Natural gas containing hydrogen sulphide （H2S） has been found in several petroliferous basins in China, such as the Sichuan Basin, Bohai Bay Basin, Ordos Basin, Tarim Basin, etc. Natural gas with higher HES contents...Natural gas containing hydrogen sulphide （H2S） has been found in several petroliferous basins in China, such as the Sichuan Basin, Bohai Bay Basin, Ordos Basin, Tarim Basin, etc. Natural gas with higher HES contents （HES 〉5 % mol.） is mostly distributed in both the gas reservoirs of Dukouhe, Luojiazhai, Puguang and Tieshanpo, which belong to the Triassic Feixianguan Formation in the northeastern Sichuan Basin and those of the Kongdian-Shahejie formations in the northeastern Jinxian Sag of the Jizhong Depression, Bohai Bay Basin. In the Sichuan Basin, the HES contents of natural gas average over 9% and some can be 17 %, while those of the Bohai Bay Basin range from 40 % to 92 %, being then one of the gas reservoirs with the highest H2S contents in the world. Based on detailed observation and sample analysis results of a total 5000 m of core from over 70 wells in the above-mentioned two basins, especially sulfur isotopic analysis of gypsum, brimstone, pyrite and natural gas, also with integrated study of the geochemical characteristics of hydrocarbons, it is thought that the natural gas with high HES contents resulted from thermochemical sulfate reduction （TSR） reactions. Among them, the natural gas in the Feixianguan Formation resulted from TSR reactions participated by hydrocarbon gas, while that in the Zhaolanzhuang of the Jinxian Sag being the product of TSR participated by crude oil. During the consumption process of hydrocarbons due to TSR, the heavy hydrocarbons were apt to react with sulfate, which accordingly resulted in the dry coefficient of natural gas increasing and the carbon isotopes becoming heavier.展开更多
TSR is an interaction between sulfate and hydrocarbons, occurring widely in carbonate reservoirs. Because this process can produce a large amount of noxious acidic gases like H2S, it has drawn seri- ous concern recent...TSR is an interaction between sulfate and hydrocarbons, occurring widely in carbonate reservoirs. Because this process can produce a large amount of noxious acidic gases like H2S, it has drawn seri- ous concern recently. This paper reports an experiment that simulated an interaction between different minerals and hydrocarbon fluids under different temperature and time using a confined gold-tube system. The results showed that the main mineral that initiates TSR is MgSO4, and adding a certain amount of NaCl into the reactive system can also promote TSR and yield more H2S. The H2S produced in TSR is an important incentive for the continuous oxidative degradation of crude oils. For instance, the yield of oil-cracking gases affected by TSR was twice of that not affected by TSR while the yield of TSR-affected methane was even higher, up to three times of that unaffected by TSR. The carbon iso- topes of wet gases also became heavier. All of the above illustrated that TSR obviously motivates the oxidative degradation of crude oils, which makes the gaseous hydrocarbon generation sooner and increases the gas dryness as well. The study on this process is important for understanding the TSR mechanism and the mechanism of natural gas generation in marine strata.展开更多
The Sinian Dengying Formation gas pool in Weiyuan is the oldest large-scale sulfur-bearing gas field in China, which has a H2S content ranging from 0.8% to 1.4%. The Cambrian Xixiangchi Formation gas pool discovered r...The Sinian Dengying Formation gas pool in Weiyuan is the oldest large-scale sulfur-bearing gas field in China, which has a H2S content ranging from 0.8% to 1.4%. The Cambrian Xixiangchi Formation gas pool discovered recently above the Dengying Formation contains gas geochemical behaviors similar to those of Dengying Formation but different in sulfur isotopes of H2S. Investigations show that though these two Sinian and Cambrian gas pools are separate ones, they share the same Cambrian source rock. The higher dry coefficient, heavier carbon isotopes, sulfur isotopes of sulfide, lower filling of gas pools, formation water characteristics, reservoir properties and H2S distribution, indicate that H2S in both the Sinian and Cambrian gas pools originates from TSR. The sulfur isotopes of sulfates have shown that H2S was formed in respective pools, namely hydrocarbons charged into the pools reacted with the Dengying Formation and the Xixiangchi Formation gypsum (TSR), respectively, to form H2S. Compared with sulfur isotopes of sulfates in each pool, δ34S values of H2S are 8‰ lighter for the Dengying Formation pool and 12‰ lighter for the Xixiangchi Formation pool, respectively, which is attributed to the difference in temperatures of TSR occurrence. The reservoir temperature of the Xixiangchi Formation pool is about 40℃ lower than that of the Dengying Formation pool. Temperature plays a controlling role in both the sulfur isotopic fractionation and amounts of H2S generation during TSR.展开更多
With the discoveries of a series of large gas fields in the northeast of Sichuan Basin, such as Puguang and Longgang gas fields, the formation mechanism of the gas reservoir containing high H2S in the ancient marine c...With the discoveries of a series of large gas fields in the northeast of Sichuan Basin, such as Puguang and Longgang gas fields, the formation mechanism of the gas reservoir containing high H2S in the ancient marine carbonate formation in superposition-basin becomes a hot topic in the field of petroleum geology. Based on the structure inversion, numerical simulation, and geochemical research, we show at least two intervals of fluid transfer in Puguang paleo-oil reservoir, one in the forepart of late Indo-Chinese epoch to early Yanshan epoch and the other in the metaphase of early Yanshan epoch. Oil and gas accumulation occurred at Puguang structure through Puguang-Dongyuezhai faults and dolomite beds in reef and shoal facies in Changxing Formation (P2ch) - Feixianguan Formation (T1f) in the northwest and southwest directions along three main migration pathways, to form Puguang paleo-oil reservoir. Since crude oil is pyrolysised in the early stage of middle Yanshan epoch, Puguang gas reservoir has experienced fluid adjusting process controlled by tectonic movement and geochemical reconstruction process controlled by thermochemical sulfate reduction (TSR). Middle Yan-shan epoch is the main period during which the Puguang gas reservoir experienced the geochemical reaction of TSR. On one hand, TSR can recreate the fluid in gas reservoir, which makes the gas drying index larger and carbon isotope heavier. On the other hand, the reciprocity between fluid regarding TSR (hydrocarbon, H2S, and water) and reservoir rock induces erosion of the reservoir rocks and anhydrite alteration, which improves reservoir petrophysical properties. Superimposed by later tectonic movement, the fluid in Puguang reservoir has twice experienced adjustment, one in the late Yanshan epoch to the early Himalayan epoch and the other time in late Himalayan epoch, after which Puguang gas reservoir is finally developed.展开更多
文摘Natural gas containing hydrogen sulphide （H2S） has been found in several petroliferous basins in China, such as the Sichuan Basin, Bohai Bay Basin, Ordos Basin, Tarim Basin, etc. Natural gas with higher HES contents （HES 〉5 % mol.） is mostly distributed in both the gas reservoirs of Dukouhe, Luojiazhai, Puguang and Tieshanpo, which belong to the Triassic Feixianguan Formation in the northeastern Sichuan Basin and those of the Kongdian-Shahejie formations in the northeastern Jinxian Sag of the Jizhong Depression, Bohai Bay Basin. In the Sichuan Basin, the HES contents of natural gas average over 9% and some can be 17 %, while those of the Bohai Bay Basin range from 40 % to 92 %, being then one of the gas reservoirs with the highest H2S contents in the world. Based on detailed observation and sample analysis results of a total 5000 m of core from over 70 wells in the above-mentioned two basins, especially sulfur isotopic analysis of gypsum, brimstone, pyrite and natural gas, also with integrated study of the geochemical characteristics of hydrocarbons, it is thought that the natural gas with high HES contents resulted from thermochemical sulfate reduction （TSR） reactions. Among them, the natural gas in the Feixianguan Formation resulted from TSR reactions participated by hydrocarbon gas, while that in the Zhaolanzhuang of the Jinxian Sag being the product of TSR participated by crude oil. During the consumption process of hydrocarbons due to TSR, the heavy hydrocarbons were apt to react with sulfate, which accordingly resulted in the dry coefficient of natural gas increasing and the carbon isotopes becoming heavier.
基金the National Natural Science Foundation of China (Grant No. 40602016)the Project of CNPC Technology Innovation
文摘TSR is an interaction between sulfate and hydrocarbons, occurring widely in carbonate reservoirs. Because this process can produce a large amount of noxious acidic gases like H2S, it has drawn seri- ous concern recently. This paper reports an experiment that simulated an interaction between different minerals and hydrocarbon fluids under different temperature and time using a confined gold-tube system. The results showed that the main mineral that initiates TSR is MgSO4, and adding a certain amount of NaCl into the reactive system can also promote TSR and yield more H2S. The H2S produced in TSR is an important incentive for the continuous oxidative degradation of crude oils. For instance, the yield of oil-cracking gases affected by TSR was twice of that not affected by TSR while the yield of TSR-affected methane was even higher, up to three times of that unaffected by TSR. The carbon iso- topes of wet gases also became heavier. All of the above illustrated that TSR obviously motivates the oxidative degradation of crude oils, which makes the gaseous hydrocarbon generation sooner and increases the gas dryness as well. The study on this process is important for understanding the TSR mechanism and the mechanism of natural gas generation in marine strata.
基金Supported by the National Natural Science Foundation of China (Grant No. 40602016)the National Basic Research Project (Grant No. 2001CB209100)
文摘The Sinian Dengying Formation gas pool in Weiyuan is the oldest large-scale sulfur-bearing gas field in China, which has a H2S content ranging from 0.8% to 1.4%. The Cambrian Xixiangchi Formation gas pool discovered recently above the Dengying Formation contains gas geochemical behaviors similar to those of Dengying Formation but different in sulfur isotopes of H2S. Investigations show that though these two Sinian and Cambrian gas pools are separate ones, they share the same Cambrian source rock. The higher dry coefficient, heavier carbon isotopes, sulfur isotopes of sulfide, lower filling of gas pools, formation water characteristics, reservoir properties and H2S distribution, indicate that H2S in both the Sinian and Cambrian gas pools originates from TSR. The sulfur isotopes of sulfates have shown that H2S was formed in respective pools, namely hydrocarbons charged into the pools reacted with the Dengying Formation and the Xixiangchi Formation gypsum (TSR), respectively, to form H2S. Compared with sulfur isotopes of sulfates in each pool, δ34S values of H2S are 8‰ lighter for the Dengying Formation pool and 12‰ lighter for the Xixiangchi Formation pool, respectively, which is attributed to the difference in temperatures of TSR occurrence. The reservoir temperature of the Xixiangchi Formation pool is about 40℃ lower than that of the Dengying Formation pool. Temperature plays a controlling role in both the sulfur isotopic fractionation and amounts of H2S generation during TSR.
基金Supported by National Basic Research Program of China (Grant No. 2005CB422105)
文摘With the discoveries of a series of large gas fields in the northeast of Sichuan Basin, such as Puguang and Longgang gas fields, the formation mechanism of the gas reservoir containing high H2S in the ancient marine carbonate formation in superposition-basin becomes a hot topic in the field of petroleum geology. Based on the structure inversion, numerical simulation, and geochemical research, we show at least two intervals of fluid transfer in Puguang paleo-oil reservoir, one in the forepart of late Indo-Chinese epoch to early Yanshan epoch and the other in the metaphase of early Yanshan epoch. Oil and gas accumulation occurred at Puguang structure through Puguang-Dongyuezhai faults and dolomite beds in reef and shoal facies in Changxing Formation (P2ch) - Feixianguan Formation (T1f) in the northwest and southwest directions along three main migration pathways, to form Puguang paleo-oil reservoir. Since crude oil is pyrolysised in the early stage of middle Yanshan epoch, Puguang gas reservoir has experienced fluid adjusting process controlled by tectonic movement and geochemical reconstruction process controlled by thermochemical sulfate reduction (TSR). Middle Yan-shan epoch is the main period during which the Puguang gas reservoir experienced the geochemical reaction of TSR. On one hand, TSR can recreate the fluid in gas reservoir, which makes the gas drying index larger and carbon isotope heavier. On the other hand, the reciprocity between fluid regarding TSR (hydrocarbon, H2S, and water) and reservoir rock induces erosion of the reservoir rocks and anhydrite alteration, which improves reservoir petrophysical properties. Superimposed by later tectonic movement, the fluid in Puguang reservoir has twice experienced adjustment, one in the late Yanshan epoch to the early Himalayan epoch and the other time in late Himalayan epoch, after which Puguang gas reservoir is finally developed.
