Reactive transport modeling(RTM)is an emerging method used to address geological issues in diagenesis research.However,the extrapolation of RTM results to practical reservoir prediction is not sufficiently understood....Reactive transport modeling(RTM)is an emerging method used to address geological issues in diagenesis research.However,the extrapolation of RTM results to practical reservoir prediction is not sufficiently understood.This paper presents a case study of the Eocene Qaidam Basin that combines RTM results with petrological and mineralogical evidence.The results show that the Eocene Xiaganchaigou Formation is characterized by mixed siliciclastic-carbonate-evaporite sedimentation in a semiclosed saline lacustrine environment.Periodic evaporation and salinization processes during the syngeneticpenecontemporaneous stage gave rise to the replacive genesis of dolomites and the cyclic enrichment of dolomite in the middle-upper parts of the meter-scale depositional sequences.The successive change in mineral paragenesis from terrigenous clastics to carbonates to evaporites was reconstructed using RTM simulations.Parametric uncertainty analyses further suggest that the evaporation intensity(brine salinity)and particle size of sediments(reactive surface area)were important rate-determining factors in the dolomitization,as shown by the relatively higher reaction rates under conditions of higher brine salinity and fine-grained sediments.Combining the simulation results with measured mineralogical and reservoir physical property data indicates that the preservation of original intergranular pores and the generation of porosity via replacive dolomitization were the major formation mechanisms of the distinctive lacustrine dolomite reservoirs(widespread submicron intercrystalline micropores)in the Eocene Qaidam Basin.The results confirm that RTM can be effectively used in geological studies,can provide a better general understanding of the dolomitizing fluid-rock interactions,and can shed light on the spatiotemporal evolution of mineralogy and porosity during dolomitization and the formation of lacustrine dolomite reservoirs.展开更多
The chemical equilibrium equations utilized in reactive transport modeling are complex and nonlinear,and are typically solved using the Newton-Raphson method.Although this algorithm is known for its quadratic converge...The chemical equilibrium equations utilized in reactive transport modeling are complex and nonlinear,and are typically solved using the Newton-Raphson method.Although this algorithm is known for its quadratic convergence near the solution,it is less effective far from the solution,especially for ill-conditioned problems.In such cases,the algorithm may fail to converge or require excessive iterations.To address these limitations,a projected Newton method is introduced to incorporate the concept of projection.This method constrains the Newton step by utilizing a chemically allowed interval that generates feasible descending iterations.Moreover,we utilize the positive continuous fraction method as a preconditioning technique,providing reliable initial values for solving the algorithms.The numerical results are compared with those derived using the regular Newton-Raphson method,the Newton-Raphson method based on chemically allowed interval updating rules,and the bounded variable least squares method in six different test cases.The numerical results highlight the robustness and efficacy of the proposed algorithm.展开更多
Geopolymers are alternative binders made solely from industrial by-products and/or natural alumino-silicates, comprising no traditional cements. Reactive transport processes in geopolymer materials play a crucial role...Geopolymers are alternative binders made solely from industrial by-products and/or natural alumino-silicates, comprising no traditional cements. Reactive transport processes in geopolymer materials play a crucial role in both the degradation process of building materials as well as in the containment of hazardous wastes. A numerical model is presented for solving transport coupled to nonlinear ion-exchange equilibria between solid-liquid phases. Bound alkalies provide the geopolymer paste with a large reservoir of exchangeable (soluble) alkalies that allow for a more gradual drop in pH of the pore solution, as compared to a sudden drop when considering only diffusion transport mechanism. The model is robust enough to handle non-linearity of the ion-exchange equations, and presents a more reliable way to obtain long term durability predictions of geopolymer materials.展开更多
It is well known that during CO2 geological storage, density-driven convective activity can significantly accelerate the dissolution of injected CO2 into water. This action could limit the escape of supercritical CO2 ...It is well known that during CO2 geological storage, density-driven convective activity can significantly accelerate the dissolution of injected CO2 into water. This action could limit the escape of supercritical CO2 from the storage formation through vertical pathways such as fractures, faults and abandoned wells, consequently increasing permanence and security of storage. First, we investigated the effect of numerical perturbation caused by time and grid resolution and the convergence criteria on the dissolution-diffusion-convection （DDC） process. Then, using the model with appropriate spatial and temporal resolution, some uncertainty parameters investigated in our previous paper such as initial gas saturation and model boundaries, and other factors such as relative liquid permeability and porosity modification were used to examine their effects on the DDC process. Finally, we compared the effect of 2D and 3D models on the simulation of the DDC process. The above modeling results should contribute to clear understanding and accurate simulation of the DDC process, especially the onset of convective activity, and the CO2 dissolution rate during the convection-dominated stage.展开更多
Under the new development philosophy of carbon peaking and carbon neutrality,CO_(2)and O_(2)in situ leaching(ISL)has been identified as a promising technique for uranium mining in China,not only because it solves carb...Under the new development philosophy of carbon peaking and carbon neutrality,CO_(2)and O_(2)in situ leaching(ISL)has been identified as a promising technique for uranium mining in China,not only because it solves carbon dioxide utilization and sequestration,but it also alleviates the environmental burden.However,significant challenges exist in assessment of CO_(2)footprint and water-rock interactions,due to complex geochemical processes.Herein this study conducts a three-dimensional,multicomponent reactive transport model(RTM)of a field-scale CO_(2)and O_(2)ISL process at a typical sandstone-hosted uranium deposit in Songliao Basin,China.Numerical simulations are performed to provide new insight into quantitative interpretation of the greenhouse gas(CO_(2))footprint and environmental impact(SO_(4)^(2–))of the CO_(2)and O_(2)ISL,considering the potential chemical reaction network for uranium recovery at the field scale.RTM results demonstrate that the fate of the CO_(2)could be summarized as injected CO_(2)dissolution,dissolved CO_(2)mineralization and storage of CO_(2)as a gas phase during the CO_(2)and O_(2)ISL process.Furthermore,compared to acid ISL,CO_(2)and O_(2)ISL has a potentially smaller environmental footprint,with 20%of SO_(4)^(2–)concentration in the aquifer.The findings improve our fundamental understanding of carbon utilization in a long-term CO_(2)and O_(2)ISL system and provide important environmental implications when considering complex geochemical processes.展开更多
Process-based reactive transport modeling(RTM)integrates thermodynamic and kinetically controlled fluid-rock interactions with fluid flow through porous media in the subsurface and surface environment.RTM is usually c...Process-based reactive transport modeling(RTM)integrates thermodynamic and kinetically controlled fluid-rock interactions with fluid flow through porous media in the subsurface and surface environment.RTM is usually conducted through numerical programs based on the first principle of physical processes.However,the calculation for complex chemical reactions in most available programs is an iterative process,where each iteration is in general computationally intensive.A workflow of neural networkbased surrogate model as a proxy for process-based reactive transport simulation is established in this study.The workflow includes(1)base case RTM design,(2)development of training experiments,(3)surrogate model construction based on machine learning,(4)surrogate model validation,and(5)prediction with the calibrated model.The training experiments for surrogate modeling are generated and run prior to the predictions using RTM.The results show that the predictions from the surrogate model agree well with those from processes-based RTM but with a significantly reduced computational time.The well-trained surrogate model is especially useful when a large number of realizations are required,such as the sensitivity analysis or model calibration,which can significantly reduce the computational time compared to that required by RTM.The benefits are(1)it automatizes the experimental design during the sensitivity analysis to get sufficient numbers and coverage of the training cases;(2)it parallelizes the calculations of RTM training cases during the sensitivity analysis to reduce the simulation time;(3)it uses the neural network algorithm to rank the sensitivity of the parameters and to search the optimal solution for model calibration.展开更多
Carbon dioxide injection into deep saline aquifers results in a variety of strongly coupled physical and chemical processes. In this study, reactive transport simulations using a 2-D radial model were performed to inv...Carbon dioxide injection into deep saline aquifers results in a variety of strongly coupled physical and chemical processes. In this study, reactive transport simulations using a 2-D radial model were performed to investigate the fate of the injected CO2, the effect of CO2-water-rock interactions on mineral alteration, and the long-term CO2 sequestration mechanisms of the Liujiagou Formation sandstone at the Shenhua CCS（carbon capture and storage） pilot site of China. Carbon dioxide was injected at a constant rate of 0.1 Mt/year for 30 years, and the fluid flow and geochemical transport simulation was run for a period of 10 000 years by the TOUGHREACT code according to the underground conditions of the Liujiagou Formation. The results show that different trapping phases of CO2 vary with time. Sensitivity analyses indicate that plagioclase composition and chlorite presence are the most significant determinants of stable carbonate minerals and CO2 mineral trapping capacity. For arkosic arenite in the Liujiagou Formation, CO2 can be immobilized by precipitation of ankerite, magnesite, siderite, dawsonite, and calcite for different mineral compositions, with Ca（2＋）, Mg（2＋）, Fe（2＋） and Na＋ provided by dissolution of calcite, albite（or oligoclase） and chlorite. This study can provide useful insights into the geochemistry of CO2 storage in other arkosic arenite（feldspar rich sandstone） formations at other pilots or target sites.展开更多
文摘Reactive transport modeling(RTM)is an emerging method used to address geological issues in diagenesis research.However,the extrapolation of RTM results to practical reservoir prediction is not sufficiently understood.This paper presents a case study of the Eocene Qaidam Basin that combines RTM results with petrological and mineralogical evidence.The results show that the Eocene Xiaganchaigou Formation is characterized by mixed siliciclastic-carbonate-evaporite sedimentation in a semiclosed saline lacustrine environment.Periodic evaporation and salinization processes during the syngeneticpenecontemporaneous stage gave rise to the replacive genesis of dolomites and the cyclic enrichment of dolomite in the middle-upper parts of the meter-scale depositional sequences.The successive change in mineral paragenesis from terrigenous clastics to carbonates to evaporites was reconstructed using RTM simulations.Parametric uncertainty analyses further suggest that the evaporation intensity(brine salinity)and particle size of sediments(reactive surface area)were important rate-determining factors in the dolomitization,as shown by the relatively higher reaction rates under conditions of higher brine salinity and fine-grained sediments.Combining the simulation results with measured mineralogical and reservoir physical property data indicates that the preservation of original intergranular pores and the generation of porosity via replacive dolomitization were the major formation mechanisms of the distinctive lacustrine dolomite reservoirs(widespread submicron intercrystalline micropores)in the Eocene Qaidam Basin.The results confirm that RTM can be effectively used in geological studies,can provide a better general understanding of the dolomitizing fluid-rock interactions,and can shed light on the spatiotemporal evolution of mineralogy and porosity during dolomitization and the formation of lacustrine dolomite reservoirs.
基金supported by the National Natural Science Foundation of China(Grant Nos.22178190 and 22008129).
文摘The chemical equilibrium equations utilized in reactive transport modeling are complex and nonlinear,and are typically solved using the Newton-Raphson method.Although this algorithm is known for its quadratic convergence near the solution,it is less effective far from the solution,especially for ill-conditioned problems.In such cases,the algorithm may fail to converge or require excessive iterations.To address these limitations,a projected Newton method is introduced to incorporate the concept of projection.This method constrains the Newton step by utilizing a chemically allowed interval that generates feasible descending iterations.Moreover,we utilize the positive continuous fraction method as a preconditioning technique,providing reliable initial values for solving the algorithms.The numerical results are compared with those derived using the regular Newton-Raphson method,the Newton-Raphson method based on chemically allowed interval updating rules,and the bounded variable least squares method in six different test cases.The numerical results highlight the robustness and efficacy of the proposed algorithm.
文摘Geopolymers are alternative binders made solely from industrial by-products and/or natural alumino-silicates, comprising no traditional cements. Reactive transport processes in geopolymer materials play a crucial role in both the degradation process of building materials as well as in the containment of hazardous wastes. A numerical model is presented for solving transport coupled to nonlinear ion-exchange equilibria between solid-liquid phases. Bound alkalies provide the geopolymer paste with a large reservoir of exchangeable (soluble) alkalies that allow for a more gradual drop in pH of the pore solution, as compared to a sudden drop when considering only diffusion transport mechanism. The model is robust enough to handle non-linearity of the ion-exchange equations, and presents a more reliable way to obtain long term durability predictions of geopolymer materials.
基金This work was supported by the National Natural Science Foundation of China （Grant No. 40872158）, China Geological Survey Project （Grant Nos. 1212011220914 and 1212011220794）, and Librarian＇s Project of National Geological Library of China （Grant No. GZ201203）.
文摘It is well known that during CO2 geological storage, density-driven convective activity can significantly accelerate the dissolution of injected CO2 into water. This action could limit the escape of supercritical CO2 from the storage formation through vertical pathways such as fractures, faults and abandoned wells, consequently increasing permanence and security of storage. First, we investigated the effect of numerical perturbation caused by time and grid resolution and the convergence criteria on the dissolution-diffusion-convection （DDC） process. Then, using the model with appropriate spatial and temporal resolution, some uncertainty parameters investigated in our previous paper such as initial gas saturation and model boundaries, and other factors such as relative liquid permeability and porosity modification were used to examine their effects on the DDC process. Finally, we compared the effect of 2D and 3D models on the simulation of the DDC process. The above modeling results should contribute to clear understanding and accurate simulation of the DDC process, especially the onset of convective activity, and the CO2 dissolution rate during the convection-dominated stage.
基金supported by the National Natural Science Foundation of China(Grant No.U2167212)。
文摘Under the new development philosophy of carbon peaking and carbon neutrality,CO_(2)and O_(2)in situ leaching(ISL)has been identified as a promising technique for uranium mining in China,not only because it solves carbon dioxide utilization and sequestration,but it also alleviates the environmental burden.However,significant challenges exist in assessment of CO_(2)footprint and water-rock interactions,due to complex geochemical processes.Herein this study conducts a three-dimensional,multicomponent reactive transport model(RTM)of a field-scale CO_(2)and O_(2)ISL process at a typical sandstone-hosted uranium deposit in Songliao Basin,China.Numerical simulations are performed to provide new insight into quantitative interpretation of the greenhouse gas(CO_(2))footprint and environmental impact(SO_(4)^(2–))of the CO_(2)and O_(2)ISL,considering the potential chemical reaction network for uranium recovery at the field scale.RTM results demonstrate that the fate of the CO_(2)could be summarized as injected CO_(2)dissolution,dissolved CO_(2)mineralization and storage of CO_(2)as a gas phase during the CO_(2)and O_(2)ISL process.Furthermore,compared to acid ISL,CO_(2)and O_(2)ISL has a potentially smaller environmental footprint,with 20%of SO_(4)^(2–)concentration in the aquifer.The findings improve our fundamental understanding of carbon utilization in a long-term CO_(2)and O_(2)ISL system and provide important environmental implications when considering complex geochemical processes.
文摘Process-based reactive transport modeling(RTM)integrates thermodynamic and kinetically controlled fluid-rock interactions with fluid flow through porous media in the subsurface and surface environment.RTM is usually conducted through numerical programs based on the first principle of physical processes.However,the calculation for complex chemical reactions in most available programs is an iterative process,where each iteration is in general computationally intensive.A workflow of neural networkbased surrogate model as a proxy for process-based reactive transport simulation is established in this study.The workflow includes(1)base case RTM design,(2)development of training experiments,(3)surrogate model construction based on machine learning,(4)surrogate model validation,and(5)prediction with the calibrated model.The training experiments for surrogate modeling are generated and run prior to the predictions using RTM.The results show that the predictions from the surrogate model agree well with those from processes-based RTM but with a significantly reduced computational time.The well-trained surrogate model is especially useful when a large number of realizations are required,such as the sensitivity analysis or model calibration,which can significantly reduce the computational time compared to that required by RTM.The benefits are(1)it automatizes the experimental design during the sensitivity analysis to get sufficient numbers and coverage of the training cases;(2)it parallelizes the calculations of RTM training cases during the sensitivity analysis to reduce the simulation time;(3)it uses the neural network algorithm to rank the sensitivity of the parameters and to search the optimal solution for model calibration.
基金supported by the Global Climate and Energy Project(No.2384638-43106-A)the National Natural Science Foundation of China(No.41072180)+1 种基金the Special Scientific Research Fund of Public Welfare Profession of the Ministry of Land and Resources of China(No.201211063)a bilateral project of China Australia Geological Storage of CO2 Project Phase 2(CAGS2)
文摘Carbon dioxide injection into deep saline aquifers results in a variety of strongly coupled physical and chemical processes. In this study, reactive transport simulations using a 2-D radial model were performed to investigate the fate of the injected CO2, the effect of CO2-water-rock interactions on mineral alteration, and the long-term CO2 sequestration mechanisms of the Liujiagou Formation sandstone at the Shenhua CCS（carbon capture and storage） pilot site of China. Carbon dioxide was injected at a constant rate of 0.1 Mt/year for 30 years, and the fluid flow and geochemical transport simulation was run for a period of 10 000 years by the TOUGHREACT code according to the underground conditions of the Liujiagou Formation. The results show that different trapping phases of CO2 vary with time. Sensitivity analyses indicate that plagioclase composition and chlorite presence are the most significant determinants of stable carbonate minerals and CO2 mineral trapping capacity. For arkosic arenite in the Liujiagou Formation, CO2 can be immobilized by precipitation of ankerite, magnesite, siderite, dawsonite, and calcite for different mineral compositions, with Ca（2＋）, Mg（2＋）, Fe（2＋） and Na＋ provided by dissolution of calcite, albite（or oligoclase） and chlorite. This study can provide useful insights into the geochemistry of CO2 storage in other arkosic arenite（feldspar rich sandstone） formations at other pilots or target sites.
