
Citation: | Haifeng YUAN, Guosheng XU, Shugen LIU, Guozhi WANG. Paleo-temperature Evolution and Water Soluble Gas in Sinian Reservoir, Anpingdian-Gaoshiti Structural Zone, Central Sichuan Basin. Journal of Earth Science, 2008, 19(6): 707-714. |
The paleo-temperature evolution of Sinian reservoir of Anping (安平) 1 well was rebuilt by taking the method of apatite fission track and Easy%Ro model. The result of apatite fission track determines the accurate burial history and overcomes the flaw that the vitrinite reflectance is taken as paleo-temperature indicator simply. The authors used the laser Raman technique to analyze the meth- ane present in the calcite and quartz fluid inclusions of Sinian reservoir,finding that the methane is water soluble gas. The authors also simulated the paleo-pressure of fluid inclusion by using PVTsim software and finally worked out the methane solubility in water.
The exploration history for hydrocarbon of Sinian has gone through more than 40 years, in Sichuan basin, and the amount of wellbore drilling to Sinian was added up to more than 40. The Weiyuan gas field, Ziyang gas pool, Longnüsi, and Gaoshiti-Anpingdian gas-bearing structures had been discovered. The hydrocarbon levels and the condition of hydrocarbon accumulation from the discovered gas fields show that the Sinian reservoir should have a bright future for oil and gas exploration in Sichuan basin (Xu et al., 2007;Yao et al., 2003). In the 1990s, a breakthrough of Sinian reservoir was achieved in the Anpingdian-Gaoshiti structural zone, Central Sichuan basin. For example, the gas production from drilling stem test (DST) in Sinian reservoir of Anping 1 well is approximately 0.248×104 m3/d, and the gas production of Gaoke 1well is 0.7×104 m3/d in the same structure. But it is a pity that no other great breakthroughs were acquired in the area. In this article, the authors mainly discussed the paleo-temperature evolution and the formation of water soluble gas in Sinian resrvoir, Anpingdian-Gaoshiti structure, for the purpose of giving some advice for the further exploration.
The research of thermal history in sedimentary basin is an important part of basin analysis and related to hydrocarbon generation, migration, and accumulation. The thermal history in basin can provide the geothermal field for the subsequent hydrocarbon generation history, hydrocarbon explusion history, and hydrocarbon accumulation history (Karsten et al., 2008;Qiu et al., 2004;di Primio, 2002). The pre-condition for reconstructing thermal history is to get accurate burial history of sedimentary basins.
The research method about geothermal history falls into two categories: (1) thermal history simulation by using all kinds of paleo-temperature scale, which mainly includes maturity indicator of organic matter, fluid inclusion, apatite fission track, etc., (2) using geophysical model of basin evolution. At present, used as paleo-temperature indicator, vitrinite reflectance and apatite fission track (AFT) have become a widely used tool in rebuilding thermal history of sedimentary basins. These two kinds of methods can be complementary in rebuilding thermal history (Qiu, 2004). The article reconstructs the paleo-temperature of Anpingdian-Gaoshiti structure zone just through applying the paleo-temperature indicator of vitrinite reflectance and apatite fission track.
Vitrinite reflectance (Ro) is currently a popular technique and one of the most effective methods to calibrate thermal history. There are some models of calibrating paleo-temperature by using vitrinite reflectance, which is proposed by previous works, and these models were improved with in-depth research. At the early stage, scholars merely established some empirical equations or graphical methods based on the relationship between vitrinite reflectance and burial depth for the sake of calibrating thermal history or paleo-temperature (Qiu et al., 2004). At present, the prevalent models, which are applied to thermal history reconstruction of the sedimentary basin, mainly include TTI (time-temperature index), the Lerche fitting model and the Easy%Ro model (Sweeney and Burnham, 1990), and the chemical kinetics model Easy%Ro is widely used to compare with these models. The Easy%Ro model is adopted to the values of vitrinite reflectance from 0.2%–4.7%, and especially, suites to middle-high thermal evolution level.
However, the values of vitrinite reflectance measured are controlled by the temperature history during the sedimentary process of vitrinite, and the temperature history is closed to burial history and geothermal gradient of the strata. Given that we make certain the burial history of vitrinite in strata, the values of vitrinite are only controlled by geothermal gradient of sedimentary basins. Unfortunately, the values of vitrinite reflectance possibly evolve into the same, because of the almost similar highest temperature experienced, despite the fact that the vitrinite ever experienced different thermal history paths. Therefore, the key to the reconstruction of paleo-temperature is how to obtain accurate burial history.
The technique of apatite fission track (AFT) is mainly used to study the thermal history and the age of the host rock at the lower temperature (< 125℃) (Green et al., 1989a;Gleadow et al., 1986;Naeser, 1979;Wanger, 1968). AFT analysis is widely used in oil and gas exploration because of the characteristic by which the technique can reconstruct thermal history well and truly, and the AFT nealing zone approaches oil window, and apatite is distributed extensively in sedimentary rocks.
Walker (1965) proposed fission-track dating based on fission-track counting of spontaneous fission and age dating of minerals. In early 1970s, scholars found the feature of fission-track annealing. Therefore, the theories and methods mentioned above open a new area for the application of fission track to geoscience, which is the reconstruction of paleo-temperature and thermal history. The research workers conceived annealing kinetics model of fission track (Ketcham, 2000, 1999;Green et al., 1989b, 1986;Duddy et al., 1988;Laslett et al., 1987) based upon experimental studies (Ketchman, 2000;Crowley et al., 1991;Laslett et al., 1987) and borehole observations (Naeser and McCullon, 1989;Gleadow and Duddy, 1981). The annealing models lead to fission-track thermochronology, which was suitable only for dating and later, it evolved into the technique of analyzing maturity and thermal history. The apatite, zircon, and sphene are often used for fission-track analysis. Since 1980s, fission-track had been widely applied to geothermal history through in-depth study of the fission track annealing law (Arne et al., 1990;Green et al., 1989a;Duddy et al., 1984;Gleadow et al., 1983).
The density and the length of fission-track are the two important parameters in the annealing kinetics models. The scholars can simulate track length distribution under the supposed geothermal field by carrying out a series of laboratory annealing experiments and annealing equations (Gleadow and Brown, 2000;Green et al., 1989b;Duddy et al., 1988). Gleadow and Brown (2000)gave three hypothetical temperaturehistory paths, and all the three paths assumed that geo-temperature dropped from 120℃ to the low temperature. The simulated results of track length distribution for these three temperature-history paths show that different temperature-history paths produced different track length distribution although they never underwent the same highest temperature. Therefore, AFT can illuminate the processes of thermal evolution, and the complicated history suffered during subsidence and upliftment of sedimentary basins. Thus, it can be seen that vitrinite reflectance itself sometimes can't truly reflect thermal history of sedimentary basin, especially in the case of complicated structural evolution basin. But AFT can resolve the problem better which vitrinite reflectance encountered, and the results of AFT can provide the accurate burial history for Easy%Ro chemical kinetics model.
The samples from Anping 1 well at the Anpingdian-Gaoshiti structural zone could not detect any apatite particle, which can be measured, and so, the authors took two samples from Moxi structure located at the contiguity to the Anpingdian-Gaoshiti structural zone for measurement. The weight of the two sandstone samples is approximately 1.5 kg, and the apatite analysis was finished at the Institute of High Energy Physics, Chinese Academy of Sciences, and the parameters such as track age and track density are obtained. The thermal history simulation mainly uses the AFT ages and track length based on laboratory annealing experiments. The simulation methods fall into two categories—one is forward model, and the other is inverse model. Calculation of the forward model requires inputing a possible time-temperature path, and then the model can produce an estimated fissiontrack age and length distribution, and so we can compare the speculated with observed AFT results, and finally get the best time-temperature path. The inverse model constructs unknown t-T path based on observed AFT data, and searches among the various permissible t-T paths for the best-fitting solutions between model predictions based on each t-T path generated and the measured data. Relatively, the inverse model is more important than the forward model in the actual application. The article mainly uses the AFT solve program (Ketcham, 2000) to simulate the thermal history of the study region.
When the samples were taken to surface from borehole, the temperature dropped from subsurface temperature to surface temperature. So, we can suppose that the average temperature is approximately 20℃ during simulating. The t-T paths and track length distribution of sample M24-2 simulated (Fig. 1) show that the temperature is 116.04℃ at approximately 59Ma, and the burial depth is approximately 3 694 m assuming that geothermal gradient is 26℃/km, and the surface temperature is 20℃. At 18 Ma, the temperature of sample is 101.0℃, and the burial depth is approximately 3 115 m. After this, the strata enter into slowly uplifted stage. The current burial depth of this sample is 2 239.0 m, and the temperature of place taking sample is 84.9℃. So, we can calculate that the denudation thickness is approximately 1 455 m because the strata begin to uplift at 59 Ma. The sample M58 represents the similar characteristic to the sample M24-2, and the denudation thickness of M58 well is approximately 1 551 m since 59 Ma. Obviously, the results of AFT not only give the thermal history of sample but also the subsidence and uplift process of these wells. Then, the determined accurate burial history can be provided for the Easy%Ro model, which is used to calculate the paleo-temperature and geothermal gradient.
The maximum burial depth in the sedimentary process can be computed by using the backstripping and compaction correction (Guidish et al., 1985;Ungerer et al., 1984), and the denudation thickness because uplift has been determined from AFT modeling. Then, we can use the vitrinite reflectance measured as the thermal maturity indicator and calculate the paleo-temperature and geothermal gradient of Anping 1 well with Easy%Ro model, and the result shows that there is a better fit between calculated Ro and measured Ro (Fig. 2, Table 1). The mud shale of Qiongzhusi Formation in Lower Cambrian is close to Sinian reservoir because the mud shale is main source rock of Sinian reservoir (Xu et al., 2007). Their paleo-temperature of Lower Cambrian and Sinian increases with increasing burial depth, but the change of the paleo-geothermal gradient has a difference (Table 1). There are mainly two reasons: (1) the heat flow was variable during different geological histories, (2) the thermal conductivity of rock is different because of sedimentary campaction and bearing-fluid. The paleo-temperature of mud shale evolves from 41.88℃/km at 550 Ma to 32.29℃/km at present, and the main process decreases, increases, and decreases. The paleo-temperature evolution is similar to that of Lower Cambrian, and the paleo-geothermal gradient changes from 25℃/km at 600 Ma to 29.33℃/km, which, in the case of Sinian, is higher than that of Lower Cambrian overall.
![]() |
The water soluble gas means that the principal gas component dissolved in groundwater is methane, and it is an important unconventional gas. Theoretically speaking, the distribution of dissolved gas resources is more extensive than conventional gas, and the potential reserve is more than the discovered gas reserves.Based on volumetric and analogy method, the resource volume dissolved is approximately 12×1012–65×1012 m3, which is greater than predicted conventional gas volume in sedimentary basins in China. The solubility of natural gas in water depends on a variety of factors.Temperature (T), pressure (P), and salinity as well as gas components are the important known factors. The influence of temperature on solubility demonstrates that the methane solubility decreases with increasing temperature under 80℃, and the solubility increases with increasing temperature above 80℃. The solubility of methane increases with increasing pressure and decreases with increasing salinity for a constant temperature.Among all the four factors mentioned above, pressure is the most important. Therefore, the distribution of water soluble gas pools is relevant to high pressure and abnormal overpressure (Chen et al., 2006;Yang et al., 1993).
The previously simulated paleo-temperature shows that the condition of temperature can form the water soluble gas in the Sinian reservoir.And the pressure effect because of the phase change of hydrocarbon with increase in temperature, such as oil cracking to gas, can cause the formation of water soluble gas.
The authors discovered that all the organic fluid inclusions of Sinian reservoir of Anping 1 well, which is captured in the quartz or calcite of the latest period, is dissolved methane.That is to say, the methane takes on dissolved state and exists in the brine water. The homogenization temperature of coeval aqueous inclusion with organic inclusions ranges from 220 to 320℃, and the peak temperature is between 260 and 290℃.Compared with the simulated paleogeotemperature of Anping 1 well, we can find that the homogenization temperature is obviously higher than simulated paleo-geotemperature background. These indicated that hydrothermal fluid ever acted in Sinian reservoir.At the same time, the thin section observation and the Sr, C, O isotope analyses show that deep hydrothermal fluid action was present in Sinian reservoir. The P-T isochore calculated with PVTsim software (Aplin et al., 1999) shows that the peak value range of pore fluid pressure is from 1.2×108 Pa to 1.26×108 Pa under the conditions of 220℃, and the range of pore fluid pressure is from 1.52×108 Pa to 1.6×108 Pa at 320℃.Namely, the fluid pressure obtained from inclusions is between 1.2×108 Pa and 1.6×108 Pa when the peak temperature ranges from 260 to 290℃. The corresponding pressure coefficient calculated is between 1.84–2.4 according to the paleoburial depth of the sample, which shows that the pore fluid pressure is overpressure at that time.Between 260 and 290℃, oil in the Sinian reservoir almost has cracked to gas completely, and the volume expansion during oil cracking to gas is the dominant factor that causes abnormal overpressure. The result that paleotemperature model for Sinian as well as the measured temperature and the simulated pressure of fluid inclusion gave shows that Sinian reservoir met with the conditions of generating water soluble gas.
The laser Raman analyses of 106 inclusions in calcite (Fig. 3a) prove that all the methane in the inclusions is not gaseous but dissolved and parts of inclusions are CO2, liquid.But, methane in the inclusions is dominated and content of CO2 is rather lower based on peak intensity and peak area of Raman map.
In the same way, the authors analyzed the inclusions in quartz (Fig. 3b) using the laser Raman technique, and the result also demonstrates that the major components are dissolved methane and a small number of other liquid components.To make sure the phase of methane in the inclusions of quartz and calcite, the method of heating and cooling is used.Figure 4 shows that inclusions are present as a single phase at room conditions, and after cooling, the vapor bubbles appear.When temperature changes from-97.5 to-119.4℃, the vapor bubbles become bigger, and when cooling to-127.1℃, liquid phase begins to ice up, and vapor phase iced up at-194.8℃.Reversely, when heated to-111.5℃, the vapor bubble begins to appear, and the vapor bubble shrinks gradually between-108.6 and-92.1℃.When heated to-88.8℃, the vapor phase will homogenize to a single liquid inclusion completely. The experiment of cooling and heating and laser Raman analysis demonstrate that the methane in 106 inclusions measured is present as liquid.At the same time, the homogenization temperature and capture pressure of inclusions indicate that formation of water soluble gas is entirely possible.
As for the methane solubility in water, previous workers have carried out a series of experiments and have plotted many relevant charts (Duan et al., 1992; Battino, 1984;Price, 1979;Bonham, 1978;Haas, 1978). Therefore, the authors use the results to access the methane solubility in water with these published charts.According to the homogenizations and capture pressure of inclusions, it is estimated that approximately 50–90 m3 (volumes of gas are given in standard temperature and pressure, i.e., 15.6℃ and 1.013kPa) methane is dissolved in per litre water under 260–290℃ and 1.2×108–1.6×108 Pa.
Necessary to mention, the abnormal temperature and pressure as well as water soluble gas are not found in the Sinian reservoir, presently.Combined with AFT model results, the authors guess that the gas which was ever dissolved in water possibly exsoluted from water, transferred, dissipated, or reaccumulated because of change of temperature and pressure during uplift.This suggests that the Sinian reservoir should have a bright future for oil and gas exploration.
(1) The thermal history of Sinian reservoir is simulated based on AFT technique and Easy%Ro model, and the result of AFT modeling provides the accurate burial history for Easy%Ro model. The vitrinite reflectance calculated which is used to calibrate paleo-temperature has a better-fit with vitrinite reflectance measured. The paleo-geothermal gradient of Sinian reservoir and source rocks of Lower Cambrian never experienced the process of drop, increasing, and drop generally. (2) The laser Raman analysis shows that the methane in the inclusions of Sinian reservoir is dissolved in the groundwater and has become water soluble gas. The formation condition for water soluble gas was met with based on the reconstructed paleo-temperature and homogenization temperature of inclusions as well as the capture pressure calculated with the PVTsim software.Under the corresponding temperature and pressure, approximately 50–90 m3methane is dissolved in per litre water.
Aplin, A. C., Macleod, G., Larter, S. R., 1999. Combined Use of Confocal Laser Scanning Microscopy and PVT Simula-tion for Estimating the Composition and Physical Proper-ties of Petroleum in Fluid Inclusions. Marine and Petro-leum Geology, 16(2): 97-110 doi: 10.1016/S0264-8172(98)00079-8 |
Arne, D. C., Green, P. F., Duddy, I. R., 1990. Thermochro-nologic Constraints on the Timing of Mississippi Valley-Type Ore Formation from Apatite Fission Track Analysis. International Journal of Radiation Applications and In-strumentation Part D. Nuclear Tracks and Radiation Measurements, 17(3): 319-323 doi: 10.1016/1359-0189(90)90053-Z |
Bonham, L. C., 1978. Solubility of Methane in Water at Ele-vated Temperatures and Pressures. AAPG Bulletin, 62(12): 2478-2481 |
Chen, R., Geng, Q. S., Su, X. B., 2006. The Formation and Accumulation of Water Soluble Gas. Journal of Henan Polytechnic University, 25(3): 205-208 (in Chinese with English Abstract) |
Crowley, K. D., Cameron, M., Schaefer, R. L., 1991. Experi-mental Studies of Annealing Etched Fission Tracks in Fluorapatite. Geochimica et Cosmochimica Acta, 55(5): 1449-1465 doi: 10.1016/0016-7037(91)90320-5 |
di Primio, R., 2002. Unraveling Secondary Migration Effects through the Regional Evaluation of PVT Data: A Case Study from Quadrant 25, NOCS. Organic Geochemistry, 33(6): 643-653 doi: 10.1016/S0146-6380(02)00023-2 |
Duan, Z., Moller, N., Greenberg, J., et al., 1992. The Prediction of Methane Solubility in Natural Waters to High Ionic Strength from 0 to 250 ℃ and from 0 to 1 600 bar. Geo-chimica et Cosmochimica Acta, 56: 1451-1460 doi: 10.1016/0016-7037(92)90215-5 |
Duddy, I. R., Gleadow, A. J. W., Lovering, J. F., 1984. Thermal History of Otway Basin, Australia—Case Study of Fission-Track Analysis in Petroleum Exploration. AAPG Bulletin, 68(4): 472-472 |
Duddy, I. R., Green, P. F., Laslett, G. M., 1988. Thermal An-nealing of Fission Tracks in Apatite: 3, Variable Tem-perature Behaviour. Chemical Geology (Isotope Geo-science Section), 73(1): 25-38 doi: 10.1016/0168-9622(88)90019-X |
Gleadow, A. J. W., Brown, R. W., 2000. Fission Track Ther-mochronology and the Long Term Denudational Response to Tectonics. In: Summerfield, M. A., ed., Geomorphology and Global Tectonics. John Wiley and Sons, Ltd., Chichester. 57-75 |
Gleadow, A. J. W., Duddy, I. R., 1981. A Natural Long-Term Annealing Experiment for Apatite. Nuclear Tracks and Radiation Measurements, 5(2): 169-174 |
Gleadow, A. J. W., Duddy, I. R., Green, P. F., et al., 1986. Con-fined Fission Track Lengths in Apatite, a Diagnostic Tool for Thermal History Analysis. Contributions to Mineral-ogy and Petrology, 94(4): 405-415 doi: 10.1007/BF00376334 |
Gleadow, A. J. W., Duddy, I. R., Lovering, J. F., 1983. Fission Track Analysis: A New Tool for Evaluation of Thermal Histories and Hydrocarbon Potential. Australian Petrol. Explor. Assoc., 23: 93-102 |
Green, P. F., Duddy, A. J. W., Lovering, J. F., 1989a. Apatite Fission Track Analysis as a Paleotemperature Indicator for Hydrocarbon Exploration. In: Naeser, N. D., McCulloh, T. H., eds., Thermal History of Sedimentary Basin. Springer-Verlag, New York. 181-195 |
Green, P. F., Duddy, I. R., Laslett, G., et al., 1989b. Thermal Annealing of Fission Tracks in Apatite: 4, Quantitative Modelling Techniques and Extension to Geological Timescales. Chemical Geology (Isotope Geoscience Sec-tion), 79(2): 155-182 doi: 10.1016/0168-9622(89)90018-3 |
Green, P. F., Duddy, I. R., Gleadow, A. J. W., et al., 1986. Thermal Annealing of Fission Tracks in Apatite 1: A Qualitative Description. Chemical Geology (Isotope Geo-science Section), 59(4): 237-253 |
Guidish, T. M., Kendall, C. G., Lerche, S. T., et al., 1985. Basin Evaluation Using Burial History Calculations—An Over-view. AAPG Bulletin, 69: 92-105 |
Haas, J. A., 1978. An Empirical Equation with Tables of Smoothed Solubilities of Methane in Water and Aqueous Sodium Chloride Solutions up to 25 Weight Percent, 360 ℃, and 138 MPa. US Geological Survey Open File Report, 1004: 42 |
Karsten, F. K., Ondrak, R., di Primio, R., et al., 2008. A Three-Dimensional Insight into the Mackenzie Basin (Canada): Implications for the Thermal History and Hy-drocarbon Generation Potential of Tertiary Deltaic Se-quence. AAPG Bulletin, 92(2): 225-247 doi: 10.1306/10110707027 |
Ketcham, R. A., Donelick, R. A., Donelick, M. B., 2003. AFTSolve: A Program for Multi-kinetic Modeling of Apatite Fission-Track Data. American Mineralogist, 88: 929 |
Laslett, G. M., Green, P. F., Duddy, I. R., et al., 1987. Thermal Annealing of Fission Tracks in Apatite, 2: A Quantitative Analysis. Chemical Geology (Isotope Geoscience Section), 65(1): 1-13 doi: 10.1016/0168-9622(87)90057-1 |
Naeser, C. W., 1979. Fission-Track Dating and Geological An-nealing of Fission Tracks. Springer-Verlag, New York |
Naeser, N. D., McCulloh, T. H., 1989. Thermal History of Sedimentary Basin. Springer-Verlag, New York |
Price, L. C., 1979. Aqueous Solubility of Methane at Elevated Pressures and Temperatures. AAPG Bulletin, 63(9): 1527-1533 |
Qiu, N. S., Hu, S. B., He, L. J., 2004. The Theory and Practice of Thermal Mechanism for Sedimentary Basins. Petro-leum Industry Press, Beijing (in Chinese) |
Sweeney, J., Burnham, A. K., 1990. Evaluation of a Simple Model of Vitrinite Reflectance Based on Chemical Kinet-ics. AAPG Bulletin, 74(4): 1559-1570 |
Ungerer, P., Bessis, F., Chenet, P. Y., 1984. Geological and Geochemical Models in Oil Exploration: Principles and Practical Examples. AAPG Memoir, 35: 53-77 |
Wang, J. A., Wang, J. Y., 1985. Geothermal Characteristics of the Liaohe Graben. Oil & Gas Geology, 6(4): 347-358 (in Chinese with English Abstract) |
Wanger, G. A., 1968. Fission Track Dating of Apatites. Earth and Planetary Science Letters, 4(5): 411-415 doi: 10.1016/0012-821X(68)90072-1 |
Xu, C. H., Zhou, Z. Y., van den Haute, P., et al., 2006. Apatite Fission-Track Thermochronology of Tectonic Evolution in Hefei Basin. Acta Petrolei Sinica, 27(6): 5-13 (in Chinese with English Abstract) |
Xu, G. S., Yuan, H. F., Ma, Y. S., et al., 2007. The Source of Sinian and Lower-Palaeozoic Bitumen and Hydrocarbon Evolution in the Middle and Southeast of the Sichuan Ba-sin. Acta Geologica Sinica, 81(8): 1143-1152 (in Chinese with English Abstract) |
Yang, Y. C., Li, S. J., Zhu, J., 1993. Water-Soluble Gas—A New Resource of Natural Gas in Sichuan Basin. Journal of Southwest Petroleum Institute, 15(1): 16-22 (in Chinese with English Abstract) |
Yao, J. J., Chen, M. J., Hua, A. G., et al., 2003. Formation of the Gas Rreservoirs of the Leshan-Longnüsi Sinian Palaeo-uplift in Central Sichuan. Petroleum Exploration and De-velopment, 30(4): 7-9 (in Chinese with English Abstract) |