含CO_2流体—泥岩相互作用的特征与机制
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摘要
松辽盆地南部中央坳陷广泛分布有指示CO_2渗漏的片钠铝石，是归纳和总结CO_2渗漏标志和揭示CO_2大规模渗漏机制的理想场所。泥质岩夹层主要由泥岩和粉砂岩组成，厚度以0.5-2m居多。岩石学与地球化学研究表明，泥岩夹层中发生溶蚀溶解的矿物包括斜长石和钾长石，沉淀的自生矿物有菱铁矿和片钠铝石。片钠铝石是典型的与CO_2充注具有成因联系的“示踪”矿物。在天然CO_2系统中的泥岩夹层与下伏含片钠铝石砂岩界面处，主要氧化物含量向上具有规律性的变化，厚层泥岩中，K_2O、Al_2O_3、Fe_2O_3、CaO和MgO的含量自砂泥岩接触界面处向上升高，Na_2O和FeO含量则相反。薄层泥岩中，地球化学特征在纵向上不显示规律性的变化。通过CO_2—泥岩相互作用实验和TOUGHREACT地球化学数值模拟，验证和补充了岩石学观察结果。在上述研究的基础上，建立了CO_2—泥岩相互作用的概念模式。本次研究成果将为CO_2地质埋存工程提供基础地质信息。
Geological sequestration of industrial CO_2is an effective way to slow down theglobal warming. Demonstration projects are done by some countries in succession,along with the further study of CO_2geologic sequestration. It becomes one of themost important problems that how to decrease the risks of CO_2leakage. The integrityand stability was brought up naturally as the leading topic of the safty for CO_2geologic sequestration. The main scientific questions are the characteristics ofCO_2-mudstone caprock interaction and its impact on the capability of CO_2sequestration during the geologic period. Natural CO_2system is the natural analoguesof CO_2geologic sequestration. And dawsonite is the traced mineral of CO_2migrationand accumulation. Therefore, mudstone interlayers in dawsonite-bearing sandstoneformations are the most ideal research objects for the study of CO_2-mudstoneinteraction. The achievements of this research would provide proofs for geologicalsafety evaluation of CO_2sequestration, which makes the research having academicvalue and actual applied value.
Comparative petrology, CO_2fluid-mudstone interaction experiments andnumerical simulation are used in the study. The object of comparative petrology is themudstone interlayers and the matched cores’ rocks in dawsonite-bearing sandstoneformation in South Songliao Basin. Matched cores’s rocks are the mudstones occurrednear the objective interlayers which show the similar sedimentary and diageneticfeatures without impact from CO_2fluid. FXY autoclave is used in the experiments of CO_2-mudstone interaction. The simulative software is TOUGHREACT.
In the natural CO_2system in Honggang anticline and Huazijing district, themudstone interlayers are mainly consist of mudstone and siltstone. Thickness of theseinterlayers focus on0.5-2m, no more than11m. Plagioclase and orthoclase in themudstone interlayers are corroded, while dawsonite and siderite are precipitated aspart of authigenic minerals. The dissolution grade of orthoclase and plagioclase in theinterlayers are obviously higher than in matched cores’s rocks. So the development ofdissolution in the interlayers could relate to the CO_2-mudstone interaction. Theauthigenic dawsonite is a typical “trace” of CO_2injection in the Honggang anticline.Authigenic siderite is developed in the Huazijing district, which could due to the CO_2injection, either. The contained Fe~(2+)in the CO_2fluid combined HCO_3~(2-), and formedsiderite during the fluid flooding the mudstone.
Contents of the main oxides change regularly upwards near the interface betweenmudstone interlayers and underlain dawsonite-bearing sandstones. In Huazijingterrace, contents of K_2O, Al_2O_3, Fe_2O_3, CaO and MgO in mudstones display afluctuating increase from the interface up while contents of Na_2O and FeO display theopposite trend. Possible explanations responsible for this change may attribute to thedissolution process of K-feldspar, calcite, dolomite and Fe~(3+)compound during CO_2leakage towards overlying mudstones and the migration of related ions. Thisphenomenon is the most obvious at the interface between dawsonite-bearingsandstones and mudstones. The decrease in the content of FeO is probably owing tothe reduction from Fe~(3+)to Fe~(2+), as for Na_2O, reasons for the decrease is yet unclear. InHonggang terrace, in the depth of1481.2~1481.22m, contentsof FeO, MgO, K_2O andAl_2O_3in mudstones tend to increase upwards near the interface between sandstonesand mudstones while content of Na_2O shows an opposite change. This change istriggered by the same mechanism related to CO_2leakage as which in Huazijingterrace. Content variation of Na_2O may be a result of dawsonite precipitation. Inmudstones interval of1477.5~1477.53m, the maim oxides display no verticallyregular change. One possible explanation is that thin layers of mudstones andsandstones sink in CO_2fluid, thus no regular petrographic and geochemical changes can be observed.
Experiments of CO_2-mudstone interactions have verified petrographicobservations. Results show that total salinity, pH values decrease and concentrationsof K~+, Na~+and SiO_2increase as the increase of reaction temperature. TheConcentration of Ca~(2+)、Mg~(2+)has increased in low temperatures, while decreased inhigh temperature. Deoxidation from Fe~(3+)to Fe~(2+)with the increasing temperaturesleads to the colour fading of mudstone surface. Feldspar, quartz has dissolved, whileCalcite, siderite and chlorite mainly dissolve under relatively low temperatures(100℃、130℃); indissolvable carbonates occur under higher temperatures(160℃、190℃、220℃).
Geochemical simulation by TOUGHREACT has reestablished thedissolution-precipitation process of minerals. The influential extent of CO_2influx is1500m horizontally and17m vertically from sand-shale interface. Results reveal thatdissolved minerals include K-feldspar, albite, chlorite and semctite; precipitatedauthigenetic carbonate minerals are calcite, ankerite, magnesite and dawsonite, othersinclude kaolinite, illite and micro-quartz. As time goes by, concentration of HCO﹣3、K~+、Ca~(2+)has increased, while Na~+、Mg~(2+)、Fe~(2+)has increased in short time, decreasingin long time.
With natural analogy, CO_2fuild and mudrock interation and numericalsimulation on the process of dissolution-percipitation, building a model of CO_2–murock interation. As thin layers of mudstone and sandstone soaking in CO_2fluidPetrological and geochemical characteristics should not display regularly change onthe longthways. CO_2was filled in sandstone leak to mudstone which is a thick layer inthe form of diffusion
The innovation points in this study mainly embodied in the method of naturalanalog, which interprets the petrology and geochemistry records of CO_2leakage inmudstone interlayers in natural CO_2system of the South Songliao Basin. And thepetrology results are complemented and verified by CO_2-mudstone interaction andnumerical simulation. CO_2-mudstone interaction model are built according to all thestudy results mentioned above. The achievements in this study could provide basic geologic information, ensure the possibility of permanent CO_2sequestration, andenhance the security of CO_2geologic sequestration.
Geological sequestration of industrial CO_2is an effective way to slow down theglobal warming. Demonstration projects are done by some countries in succession,along with the further study of CO_2geologic sequestration. It becomes one of themost important problems that how to decrease the risks of CO_2leakage. The integrityand stability was brought up naturally as the leading topic of the safty for CO_2geologic sequestration. The main scientific questions are the characteristics ofCO_2-mudstone caprock interaction and its impact on the capability of CO_2sequestration during the geologic period. Natural CO_2system is the natural analoguesof CO_2geologic sequestration. And dawsonite is the traced mineral of CO_2migrationand accumulation. Therefore, mudstone interlayers in dawsonite-bearing sandstoneformations are the most ideal research objects for the study of CO_2-mudstoneinteraction. The achievements of this research would provide proofs for geologicalsafety evaluation of CO_2sequestration, which makes the research having academicvalue and actual applied value.
Comparative petrology, CO_2fluid-mudstone interaction experiments andnumerical simulation are used in the study. The object of comparative petrology is themudstone interlayers and the matched cores’ rocks in dawsonite-bearing sandstoneformation in South Songliao Basin. Matched cores’s rocks are the mudstones occurrednear the objective interlayers which show the similar sedimentary and diageneticfeatures without impact from CO_2fluid. FXY autoclave is used in the experiments of CO_2-mudstone interaction. The simulative software is TOUGHREACT.
In the natural CO_2system in Honggang anticline and Huazijing district, themudstone interlayers are mainly consist of mudstone and siltstone. Thickness of theseinterlayers focus on0.5-2m, no more than11m. Plagioclase and orthoclase in themudstone interlayers are corroded, while dawsonite and siderite are precipitated aspart of authigenic minerals. The dissolution grade of orthoclase and plagioclase in theinterlayers are obviously higher than in matched cores’s rocks. So the development ofdissolution in the interlayers could relate to the CO_2-mudstone interaction. Theauthigenic dawsonite is a typical “trace” of CO_2injection in the Honggang anticline.Authigenic siderite is developed in the Huazijing district, which could due to the CO_2injection, either. The contained Fe~(2+)in the CO_2fluid combined HCO_3~(2-), and formedsiderite during the fluid flooding the mudstone.
Contents of the main oxides change regularly upwards near the interface betweenmudstone interlayers and underlain dawsonite-bearing sandstones. In Huazijingterrace, contents of K_2O, Al_2O_3, Fe_2O_3, CaO and MgO in mudstones display afluctuating increase from the interface up while contents of Na_2O and FeO display theopposite trend. Possible explanations responsible for this change may attribute to thedissolution process of K-feldspar, calcite, dolomite and Fe~(3+)compound during CO_2leakage towards overlying mudstones and the migration of related ions. Thisphenomenon is the most obvious at the interface between dawsonite-bearingsandstones and mudstones. The decrease in the content of FeO is probably owing tothe reduction from Fe~(3+)to Fe~(2+), as for Na_2O, reasons for the decrease is yet unclear. InHonggang terrace, in the depth of1481.2~1481.22m, contentsof FeO, MgO, K_2O andAl_2O_3in mudstones tend to increase upwards near the interface between sandstonesand mudstones while content of Na_2O shows an opposite change. This change istriggered by the same mechanism related to CO_2leakage as which in Huazijingterrace. Content variation of Na_2O may be a result of dawsonite precipitation. Inmudstones interval of1477.5~1477.53m, the maim oxides display no verticallyregular change. One possible explanation is that thin layers of mudstones andsandstones sink in CO_2fluid, thus no regular petrographic and geochemical changes can be observed.
Experiments of CO_2-mudstone interactions have verified petrographicobservations. Results show that total salinity, pH values decrease and concentrationsof K~+, Na~+and SiO_2increase as the increase of reaction temperature. TheConcentration of Ca~(2+)、Mg~(2+)has increased in low temperatures, while decreased inhigh temperature. Deoxidation from Fe~(3+)to Fe~(2+)with the increasing temperaturesleads to the colour fading of mudstone surface. Feldspar, quartz has dissolved, whileCalcite, siderite and chlorite mainly dissolve under relatively low temperatures(100℃、130℃); indissolvable carbonates occur under higher temperatures(160℃、190℃、220℃).
Geochemical simulation by TOUGHREACT has reestablished thedissolution-precipitation process of minerals. The influential extent of CO_2influx is1500m horizontally and17m vertically from sand-shale interface. Results reveal thatdissolved minerals include K-feldspar, albite, chlorite and semctite; precipitatedauthigenetic carbonate minerals are calcite, ankerite, magnesite and dawsonite, othersinclude kaolinite, illite and micro-quartz. As time goes by, concentration of HCO﹣3、K~+、Ca~(2+)has increased, while Na~+、Mg~(2+)、Fe~(2+)has increased in short time, decreasingin long time.
With natural analogy, CO_2fuild and mudrock interation and numericalsimulation on the process of dissolution-percipitation, building a model of CO_2–murock interation. As thin layers of mudstone and sandstone soaking in CO_2fluidPetrological and geochemical characteristics should not display regularly change onthe longthways. CO_2was filled in sandstone leak to mudstone which is a thick layer inthe form of diffusion
The innovation points in this study mainly embodied in the method of naturalanalog, which interprets the petrology and geochemistry records of CO_2leakage inmudstone interlayers in natural CO_2system of the South Songliao Basin. And thepetrology results are complemented and verified by CO_2-mudstone interaction andnumerical simulation. CO_2-mudstone interaction model are built according to all thestudy results mentioned above. The achievements in this study could provide basic geologic information, ensure the possibility of permanent CO_2sequestration, andenhance the security of CO_2geologic sequestration.
引文
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