Figure
1.
Homogeneous temperature histogram of saline inclusion in calcite from sample A7 (depth: 5 037 m, statistic number of inclusion: 20).
| Citation: | Guozhi Wang, Shugen Liu, Wenchao Su, Wei Sun, Dong Wang, Haifeng Yuan, Guosheng Xu, Can Zou. Water Soluble Gas in Deep Carbonate Reservoir, Sichuan Basin, Southwest China. Journal of Earth Science, 2008, 19(6): 636-644.
|
Based on temperature and pressure of fluid inclusion, phase of organic inclusion in calcite and quartz filled in vug in the deep carbonate reservoir and the natural gas composition in Weiyuan (威远) gas field in Sichuan (四川) basin, research indicates that water soluble gas exists in deep carbonate reservoir, which reconstructs development and effusion process of water soluble gas. The overpressure formed during oil thermal cracking can reach 105-170 MPa in Sinian and Cambrian reservoir in Central Sichuan and 78-86 MPa in Cambrian reservoir in Southeast Sichuan. The high temperature caused by deep burial and overpressure caused by thermal cracking make thermal cracking gas dissolve in water so that it becomes water soluble gas. The ratios of gas to water can reach 50-90 m3/m3 and 10-30 m3/m3, respectively, in deep carbonate reservoir in Central and Southeast Sichuan. Methane dissolving in water exists in form of liquid phase. Until now, the decreases in temperature and pressure due to the uplift during 74 Ma make water soluble gas separate from water, water soluble gas pool or mixed gas pool of thermal-cracking gas and water soluble gas are modified or even destroyed in varying degrees.This may be the case of Weiyuan gas field.
Water soluble gas, dissolving in formation water under certain conditions, is defined as natural gas mainly consisting of methane and some nonhydrocarbon gas such as CO2 and nitrogen. The total resource of water soluble gas around the world is about n× 1016–n×1018 m3, which is more than ten or even hundred times than that of conventional natural gas (Wu et al., 2003) and is a potential natural gas resource. It has been found in many oil-gas basins, such as some American basins along the Gulf of Mexico (Price, 1978; Jones, 1977), basins in North Caucasia in Ukraine (Zhang, 1995), Ya-1321 gas field in YingQiong basin (Chen et al., 1997), Tuha basin (Zhang et al., 2002), central gas fields in Ordos basin (Li et al., 2002), foreland basins in Kuche (Li et al., 2003), Kela 2 gas field in Tarim basin (Qin et al., 2007; Wang et al., 2004), and Hetianhe gas field (Qin et al., 2006). It has been found that comparative high temperature and overpressure benefit the formation of water soluble gas according to the research on the solution mechanism of water soluble gas (Fu et al., 1996) and factors affecting solubility (Liu et al., 2004; Hao and Zhang, 1993; Price, 1979; Bonham, 1978; Takenouchi and Kennedy, 1964; Culberson and McKetta, 1951) in recent years. Water soluble gas is often discriminated by heavy hydrocarbon coefficient, methane coefficient, butane coefficient, pentane coefficient, hydrocarbon/nitrogen ratio, and helium-argon ratio (Li et al., 2002; Zhang, 1995). The deeply buried underground and undergone high temperature and overpressure and the deep carbonate reservoirs in Sichuan basin have prepared the basis for the formation of deep water soluble gas. The available documents and materials show that water soluble gas in Sichuan basin is the probable mechanism of migration and accumulation (Wang et al., 1997). There are two different opinions on natural gas existing in water under the original gas-water interface in Weiyuan gas field; one being water soluble gas (Yang et al., 1993) and the other not so (He et al., 1983). On the basis of research on fluid inclusion in carbonate reservoirs of Cambrian and Sinian in Anping 1 well and Dingshan 1 well in Sichuan basin, this article tries to reveal the existence of water soluble gas in deep carbonate reservoirs.
Located in Southwest China, Sichuan basin is a coincidence basin and belongs to marine craton basin from Sinian to Middle Triassic. From Late Triassic, the basin nature and deposit environment have transformed from marine craton to continental deposit (Xu et al., 2004; Liu et al., 2003). Dengying Formation of Sinian and reservoirs of Cambrian, mainly consisting of dolomites having fissures and plentiful secondary solution porosity, are deeply buried underground today and only scattered outcrop appears in peripheral areas of the basin. Anping 1 well that is studied now is located in Caledonian paleohigh of Leshan-Longnüsi in Central Sichuan basin. Cambrian and Dengying Formation of Sinian were deeply buried to 4 480.48 m and 5 035.8 m underground, respectively. In geologic history, Dengying Formation of Sinian here was once deeply buried to 5 000–8 000 m underground (Wang et al., 1996). Dingshan 1 well is located in the west limb of NE-striking steep anticline belt along the southeast margin of Sichuan basin. The core of anticline is composed of Sinian and Cambrian, which is exposed on the surface. Once deeply buried to about 5 000–6 000 m, Cambrian and Sinian Dengying Formation in the west limb of anticline were deeply buried to 1 979 m and 3 485.59 m, respectively, today according to the analysis of apatite fission track. The unconformity between Permian and Silurian demonstrates that the spot where Dingshan 1 well is located was once a paleohigh during Devonian to Carboniferous.
Although the locations of Anping 1 well and Dingshan 1 well in the basin are different, it has been found that there exists similar mineral filling succession in vugs or fissures of dolomite reservoir through minute observation of core interval, from which mineral fillings of four generations can be clearly identified. They are grain dolomite of the first generation, coarse dolomite with clouded core and clean outer rim of the second, bitumen of the third, and calcite and/or quartz of the fourth. Dolomite of the first and second generations was mainly formed during deep burial. The organic geochemical analysis of bitumen of the third generation indicates that there exists plentiful diamantane, which shows that these bitumens were product of oil thermal cracking. Besides bitumen, natural gas was another important product of oil thermal cracking. Calcite and quartz of the fourth generation were formed after oil thermal cracking. The fluid inclusion preserved in calcite and quartz in carbonate reservoir records the state of natural gas formed during oil thermal cracking. Therefore, the samples used in this research are mainly calcite and quartz of the fourth generation.
Samples A7 and A48 were taken from fillings of vug or karst caves of 5 037 and 4 551.30 m in Anping 1 well, and the host rocks of them were dolomites of Sinian and Cambrian, respectively. Sample DS32 was taken from fissure fillings of 1 531.71–1 533.53 m in Dingshan 1 well, and the country rocks were dolomites of Cambrian.
The homogeneous temperature of fluid inclusion has been measured on Linkam Heating and Cooling Cell THMSG600, which can measure temperature from -196 to 600 ℃ with minimum temperature step size of 0.01 ℃; the velocity of heating and cooling of the apparatus is 0.01–130 ℃ /min. All Raman analyses of fluid inclusion are finished on Renishaw inVia spectrometer produced in Britain. The laser power is 40 mW at 514.5 nm; the spectrum slit is 10 µm and the speed of scanning is 6 times per 10 s. The analytical results of all samples would be mentioned afterwards.
It has been found that abundant saline inclusion with gas-liquid binary phase and organic inclusion exist in both calcite and quartz. Mostly being in the shape of ellipse, saline inclusion is about 5–10 µm big and organic inclusion is about 10–25 µm big.
The average homogeneous temperature of 20 saline inclusions from sample A7 in Anping 1 well ranges from 220 to 320 ℃, and most of them concentrate at 260 to 290 ℃ (Fig. 1). The contrast analysis of carbon, oxygen, and strontium isotope of calcite in samples A7 and A48 reveals that they are homologous synchronous fluid. According to triple point temperature of CO2, some average homogeneous temperature of methane and Raman composition of 105 CH4-CO2 organic inclusions in samples A7 and 92 CH4-CO2 or CH4 organic inclusions in sample A48, the minimum pressure value trapped by hydrocarbon inclusion in samples A7 and A48 under 220 and 320 ℃ has been imitantly calculated by using equation of SoaveRedlich-Kwong (Figs. 2, 3). The principles and methods of pressure capture can be found in detail in literature of Liu et al. (2007). The corresponding pressure peak values of sample A7 from Sinian under 220 and 320 ℃ range from 120 to 126 MPa and from 152 to 160 MPa, respectively (Fig. 2); the corresponding pressure peak values of sample A48 from Cambrian under 220 and 320 ℃ range from 105 to 135 MPa and from 135 to 170 MPa (Fig. 3). The corresponding minimum trap pressures of samples A7 and A48 under 260–290 ℃ are (120–126)–(152–160) MPa and (105–135)–(135–170) MPa, respectively. The paleo-pressure coefficients of samples A7 and A48 are 1.97–2.4 and 2.2–2.5, respectively.
The average homogeneous temperature of 38 saline inclusions of sample DS32 in Dingshan 1 well is between 170–195 ℃ (Fig. 4). According to triple point temperature of CO2, some average homogeneous temperatures of methane and Raman composition of 32 CH4-CO2 or CH4 organic inclusions in sample DS32, the minimum pressure value under 170 and 190 ℃ has been calculated to be 78–81 MPa and 84–86 MPa by using the similar way to A7 and A48 (Fig. 5). The paleo-pressure coefficient of sample DS32 is 1.78–1.83.
The temperature and pressure of fluid inclusion reveal that the fluid inclusion of Anping 1 well in Central Sichuan was formed under high temperature and high pressure and that of Dingshan 1 well in Southeast Sichuan under overpressure. Overpressure is the sharing feature of these fluid inclusions, which shows that calcite and/or quartz of the fourth generation was tion was formed under overpressure.
Research shows that higher temperature and pressure are good for formation of water soluble gas (Liu et al., 2004; Hao and Zhang, 1993; Price, 1979; Bonham, 1978; Takenouchi and Kennedy, 1964; Culberson and McKetta, 1951). The dissolving capacity of natural gas in water would increase as temperature increases when it is above 80 ℃, and the dissolving capacity would increase greatly as pressure increases. According to the experiment, Price (1979) imitantly established the relation between dissolving capacity of methane in water and temperature and pressure on the condition of high temperature and overpressure (Fig. 6). Based on the measured average temperature and the minimum fluid pressure, it could be sure that under 120–170 MPa and 260–290 ℃, about 50–90 m3 methane could be dissolved in every 1 m3 water in Anping 1 well (Fig. 6). Under high temperature and overpressure, the gas-water ratio of Sinian and Cambrian reservoir in Anping 1 well is higher than that of typical water soluble gas pool (27 m3/m3) under high temperature and pressure in the areas along Gulf of Mexico in USA and that of water soluble gas field under 4 000–5 000 m (19 m3/m3) in Kertch Peninsula in former Soviet Union (Yang et al., 1993). The gas-water ratio of Cambrian reservoir in Dingshan 1 well is quite similar to that of water soluble gas field in the areas along Gulf of Mexico and Kertch Peninsula.
Based on the analysis of Raman composition of 197 organic inclusions in samples A7 and A48 in Anping 1 well, it is revealed that the organic inclusion in sample A7 mainly consists of CH4 with little CO2 and some even contain H2S; whereas little CO2 exists in A48 simultaneously except single-phase CH4 inclusion. The composition of 32 organic inclusions in sample DS32 in Dingshan 1 well shows that some are singlephase CH4 and sometimes besides CH4, there exists little CO2 or H2S.
The statistic of Raman characteristic spectra of all organic inclusions indicates that characteristic spectra of CH4 concentrates on 2 910–2 914 cm-1. Research shows that gas and liquid phase CH4 have different values of characteristic spectra; whereas characteristic spectra values of liquid and gas phase CH4 are 2 909–2 915 cm-1 and 2 913–2 918 cm-1, respectively (Xu et al., 1996). The characteristic spectra of organic inclusion analyzed are similar to that of liquid phase CH4; it reveals that CH4 exists in form of liquid. Because some characteristic spectra of liquid and gas phase CH4 overlap partially, further cooling and heating experiment of inclusion is needed to confirm the phase of CH4 better. Organic inclusion appears to be homogeneous under the indoor temperature and bubbles come out when it is frozen. The bubbles become bigger and bigger from -104 to -194.6 ℃, and the part of liquid phase begins to freeze. The ice melts when it is heated to -188.6 ℃, and bubbles become very small at -103.6 ℃. Gas phase totally becomes single liquidphase inclusion homogeneously when it is heated to -93.3 ℃ (Fig. 7). The cooling and heating experiment of inclusion and characteristic spectra of Raman show together that methane always exists in form of liquid phase. Judging from this, when these organic inclusions were trapped, methane in reservoirs existed in water in form of liquid phase; namely, methane existed in saline fluid as water soluble gas.
Drilling suggests that Weiyuan gas field, located in the same paleohigh of Leshan-Longnüsi as Anping 1 well and mainly forming reservoirs of Dengying Formation, exists free natural gas within gas-bearing scope of gas pool and under the universal original gas-water interface (He et al., 1983). As for these natural gases, some regard them as water soluble gas (Yang et al., 1993) and others hold conflicting opinion (He et al., 1983).
Qin et al. (2006) proposed that such index as CO2/CH4, CH4/N2, N2/C2 H6, ln (C1/C2), and ln (C2/C3) could be used to reveal the migration path of water soluble gas. Due to different dissolving capacities of natural gas composition in water, these indexes would get higher as water soluble gas migrates theoretically. When natural gas in Weiyuan gas field is compared with typical water soluble gas of Hetianhe gas field in Tarim basin by using figure of CH4/N2-N2/C2 H6, it is not hard to discover that the gas of Weiyuan gas field, with higher CH4/N2 and N2/C2H6, is equivalent to the evolutionary ending of water soluble gas of Hetianhe gas field (Fig. 8), which suggests that the gas of Weiyuan gas field tends much to be water soluble gas than that of Hetianhe gas field. All these indicate that the free gas in Weiyuan gas field today may be classified into water soluble gas pool because of the separation of water soluble gas from water. The research mentioned above demonstrates that water soluble gas exists in all deep carbonate reservoirs of Anping 1 well, Weiyuan gas field in Central Sichuan, and Dingshan 1 well in Southeast Sichuan.
The analysis of Anping 1 well, Dingshan 1 well, and Weiyuan gas field above suggests that, existing in saline fluid as water soluble gas, methane of deep carbonate reservoirs is liquid-phase methane. Calcite and quartz analyzed were mainly formed after bitumen filling, which means that liquid-phase methane trapped by calcite and quartz was chiefly formed after oil thermal cracking. Through minute research on the vug fillings of core interval in Anping 1 well, Gaoke 1 well in Central Sichuan, and Dingshan 1 well in Southeast Sichuan and along with temperaturepressure of fluid inclusion and phase of organic inclusion, the development and effusion of water soluble gas in deep carbonate reservoirs could be rebuilt.
In process of deep burial, oil migrated and accumulated in carbonate reservoirs to form paleo-oil pools (Fig. 9a). As burial deepened and temperature increased, oil in paleo-oil pools began to crack to form thermal cracking gas and bitumen. These bitumens filled the edges of vug and the rest parts of vug were filled with thermal cracking gas (Fig. 9b). Research indicates that the thermal cracking of 1 t oil could produce gas of 550–720 m3 (Barker, 1990). The accommodation capacity of reservoir is almost constant, and the gas volume produced by oil thermal cracking is far bigger than oil volume; therefore, overpressure is certainly formed in reservoirs. Under high temperature and overpressure, a portion of thermal cracking gas dissolved in water to form water soluble gas, whose gas-water ratio could reach 10–30 m3/m3 and 50–90 m 3 /m3. The abrupt increase in pressure made the gas-water interface much lower than that of oil-water before oil thermal cracking and the majority of thermal cracking gas mainly filled in reservoir without water above the gas-water interface. The T-t thermohistory imitation of apatite fission track shows the tectonic shifted from the early constant sinking to rapid uplift since 74 Ma. The constant uplift of 74 Ma produced numerous fissures. The overpressure compartment formed in earlier time was destroyed, thermal cracking gas effused upward, and both pressure and temperature of fluid system dropped rapidly. Water soluble gas dissolved in water began to separate from water. Therefore, thermal cracking gas and water soluble gas mixed together to form mixed gas pools. At the same time, gas-water interface kept moving upward due to rapid depressurization (Fig. 9c). The pressure in compartment rapidly fell down as natural gas kept escaping along fissure. The constant separation of water soluble gas from water made the mixed gas in gas pools replaced by water soluble gas gradually. The saline fluid under gas-water interface migrated upward to the space, which was once occupied by water soluble gas or mixed gas of water soluble gas and thermal cracking gas, to precipitate and form calcite and quartz. The water soluble gas that still remained in water was preserved in form of fluid inclusion in calcite and/or quartz (Fig. 9d).
(1) There exists water soluble gas in deep carbonate reservoirs in Sichuan basin.
(2) The formation of water soluble gas is closely related to thermal cracking in paleo-oil pools. The overpressure produced during oil thermal cracking and high temperature produced during deep burial lead abundant thermal cracking gas to dissolve in water to form water soluble gas.
(3) Until now, the constant uplift, depressurization, and temperature falling from 74 Ma make water soluble gas separate from water and water soluble gas pool modified or destroyed in different degrees.
(4) Weiyuan gas field may be classified into water soluble gas pool due to uplift and separation of water soluble gas from water.
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Guozhi Wang, Shugen Liu, Wenchao Su, Wei Sun, Dong Wang, Haifeng Yuan, Guosheng Xu, Can Zou. Water Soluble Gas in Deep Carbonate Reservoir, Sichuan Basin, Southwest China. Journal of Earth Science, 2008, 19(6): 636-644.
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