas may be lower than that of the deeply buried conventional hydrocarbons discovered in the Baiyun Sag-Panyu Low Uplift area. The seismic profile crossing the shallow gas hydrate accumulations and deep conventional gas reservoirs clearly shows that the proven LW3-1 thermogenic gas reservoir communicated with the gas hydrate stability zone through vertical migration pathways formed by high-angle faults and gas chimneys. This indicates that there was a cogenetic relationship between the thermogenic hydrate gas and the deep conventional hydrocarbon reservoir, which was supplied the thermogenic gas derived from both the Wenchang and Enping formations. The major implications of this finding are that it confirms, rather than theorizes, the identity of the hydrocarbon source rocks of the thermogenic hydrate gas in the Shenhu area for the first time, and it demonstrates the coupling relationship between the shallow gas hydrate accumulations and the deep conventional reservoirs proposed in previous studies. The mechanisms of hydrocarbon migration and gas hydrate accumulation in the production test gas hydrate reservoirs in the Shenhu area were also identified, providing a valuable reference for subsequent exploration and for the potential exploitation of gas hydrate reservoirs in the South China Sea. • The δ13C and δD isotopes of the heavier hydrocarbons (C2+) in the Shenhu area are obtained for the first time. • The origin of the hydrate gas obtained from the second trial production well in the Shenhu area is confirmed. • The hydrocarbon source rocks of the thermogenic hydrate gas in the Shenhu area are identified. • Coupled paragenetic relationship between shallow gas hydrate and deep petroleum system is revealed. [ABSTRACT FROM AUTHOR]

Abstract: In this study, a simple solvent dilution followed by highly selective and sensitive gas chromatography–triple quadrupole mass spectrometry (GC–MS–MS) detection was employed to quantify diamondoids in crude oils. Runtime parameters, i.e., parent and daughter ions, collision energy (CE) and scan time, were optimized to obtain maximum selectivity and sensitivity for target analytes. Under optimum conditions, the reproducibility and accuracy of the method were tested and found to be satisfactory. Comparison of GC–MS–MS and GC–MS methods for the determination of diamondoids indicates that GC–MS–MS yields higher sensitivity (method quantitation limits of 0.08–0.37μg/goil) and better selectivity than GC–MS (method quantitation limits of 0.78–8.44μg/goil) due to the elimination of matrix ion interferences using the selected reaction monitoring (SRM) mode. In addition, quantitative data confirm that group separation has a considerable effect on the quantification of diamondoids and the effect appears to depend on multiple factors. Two crude oils (TZ261 and TD2) from the Tarim Basin, China were used to evaluate the GC–MS–MS method. The results prove that the GC–MS–MS method is a promising tool for quantitative analysis of diamondoids in crude oils, especially for oil samples with low diamondoid concentrations. [Copyright &y& Elsevier]

• The gas production from hydrate dissociation accounting for about 85%. • Analysis of the radius of the hydrate dissociation area in this production test. • Five-year prediction of long-term influence radius of pressure drop. • Exploration of favorable areas for the formation of secondary hydrates. • Analysis of the response of pressure and temperature of hydrate reservoirs. The first offshore natural gas hydrate production test of China in 2017 has proved the feasibility of hydrate exploitation from clayey-silt reservoirs, which possesses the highest reservoirs than other types of hydrate resources. However, owing to the absence of monitoring wells in this production test, the hydrate dissociation behavior cannot be analyzed through pressure and temperature changes of hydrate reservoirs. This paper focuses on the simulation study on the detailed response of the temperature and pore pressure of hydrate reservoirs of Well SHSC-4 during the gas production by depressurization. Meanwhile, it highlights the analysis of favorable areas for the formation of secondary hydrates and the influence of the secondary hydrates on pressure and temperature field of hydrate reservoirs. The simulation results indicate that in the first 60 days, the hydrate reservoirs feature a dissociation radius of about 5 m, and the gas production from hydrate dissociation accounts for about 85%. After 1 year, 2 years and 5 years of hydrate exploitation, the influence radius of low-pressure area (<10 MPa) is 15 m, 16 m and 17 m, respectively, suggesting that the hydrate reservoirs have higher gas production efficiency in the first year. Furthermore, the temperature and pressure of hydrate reservoirs are not favorable to the formation of secondary hydrates in the first 60 days. In long-term production, secondary hydrates are mainly formed at hydrate dissociation front. This can increase the pore pressure and further decrease the effective stress in the local areas of hydrate reservoirs, thus affecting mechanical stability of the local hydrate reservoirs. [ABSTRACT FROM AUTHOR]

Upward diffusion of dissolved methane and associated anaerobic oxidation of methane (AOM) coupled with microbial sulfate reduction (MSR) are widespread in normal hemipelagic sediments of continental margins. The occurrence of authigenic sulfur enrichment in such sediments is usually regarded as an indicator of AOM; however, extensive MSR and authigenic iron sulfide generation also occur in turbidites. Therefore, research attention should be directed toward determining the geochemical features of authigenic sulfur mineralization in methane-rich background sediments and turbidites. Here we report the sedimentology and geochemical composition of sediments from four piston cores (CL30, CL44, CL47, and CL3A) containing turbidite layers from methane-rich areas of the South China Sea. The turbidite layers were deposited at 17–15 kyr BP or earlier during the last glacial period and were located above the present sulfate–methane transition zone (SMTZ). The median grain size, proportion of sand-sized grains, and Si, Ti, K, and Zr contents show marked elevation in the turbidite layers compared with the background sediments, indicating the input of large amounts of terrigenous detrital matter with coarser grains. High total sulfur (TS) contents and low δ34S AIS values (AIS: acid-insoluble sulfur) (−35.2‰ to −26.1‰) are observed within turbidite layers relative to the background hemipelagic sediments in core CL44. These results suggest that intensive sulfidization occurred as a result of enhanced organoclastic sulfate reduction rates in turbidite horizons, which were probably caused by the resultant decrease in downward oxygen flux and waning bioturbation after rapid deposition of turbidites. In comparison, TS contents are higher and δ34S AIS values are positive (0.2‰–46.8‰) within the SMTZ on account of the rapid consumption of sulfate and build-up of isotopically heavier hydrogen sulfide pools via intensive AOM. Moreover, authigenic barium (Ba) enrichments commonly occur in the depth interval immediately above the SMTZ rather than within turbidite layers; therefore, they serve as a useful indicator of the position of the SMTZ. This study presents distinct differences in the geochemical compositions of turbidity deposits and methane-rich background sediments and highlights that a multi-proxy approach including sedimentological and geochemical analyses should be used to constrain the types of MSR in deep-sea sediments, given the common occurrence of turbidites and subsurface methane release in marginal deep-sea areas. It is also suggested that if applied with caution, S–C–Ba geochemical patterns can be used to identify palaeo-SMTZs and palaeo methane-rich zones in turbidite-containing strata. • Both authigenic sulfur enrichment occurred in turbidite and seep sediments in the SCS. • Sulfidization in turbidite layer may be characterized by OSR with high SRR. • Combined S, C, and Ba geochemical patterns can be used to identify turbidite and seeps. [ABSTRACT FROM AUTHOR]