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1.
The northeastern area of Sichuan Basin, southwestern China, is the area with the maximal reserve of natural gas containing higher hydrogen sulphide (H2S) that has been found among the petroliferous basins of China, with the proven and controlled gas reserve of more than 200 billion cubic meters. These gas pools, with higher H2S contents averaging 9%, some 17%, are mainly distributed on structural belts of Dukouhe, Tieshanpo, Luojiazhai, Puguang, etc., while the oolitic-shoal dolomite of the Triassic Feixianguan Fm. (T1f) is the reservoir. Although many scholars regard the plentiful accumulation of H2S within the deep carbonate reservoir as the result of Thermochemical Sulfate Reduction (TSR), however, the process of TSR as well as its residual geological and geochemical evidence is still not quite clear. Based on the carbon isotopic analysis of carbonate strata and secondary calcite, etc., together with the analysis of sulfur isotopes within H2S, sulphur, gypsum, iron pyrites, etc., as well as other aspects including the natural gas composition, carbon isotopes of hydrocarbons reservoir petrology, etc., it has been proved that the above natural gas is a product of TSR. The H2S, sulphur and calcite result from the participation of TSR reactions by hydrocarbon gas. During the process for hydrocarbons being consumed due to TSR, the carbons within the hydrocarbon gas participate in the reactions and finally are transferred into the secondary calcite, and become the carbon source of secondary calcite, consequently causing the carbon isotopes of the secondary calcite to be lower (−18.2‰). As for both the intermediate product of TSR, i.e. sulfur, and its final products, i.e. H2S and iron pyrites, their sulfur elements are all sourced from the sulfate within the Feixianguan Fm. During the fractional processes of sulfur isotopes, the bond energy leads to the 32S being released firstly, and the earlier it is released, the lower δ 34S values for the generated sulphide (H2S) or sulfur will be. However, for the anhydrite that participates in reactions, the higher the reaction degree, the more 32S is released, while the less 32S remains and the more δ 34S is increased. The testing results have proved the process of the dynamic fractionation of sulfur isotopes.  相似文献   

2.
Fluid inclusions as captured in homogeneous fluids in rocks and minerals have been extensively studied and successfully applied to exploring the metalloge- netic temperature and pressure of metallic ore deposits and in investigating hydrocarbon generation, migra- tion, etc.[1―6]. In regard to multiple forms of immis- cible inclusions in rocks and minerals, a significant amount of research has already been conducted toward the immiscible inclusions and “boiling” inclusions in CO2-H2O system…  相似文献   

3.
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.  相似文献   

4.
The mechanism of hydrogen sulfide (H2S) generation plays a key role in the exploration and development of marine high-sulfur natural gas, of which the major targets are the composition and isotope characteristics of sulfur-containing compounds. Hydrocarbon source rocks, reservoir rocks, natural gases and water-soluble gases from Sichuan Basin have been analyzed with an online method for the content of H2S and isotopic composition of different sulfur-containing compounds. The results of comparative analysis show that the sulfur-containing compounds in the source rocks are mainly formed by bacterial sulfate reduction (BSR), and the sulfur compounds in natural gas, water and reservoir are mainly formed by thermal sulfate reduction (TSR). Moreover, it has been shown that the isotopically reversion for methane and ethane in high sulfur content gas is caused by TSR. The sulfur isotopic composition of H2S in natural gas is inherited from the gypsum or brine of the same or adjacent layer, indicating that the generation and accumulation of H2S have the characteristics of either a self-generated source or a near-source.  相似文献   

5.
Based on results of microscopic observation and laser Raman analysis about fluid inclusions, multiple special forms of immiscible inclusions that contain sulphur, liquid hydrocarbon, bitumen, etc. were discovered in samples collected from the H2S gas reservoir-containing carbonates in the Lower Triassic Feixianguan Formation in the Jinzhu-Luojia area, Kai County, Sichuan Province. Based on the lithology and burial history of the strata involved as well as measurement results of homogenization temperature of fluid inclusions, bitumen reflectivity, etc., it is concluded that the H2S in the gas reservoir resulted from the thermal reaction between hydrocarbons in reservoir and CaSO4 in the gypsum-bearing dolostone section at the high temperature (140°C–17°C) oil-cracked gas formation stage in Late Cretaceous. Thereafter, research on a great number of immiscible inclusions in the reservoir reveals that elemental sulphur resulted from oxidation of part of the earlier-formed H2S and further reaction between sulphates, hydrocarbons and H2S in geological fluids in H2S-bearing gas reservoir at a temperature of 86°C–89°C and a pressure of 340×105Pa and during the regional uplift stage as characterized by temperature decrease and pressure decrease in Tertiary. Meanwhile, gypsum, anhydrite and calcite formed at this stage would trap particles like elemental sulphur and result in a variety of special forms of immiscible inclusions, and these inclusions would contain information concerning the complexity of the fluids in the reservoir and the origin of H2S and natural sulphur in the gas reservoir.  相似文献   

6.
The continent is the second largest carbon sink on Earth’s surface.With the diversification of vascular land plants in the late Paleozoic,terrestrial organic carbon burial is represented by massive coal formation,while the development of soil profiles would account for both organic and inorganic carbon burial.As compared with soil organic carbon,inorganic carbon burial,collectively known as the soil carbonate,would have a greater impact on the long-term carbon cycle.Soil carbonate would have multiple carbon sources,including dissolution of host calcareous rocks,dissolved inorganic carbon from freshwater,and oxidation of organic matter,but the host calcareous rock dissolution would not cause atmospheric CO2drawdown.Thus,to evaluate the potential effect of soil carbonate formation on the atmospheric p CO2level,different carbon sources of soil carbonate should be quantitatively differentiated.In this study,we analyzed the carbon and magnesium isotopes of pedogenic calcite veins developed in a heavily weathered outcrop,consisting of limestone of the early Paleogene Guanzhuang Group in North China.Based on the C and Mg isotope data,we developed a numerical model to quantify the carbon source of calcite veins.The modeling results indicate that4–37 wt%of carbon in these calcite veins was derived from atmospheric CO2.The low contribution from atmospheric CO2might be attributed to the host limestone that might have diluted the atmospheric CO2sink.Nevertheless,taking this value into consideration,it is estimated that soil carbonate formation would lower 1 ppm atmospheric CO2within 2000 years,i.e.,soil carbonate alone would sequester all atmospheric CO2within 1 million years.Finally,our study suggests the C–Mg isotope system might be a better tool in quantifying the carbon source of soil carbonate.  相似文献   

7.
Temperature-programmed simulation experiments of saturated hydrocarbons with calcium sulfate and element sulfur were compared in this study. Based on the variation analysis of the yields and evolvement features of gaseous hydrocarbon (C1-C5) and inorganic gaseous CO2, H2 and H2S, the reaction mechanisms were analyzed and discussed. In the calcium sulfate-saturated hydrocarbon system, H2S was produced by a small quantity, which indicates this reaction belongs to the low-degreed thermal sulfate reduction (TSR...  相似文献   

8.
Multiple sulfur and oxygen isotope compositions in Beijing aerosol   总被引：1，自引：0，他引：1  
Multiple sulfur isotopes(32S, 33 S, 34 S, 36S) and oxygen isotopes(16O, 18O) in Beijing aerosols were measured with MAT-253 isotope mass spectrometer. The δ34S values of Beijing aerosol samples range from 1.68‰ to 12.57‰ with an average value of 5.86‰, indicating that the major sulfur source is from direct emission during coal combustion. The δ18O values vary from 5.29‰ to 9.02‰ with an average value of 5.17‰, revealing that the sulfate in Beijing aerosols is mainly composed of the secondary sulfate. The main heterogeneous oxidation of SO2 in atmosphere is related to H2O2 in July and August, whereas H2O2 oxidation and Fe3+ catalytic oxidation with SO2 exist simultaneously in September and October. Remarkable sulfur isotope mass-independent fractionation effect is found in Beijing aerosols, which is commonly attributed to the photochemical oxidation of SO2 in the stratosphere. In addition, thermochemical reactions of sulfur-bearing compounds might be also a source of sulfur isotope anomalies based on the correlation between ?33S and CAPE.  相似文献   

9.
The composition of fluid inclusions(FI)often represents the initial geochemical characteristics of palaeo-fluid in reservoir rock.Influence on composition and carbon isotopic composition of gas during primary migration,reservoir-forming and subsequent secondary alterations are discussed through comparing fluid inclusion gas with coal-formed gas and natural gas in present gas reservoirs in the Ordos Basin.The results show that primary migration of gas has significant effect on the molecular but not on the carbon isotopic composition of methane.Migration and diffusion fractionation took place during the secondary migration of gas in Upper Paleozoic gas reservoir according to carbon isotopic composition of methane in FIs.Composition and carbon isotopic composition of natural gas were nearly unchanged after the gas reservoir forming through comparing the FI gases with the natural gas in present gas reservoir.  相似文献   

10.
The components and carbon isotope of gases in inclusions are one of the most important geochemical indexes for gas pools.The analysis results of the components and carbon isotope of gases from inclusions in reservoir layers of Upper Palaeozoic gas pools in the Ordos Basin show that most inclusions grown in reservoir sandstone are primary inclusions.There is only a little difference about the components and carbon isotope between the well gases and the secondary inclusions gases.This indicated that the epigenetic change of gas pools is little.This difference between the well gases and the secondary inclusions gases is caused by two reasons:(i)The well gases come from several disconnected sand bodies buried in a segment of depth,while the inclusion gases come from a point of depth.(ii)The secondary inclusions trapped the gases generated in the former stage of source rock gas generation,and the well gases are the mixed gases generated in all the stages.It is irresponsible to reconstruct the palaeo-temperature and palaeo-pressure under which the gas pool formed using carbon dioxide inclusions.  相似文献   

11.
This study is undertaken to understand how calcite precipitation and dissolution contributes to depth-related changes in porosity and permeability of gas-bearing sandstone reservoirs in the Kela 2 gas field of the Tarim Basin, Northwestern China. Sandstone samples and pore water samples are col-lected from well KL201 in the Tarim Basin. Vertical profiles of porosity, permeability, pore water chem-istry, and the relative volume abundance of calcite/dolomite are constructed from 3600 to 4000 m below the ground surface within major oil and gas reservoir rocks. Porosity and permeability values are in-versely correlated with the calcite abundance, indicating that calcite dissolution and precipitation may be controlling porosity and permeability of the reservoir rocks. Pore water chemistry exhibits a sys-tematic variation from the Na2SO4 type at the shallow depth (3600-3630 m), to the NaHCO3 type at the intermediate depth (3630―3695 m),and to the CaCl2 type at the greater depth (3728―3938 m). The geochemical factors that control the calcite solubility include pH, temperature, pressure, Ca2 concen-tration, the total inorganic carbon concentration (ΣCO2), and the type of pore water. Thermodynamic phase equilibrium and mass conservation laws are applied to calculate the calcite saturation state as a function of a few key parameters. The model calculation illustrates that the calcite solubility is strongly dependent on the chemical composition of pore water, mainly the concentration difference between the total dissolved inorganic carbon and dissolved calcium concentration (i.e., [ΣCO2] -[Ca2 ]). In the Na2SO4 water at the shallow depth, this index is close to 0, pore water is near the calcite solubility. Calcite does not dissolve or precipitate in significant quantities. In the NaHCO3 water at the intermedi-ate depth, this index is greater than 0, and pore water is supersaturated with respect to calcite. Massive calcite precipitation was observed at this depth interval and this intensive cementation is responsible for decreased porosity and permeability. In the CaCl2 water at the greater depth, pore water is un-der-saturated with respect to calcite, resulting in dissolution of calcite cements, as consistent with microscopic dissolution features of the samples from this depth interval. Calcite dissolution results in formation of high secondary porosity and permeability, and is responsible for the superior quality of the reservoir rocks at this depth interval. These results illustrate the importance of pore water chemis-try in controlling carbonate precipitation/dissolution, which in turn controls porosity and permeability of oil and gas reservoir rocks in major sedimentary basins.  相似文献   

12.
A type of authigenic pyrites that fully fill or semi-fill the rock fractures of drillholes with gas hydrate anomalies are found in the Qilian Mountain permafrost; this type of pyrite is known as “fracture-filling” pyrite. The occurrence of “fracture-filling” pyrite has a certain similarity with that of the hydrate found in this region, and the pyrite is generally concentrated in the lower part of the hydrate layer or the hydrate anomaly layer. The morphology, trace elements, rare earth elements, and sulfur isotope analyses of samples from drillhole DK-6 indicate that the “fracture-filling” pyrites are dominated by cubic ones mainly aligned in a step-like fashion along the surfaces of rock fractures and are associated with a circular structure, lower Co/Ni and Sr/Ba, lower ΣREE, higher LREE, significant Eu negative anomalies, and Δ34SCDT positive bias. In terms of the pyrites’ unique crystal morphology and geochemical characteristics and their relationship with the hydrate layers or abnormal layers, they are closely related with the accumulation system of the gas hydrate in the Qilian Mountain permafrost. As climate change is an important factor in affecting the stability of the gas hydrate, formation of fracture-filling pyrites is most likely closely related to the secondary change of the metastable gas hydrate under the regional climate warming. The distribution intensity of these pyrites indicates that when the gas hydrate stability zone (GHSZ) is narrowing, the hydrate decomposition at the bottom of the GHSZ is stronger than that at the top of the GHSZ, whereas the hydrate decomposition within the GHSZ is relatively weak. Thus, the zone between the shallowest and the deepest distribution of the fracture-filling pyrite recorded the largest possible original GHSZ.  相似文献   

13.
Hetianhe gasfield in Bachu region of the Tarim Basin is mainly composed of three reservoir-caprock assembly,namely regional caprock of upper mudstone,middle mudstone and lower mudstone of the Carboniferous and reservoir of Bachu bioclastic limestone,glutenite and the Ordovician carbonate buried hill.Natural gas in Hetianhe gasfield sourced from the Cambrian source rock.It is thought that gases in Ma4 well block in the east of Hetianhe gasfield are mainly crude-oil cracked gases,while those in Ma3 and Ma8 well blocks in the west are the mixture gases of kerogen cracked gases and crude-oil cracked gases.Natural gas is rich in H2S and accumulated in multiply stages as the result of TSR.The accumulation history is divided into three stages,namely accumulation and breakage in the late Caledonian-early Hercynian,migration and dissipation in the late Hercynian and accumulation in Himalayan. The main accumulation of reformed gas reservoir is in Himalayan.  相似文献   

14.
Shallow gas reservoirs are distributed widely in Chinese heavy oil-bearing basins.At present,shallow gas resources have opened up giant potentials.The previous researches indicate the intimate genetic relationship between shallow gas and heavy oil.Shallow gas resources are generated from crude oil degraded by anaerobic microscopic organism,it belongs to biogenic gas family of secondary genesis, namely heavy oil degraded gas.Shallow gas resources are usually distributed in the upward position or the vicinity of heavy oil reservoirs.They are mainly of dry gas,which are composed of methane and only tiny C2 heavy hydrocarbon and relatively higher contents of nitrogen gas.Generally,methane isotopes are light,whose values are between biogenic gas and thermal cracking gas.Ethane isotopes are heavy,which mixed possibly with thermogenic gas.Carbon dioxide bear the characteristics of very heavy carbon isotope,so carbon isotopic fractionation effects are very obvious on the process of microscopic organism degradation crude oil.The heavy oil degraded gas formation,a very complex geological,geochemical and microbiological geochemical process,is the result of a series of reactions of organic matter-microbes and water-hydrocarbon,which is controlled by many factors.  相似文献   

15.
Gaseous components of gas inclusions in deep carbonate rocks (>5700 m) from the Tacan 1 well were analyzed by online mass spectrometry by means of either the stepwise heating technique or vacuum electromagnetism crushing. The carbon isotopic compositions of gases released by vacuum electromagnetism crushing were also measured. Although the molecular compositions of gas inclusions show differences between the two methods, the overall characteristics are that gas inclusions mainly contain CO2, whilst hydrocarbon gases, such as CH4, C2H6 and C3H8, are less abundant. The content of CO is higher in the stepwise heating experiment than that in the method of vacuum electromagnetism crushing, and there are only minor amounts of N2, H2 and O2 in gas inclusions. Methane δ13C values of gas inclusions in Lower Ordovician and Upper Cambrian rocks (from 5713.7 to 6422 m; -52‰-63‰) are similar to those of bacterial methane, but their chemical compositions do not exhibit the dry character in comparison with biogenic gases. These characteristics of deep gas inclusions may be related to the migration fractionation. Some deep natural gases with light carbon isotopic characteristics in the Tazhong Uplift may have a similar origin. The δ13C1 values of gas inclusions in Lower Cambrian rocks (7117-7124 m) are heavier (-39‰), consistent with highly mature natural gases. Carbon isotopic compositions of CO2 in the gas inclusions of deep carbonate rocks are similar (from -4‰ to -13‰) to those of deep natural gases, indicating predominantly an inorganic origin.  相似文献   

16.
Routine GC/MS analysis may apply to the volatilized Low-Molecular-Weight compounds in saturate and aromatic hydrocarbon fractions;thus,relative studies using this technique inevitably bring about some limitations on distribution of miscellaneous sulfur atom.In this article,Fourier Transform Ion Cyclotron Resonance Mass Spectrometry(FT-ICR MS)with high resolution is employed to investigate the distribution of organic sulfur compounds(OSCs)in the crude oil typically derived from the Eogene carbonate-evaporite sediments with further chemical compositional characterization in molecular level by miscellaneous atomic type,carbon number,and double bond equivalent(DBE).A variety of miscellaneous atomic types with S1,S2,S3,OS,OS2,O2S,O2S2,NS,and NOS etc.(S1 means those OSCs with one sulfur atom in a molecule)were identified in OSCs in these oil samples.High levels of alkyl thioether series compounds with one ring structure were presented mainly in the crude oil in the Jianghan Basin whereas high amounts of benzothiophene,dibenzothiophene etc.compounds with higher values in DBE and carbon number range occurred in the sulfur-rich heavy oil in the Jinxian Sag.Although carbonate-evaporite sediments deposited in the saline lacustrine facies in the Eogene basin both occurred in the Jinxian Sag and Jianghan Basin,obviously,they possess different chemical diagenetic pathway of sulfur under various microbial reactions,leading to diverse distributional characteristics on biomarkers,OSCs,and even different hydrocarbon generation mechanism of immature crude oil.  相似文献   

17.
Since the Meso-Cenozoic, controlled by paleoclimate, a series of fresh to brackish water basins and salt to semi-salt water basins were developed in wet climatic zones and in dry climate zones in China, respectively[1]. The geological and geochemical char…  相似文献   

18.

The composition of fluid inclusions (FI) often represents the initial geochemical characteristics of palaeo-fluid in reservoir rock. Influence on composition and carbon isotopic composition of gas during primary migration, reservoir-forming and subsequent secondary alterations are discussed through comparing fluid inclusion gas with coal-formed gas and natural gas in present gas reservoirs in the Ordos Basin. The results show that primary migration of gas has significant effect on the molecular but not on the carbon isotopic composition of methane. Migration and diffusion fractionation took place during the secondary migration of gas in Upper Paleozoic gas reservoir according to carbon isotopic composition of methane in Fls. Composition and carbon isotopic composition of natural gas were nearly unchanged after the gas reservoir forming through comparing the FI gases with the natural gas in present gas reservoir.

  相似文献   

19.
The fault-controlled Nibao Carlin-type gold deposit,together with the strata-bound Shuiyindong deposit,comprise a significant amount of the disseminated gold deposits in southwestern Guizhou Province,China.Five main types and two sub-types of pyrite at the Nibao deposit(Py1a/Py1b,Py2,Py3,Py4,Py5)were distinguished based on detailed mineralogical work.Py1,Py2and Py3 are Au-poor,whereas Py4 and Py5 are Au-rich,corresponding to a sedimentary and hydrothermal origin,respectively.Through systematic in situ analyses of NanoSIMS sulfur isotopes,the framboid pyrite Py1a with negative δ^34S values(-53.3 to-14.9%)from the Nibao deposit were found to originate from bacterial sulfate reduction(BSR)processes in an open and sulfate-sufficient condition while the superheavy pyrite Py1b(73.7–114.8%)is probably due to the potential influence of closed-system Rayleigh fractionation or the lack of preservation of deepsea sediments.Data of Py2 and Py3 plot within the area of S isotope compositions from biogenic and abiogenic sulfate reduction.In view of few coeval magmatic rocks in the mining district,the near zero δ^34S values of the Au-rich pyrites(Py4 and Py5)may discount the potential involvement of magmatic but metamorphic or sedimentary origin.LA-ICP-MS and TEM work show that Au in ore-related pyrite is present as both nanoparticles and structurally bound.LA-ICP-MS analyses show that the Au-rich pyrite also contains higher As,Cu,Sb,Tl and S than other types of pyrite,which inferred a distal manifestation of deep hydrothermal mineralization systems.  相似文献   

20.
Shallow gas reservoirs are distributed widely in Chinese heavy oil-bearing basins. At present, shallow gas resources have opened up giant potentials. The previous researches indicate the intimate genetic relationship between shallow gas and heavy oil. Shallow gas resources are generated from crude oil degraded by anaerobic microscopic organism, it belongs to biogenic gas family of secondary genesis, namely heavy oil degraded gas. Shallow gas resources are usually distributed in the upward position or the vicinity of heavy oil reservoirs. They are mainly of dry gas, which are composed of methane and only tiny C 2 + heavy hydrocarbon and relatively higher contents of nitrogen gas. Generally, methane isotopes are light, whose values are between biogenic gas and thermal cracking gas. Ethane isotopes are heavy, which mixed possibly with thermogenic gas. Carbon dioxide bear the characteristics of very heavy carbon isotope, so carbon isotopic fractionation effects are very obvious on the process of microscopic organism degradation crude oil. The heavy oil degraded gas formation, a very complex geological, geochemical and microbiological geochemical process, is the result of a series of reactions of organic matter-microbes and water-hydrocarbon, which is controlled by many factors.  相似文献   

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