CO_(2)+O_(2) in-situ leaching(ISL)of sandstonetype uranium ore represents the third generation of solution mining in China.In this study,reactive transport modeling of the interaction between hydrodynamic and geochemi...CO_(2)+O_(2) in-situ leaching(ISL)of sandstonetype uranium ore represents the third generation of solution mining in China.In this study,reactive transport modeling of the interaction between hydrodynamic and geochemical reactions is performed to enable better prediction and regulation of the CO_(2)+O_(2) in-situ leaching process of uranium.Geochemical reactions between mining solutions and rock,and the kinetic uranium dissolution controlled by O_(2)(aq)and bicarbonate(HCO_(3)-)are considered in the CO_(2)+O_(2) ISL reactive transport model of a typical sandstone-hosted uranium ore deposit in northern China.The reactive leaching of uranium is most sensitive to the spatial distribution of the mineralogical properties of the uranium deposit.Stochastic geostatistical models are used to represent the uncertainty on the spatial distribution of mineral grades.A Monte Carlo analysis was also performed to simulate the uranium production variability over an entire set of geostatistical realizations.The ISL stochastic simulation performed with the selected geostatistical realizations approximates the uranium production variability well.The simulation results of the ISL reactive transport model show that the extent of the uranium plume is highly dependent on mineralogical heterogeneity.The uncertainty analysis suggests the effect of uranium grade heterogeneity was found to be important to improve the accurate capture of the uncertainty.This study provides guidance for the accurate simulation and dynamic regulation of the CO_(2)+O_(2) leaching process of uranium at the scale of large mining areas.展开更多
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
A three-dimensional multicomponent multiphase lattice Boltzmann model(LBM)is established to model the coupled two-phase and reactive transport phenomena in the cathode electrode of proton exchange membrane fuel cells....A three-dimensional multicomponent multiphase lattice Boltzmann model(LBM)is established to model the coupled two-phase and reactive transport phenomena in the cathode electrode of proton exchange membrane fuel cells.The gas diff usion layer(GDL)and microporous layer(MPL)are stochastically reconstructed with the inside dynamic distribution of oxygen and liquid water resolved,and the catalyst layer is simplifi ed as a superthin layer to address the electrochemical reaction,which provides a clear description of the fl ooding eff ect on mass transport and performance.Diff erent kinds of electrodes are reconstructed to determine the optimum porosity and structure design of the GDL and MPL by comparing the transport resistance and per-formance under the fl ooding condition.The simulation results show that gradient porosity GDL helps to increase the reactive area and average concentration under fl ooding.The presence of the MPL ensures the oxygen transport space and reaction area because liquid water cannot transport through micropores.Moreover,the MPL helps in the uniform distribution of oxygen for an effi cient in-plane transport capacity.Crack and perforation structures can accelerate the water transport in the assembly.The systematic perforation design yields the best performance under fl ooding by separating the transport of liquid water and oxygen.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
Reactive transport equations in porous media are critical in various scientific and engineering disciplines,but solving these equations can be computationally expensive when exploring different scenarios,such as varyi...Reactive transport equations in porous media are critical in various scientific and engineering disciplines,but solving these equations can be computationally expensive when exploring different scenarios,such as varying porous structures and initial or boundary conditions.The deep operator network(DeepONet)has emerged as a popular deep learning framework for solving parametric partial differential equations.However,applying the DeepONet to porous media presents significant challenges due to its limited capability to extract representative features from intricate structures.To address this issue,we propose the Porous-DeepONet,a simple yet highly effective extension of the DeepONet framework that leverages convolutional neural networks(CNNs)to learn the solution operators of parametric reactive transport equations in porous media.By incorporating CNNs,we can effectively capture the intricate features of porous media,enabling accurate and efficient learning of the solution operators.We demonstrate the effectiveness of the Porous-DeepONet in accurately and rapidly learning the solution operators of parametric reactive transport equations with various boundary conditions,multiple phases,and multiphysical fields through five examples.This approach offers significant computational savings,potentially reducing the computation time by 50–1000 times compared with the finite-element method.Our work may provide a robust alternative for solving parametric reactive transport equations in porous media,paving the way for exploring complex phenomena in porous media.展开更多
Acid mine drainage（AMD） is commonly treated by neutralization with alkaline substances.This treatment is supported by titration experiments that illustrate the buffering mechanisms and estimate the base neutralizati...Acid mine drainage（AMD） is commonly treated by neutralization with alkaline substances.This treatment is supported by titration experiments that illustrate the buffering mechanisms and estimate the base neutralization capacity（BNC） of the AMD.Detailed explanation of titration curves requires modeling with a hydro-chemical model.In this study the titration curves of water samples from the drainage of the As Pontes mine and the corresponding dumps have been investigated and six buffers are selerted by analyzing those curves.Titration curves have been simulated by a reactive transport model to discover the detailed buffering mechanisms.These simulations show seven regions involving different buffering mechanism.The BNC is primarily from buffers of dissolved Fe,Al and hydrogen sulfate.The BNC can be approximated by：BNC = 3（C_（Fe） ＋ C_（Al）） ＋ 0.05C_（sulfate）,where the units are mol/L.The BNC of the sample from the mine is 9.25×10^（-3） mol/L and that of the dumps sample is 1.28×10^（-2） mol/L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
Earthquake-related hydrochemical changes in thermal springs have been widely observed;however,quantitative modeling of the reactive transport process is absent.In the present study,we apply reactive transport simulati...Earthquake-related hydrochemical changes in thermal springs have been widely observed;however,quantitative modeling of the reactive transport process is absent.In the present study,we apply reactive transport simulation to capture the hydrochemical responses in a thermal spring following the Wenchuan Ms 8.0 and Lushan Ms 7.0 earthquakes.We first constrain deep reservoir geothermal fluid compositions and temperature by multicomponent geothermometry,and then a reactive geochemical transport model is constructed to reproduce the hydrochemical evolution process.The results show that the recharge from the shallow aquifer increases gradually until it reaches a peak because of the permeability enhancement caused by the Lushan earthquake,which may be the mechanism to explain the earthquake-related hydrochemical responses.In contrast to the postseismic effect of the Wenchuan earthquake,the chemical evolution can be considered as hydrochemical anomalies related to the Lushan earthquake.This study proves that the efficient simulation of reactive transport processes is useful for investigating earthquake-related signals in hydrochemical time series.展开更多
The overestimation of the contaminant concentration is a main issue in simulating the reactive transport using the common advection-dispersion-reaction equation （ADRE）. To solve this problem, a new modeling method i...The overestimation of the contaminant concentration is a main issue in simulating the reactive transport using the common advection-dispersion-reaction equation （ADRE）. To solve this problem, a new modeling method is developed. The parameters of the model are identified based on experimental data. The results of the model are compared with previous results in the literature, and the sensitivity of the model is analyzed by examining the model＇s response to changes of the model parameters. Main conclusions are as follows： （1） The numerical modeling approach is feasible with an improved simulating accuracy. The predicted values are in agreement with the experimental measurements. The relative errors of the peak concentration between the simulated and experimental values are less than 2.5%. The errors are greatly reduced as compared with the results （about 67.8% as the maximum） based on a traditional ADRE in the literature. （2） There are three parameters （m, β0 and D ） which can be calibrated on the basis of experimental data in the model. The reactive product concentrations are mainly influenced by the parameters involved in the reactive ratio such as m and β0 The hydrodynamic dispersion coefficient D has almost no influence on the reactive product transport. （3） Our model does not provide better fitting curves for the ＂early arrival＂ and the ＂long tail＂. The ＂early arrival＂ and the ＂long tail＂ are associated with low values of the product AB. Under these conditions, the reaction rate is close to 0, and the model of the ADRE reduces to the advection-dispersion equation （ADE）. Further mechanism study is needed in the future.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
Porosity,tortuosity,specific surface area(SSA),and permeability are four key parameters of reactive transport modeling in sandstone,which are important for understanding solute transport and geochemical reaction pro-c...Porosity,tortuosity,specific surface area(SSA),and permeability are four key parameters of reactive transport modeling in sandstone,which are important for understanding solute transport and geochemical reaction pro-cesses in sandstone aquifers.These four parameters reflect the characteristics of pore structure of sandstone from different perspectives,and the traditional empirical formulas cannot make accurate predictions of them due to their complexity and heterogeneity.In this paper,eleven types of sandstone CT images were firstly segmented into numerous subsample images,the porosity,tortuosity,SSA,and permeability of the subsamples were calculated,and the dataset was established.The 3D convolutional neural network(CNN)models were subse-quently established and trained to predict the key reactive transport parameters based on subsample CT images of sandstones.The results demonstrated that the 3D CNN model with multiple outputs exhibited excellent prediction ability for the four parameters compared to the traditional empirical formulas.In particular,for the prediction of tortuosity and permeability,the 3D CNN model with multiple outputs even showed slightly better prediction ability than its single-output variant model.Additionally,it demonstrated good generalization per-formance on sandstone CT images not included in the training dataset.The study showed that the 3D CNN model with multiple outputs has the advantages of simplifying operation and saving computational resources,which has the prospect of popularization and application.展开更多
Naturally occurring radium(^(223)Ra,^(224)Ra,^(226)Ra,and^(228)Ra)isotopes have been widely applied as geochemical tracers in marine environments,especially when estimating the submarine groundwater discharge(SGD).In ...Naturally occurring radium(^(223)Ra,^(224)Ra,^(226)Ra,and^(228)Ra)isotopes have been widely applied as geochemical tracers in marine environments,especially when estimating the submarine groundwater discharge(SGD).In this sense,the influencing factors and transport mechanism of radium isotope activity in aquifers can be key information for SGD estimation.This work evaluates the adsorption/desorption behavior of^(224)Ra and^(226)Ra in the solid-liquid phase through a leaching experiment and analysis of field data.The results suggested that radium isotope activity was positively correlated with salinity and grain size,in the case of abundant sediments.Through ion analysis,we found that the ions(Na^(+),Ca^(2+),Mg^(2+),and Ba^(2+))exchanged with radium isotopes in the process of transport.A 1-D reactive transport model was established to simulate the transport process of radium isotope in aquifers.The model successfully simulated the variation of radium isotope desorption activity with salinity and was subsequently verified in the field.This study contributes to the understanding of the geochemical behavior of radium isotopes in aquifers and provides guidance for selecting a suitable groundwater endmember in SGD estimation.展开更多
The Enhanced Geothermal System(EGS) is an artificial geothermal system that aims to economically extract heat from hot dry rock(HDR) through the creation of an artificial geothermal reservoir. Chemical stimulation is ...The Enhanced Geothermal System(EGS) is an artificial geothermal system that aims to economically extract heat from hot dry rock(HDR) through the creation of an artificial geothermal reservoir. Chemical stimulation is thought to be an effective method to create fracture networks and open existing fractures in hot dry rocks by injecting chemical agents into the reservoir to dissolve the minerals. Granite is a common type of hot dry rock. In this paper, a series of chemical stimulation experiments were implemented using acid and alkaline agents under high temperature and pressure conditions that mimic the environment of formation. Granite rock samples used in the experiments are collected from the potential EGS reservoir in the Matouying area, Hebei, China. Laboratory experimental results show that the corrosion ratio per unit area of rock is 3.2% in static acid chemical experiments and 0.51% in static alkaline chemical experiments. The permeability of the core is increased by 1.62 times in dynamic acid chemical experiments and 2.45 times in dynamic alkaline chemical experiments. A scanning electron microscope analysis of the core illustrates that secondary minerals, such as chlorite, spherical silica, and montmorillonite, were formed, due to acid-rock interaction with plagioclase being precipitated by alkaline-rock interactions. Masking agents in alkaline chemical agents can slightly reduce the degree of plagioclase formation. A chemical simulation model was built using TOUGHREACT, the mineral dissolution and associated ion concentration variation being reproduced by this reactive transport model.展开更多
Dissolution of fluorite(CaF2)and/or fluorapatite(FAP)[Cas(PO4)3F],pulled by calcite precipitation,is thought to be the dominant mechanism responsible for groundwater fluoride(F)contamination.Here,one dimensional react...Dissolution of fluorite(CaF2)and/or fluorapatite(FAP)[Cas(PO4)3F],pulled by calcite precipitation,is thought to be the dominant mechanism responsible for groundwater fluoride(F)contamination.Here,one dimensional reactive-transport models are developed to test this mechanism using the published dissolution and precipitation rate kinetics for the mineral pair FAP and calcite.Simulation results correctly show positive correlation between the aqueous concentrations of F and CO_(2)and negative correlation between F-and Ca^2+.Results also show that precipitation of calcite,contrary to the present understanding,slows down the FAP dissolution by 10G orders of magnitude compared to the FAP dissolution by hydrolysis.For appreciable amount of fluoride contamination rock-water interaction time must be long and of order 106 years.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
Geomaterials with inferior hydraulic and strength characteristics often need improvement to enhance their engineering behaviors.Traditional ground improvement techniques require enormous mechanical effort or synthetic...Geomaterials with inferior hydraulic and strength characteristics often need improvement to enhance their engineering behaviors.Traditional ground improvement techniques require enormous mechanical effort or synthetic chemicals.Sustainable stabilization technique such as microbially induced calcite precipitation(MICP)utilizes bacterial metabolic processes to precipitate cementitious calcium carbonate.The reactive transport of biochemical species in the soil mass initiates the precipitation of biocement during the MICP process.The precipitated biocement alters the hydro-mechanical performance of the soil mass.Usually,the flow,deformation,and transport phenomena regulate the biocementation technique via coupled bio-chemo-hydro-mechanical(BCHM)processes.Among all,one crucial phenomenon controlling the precipitation mechanism is the encapsulation of biomass by calcium carbonate.Biomass encapsulation can potentially reduce the biochemical reaction rate and decelerate biocementation.Laboratory examination of the encapsulation process demands a thorough analysis of associated coupled effects.Despite this,a numerical model can assist in capturing the coupled processes influencing encapsulation during the MICP treatment.However,most numerical models did not consider biochemical reaction rate kinetics accounting for the influence of bacterial encapsulation.Given this,the current study developed a coupled BCHM model to evaluate the effect of encapsulation on the precipitated calcite content using a micro-scale semiempirical relationship.Firstly,the developed BCHM model was verified and validated using numerical and experimental observations of soil column tests.Later,the encapsulation phenomenon was investigated in the soil columns of variable maximum calcite crystal sizes.The results depict altered reaction rates due to the encapsulation phenomenon and an observable change in the precipitated calcite content for each maximum crystal size.Furthermore,the permeability and deformation of the soil mass were affected by the simultaneous precipitation of calcium carbonate.Overall,the present study comprehended the influence of the encapsulation of bacteria on cement morphology-induced permeability,biocement-induced stresses and displacements.展开更多
The purpose of this paper is to analyze some features of contaminant flow passing through cracked porous medium,such as the influence of fracture network on the advection and diffusion of contaminant species,the impac...The purpose of this paper is to analyze some features of contaminant flow passing through cracked porous medium,such as the influence of fracture network on the advection and diffusion of contaminant species,the impact of adsorption on the overall transport of contaminant wastes.In order to precisely describe the whole process,we firstly build the mathematical model to simulate this problem numerically.Taking into consideration of the characteristics of contaminant flow,we employ two partial differential equations to formulate the whole problem.One is flow equation;the other is reactive transport equation.The first equation is used to describe the total flow of contaminant wastes,which is based on Darcy law.The second one will characterize the adsorption,diffusion and convection behavior of contaminant species,which describes most features of contaminant flow we are interested in.After the construction of numerical model,we apply locally conservative and compatible algorithms to solve this mathematical model.Specifically,we apply Mixed Finite Element(MFE)method to the flow equation and Discontinuous Galerkin(DG)method for the transport equation.MFE has a good convergence rate and numerical accuracy for Darcy velocity.DG is more flexible and can be used to deal with irregular meshes,as well as little numerical diffusion.With these two numerical means,we investigate the sensitivity analysis of different features of contaminant flow in our model,such as diffusion,permeability and fracture density.In particular,we study Kd values which represent the distribution of contaminant wastes between the solid and liquid phases.We also make omparisons of two different schemes and discuss the advantages of both methods.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
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
基金jointly supported by the National Key Research and Development Program of China(No.2019YFC1804304)the National Natural Science Foundation of China(Nos.2167212,41772254)。
文摘CO_(2)+O_(2) in-situ leaching(ISL)of sandstonetype uranium ore represents the third generation of solution mining in China.In this study,reactive transport modeling of the interaction between hydrodynamic and geochemical reactions is performed to enable better prediction and regulation of the CO_(2)+O_(2) in-situ leaching process of uranium.Geochemical reactions between mining solutions and rock,and the kinetic uranium dissolution controlled by O_(2)(aq)and bicarbonate(HCO_(3)-)are considered in the CO_(2)+O_(2) ISL reactive transport model of a typical sandstone-hosted uranium ore deposit in northern China.The reactive leaching of uranium is most sensitive to the spatial distribution of the mineralogical properties of the uranium deposit.Stochastic geostatistical models are used to represent the uncertainty on the spatial distribution of mineral grades.A Monte Carlo analysis was also performed to simulate the uranium production variability over an entire set of geostatistical realizations.The ISL stochastic simulation performed with the selected geostatistical realizations approximates the uranium production variability well.The simulation results of the ISL reactive transport model show that the extent of the uranium plume is highly dependent on mineralogical heterogeneity.The uncertainty analysis suggests the effect of uranium grade heterogeneity was found to be important to improve the accurate capture of the uncertainty.This study provides guidance for the accurate simulation and dynamic regulation of the CO_(2)+O_(2) leaching process of uranium at the scale of large mining areas.
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by the National Natural Science Foundation of China(No.51976138)National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019A10).
文摘A three-dimensional multicomponent multiphase lattice Boltzmann model(LBM)is established to model the coupled two-phase and reactive transport phenomena in the cathode electrode of proton exchange membrane fuel cells.The gas diff usion layer(GDL)and microporous layer(MPL)are stochastically reconstructed with the inside dynamic distribution of oxygen and liquid water resolved,and the catalyst layer is simplifi ed as a superthin layer to address the electrochemical reaction,which provides a clear description of the fl ooding eff ect on mass transport and performance.Diff erent kinds of electrodes are reconstructed to determine the optimum porosity and structure design of the GDL and MPL by comparing the transport resistance and per-formance under the fl ooding condition.The simulation results show that gradient porosity GDL helps to increase the reactive area and average concentration under fl ooding.The presence of the MPL ensures the oxygen transport space and reaction area because liquid water cannot transport through micropores.Moreover,the MPL helps in the uniform distribution of oxygen for an effi cient in-plane transport capacity.Crack and perforation structures can accelerate the water transport in the assembly.The systematic perforation design yields the best performance under fl ooding by separating the transport of liquid water and oxygen.
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.
基金supported by the National Key Research and Development Program of China(2022YFA1503501)the National Natural Science Foundation of China(22378112,22278127,and 22078088)+1 种基金the Fundamental Research Funds for the Central Universities(2022ZFJH004)the Shanghai Rising-Star Program(21QA1401900).
文摘Reactive transport equations in porous media are critical in various scientific and engineering disciplines,but solving these equations can be computationally expensive when exploring different scenarios,such as varying porous structures and initial or boundary conditions.The deep operator network(DeepONet)has emerged as a popular deep learning framework for solving parametric partial differential equations.However,applying the DeepONet to porous media presents significant challenges due to its limited capability to extract representative features from intricate structures.To address this issue,we propose the Porous-DeepONet,a simple yet highly effective extension of the DeepONet framework that leverages convolutional neural networks(CNNs)to learn the solution operators of parametric reactive transport equations in porous media.By incorporating CNNs,we can effectively capture the intricate features of porous media,enabling accurate and efficient learning of the solution operators.We demonstrate the effectiveness of the Porous-DeepONet in accurately and rapidly learning the solution operators of parametric reactive transport equations with various boundary conditions,multiple phases,and multiphysical fields through five examples.This approach offers significant computational savings,potentially reducing the computation time by 50–1000 times compared with the finite-element method.Our work may provide a robust alternative for solving parametric reactive transport equations in porous media,paving the way for exploring complex phenomena in porous media.
文摘Acid mine drainage（AMD） is commonly treated by neutralization with alkaline substances.This treatment is supported by titration experiments that illustrate the buffering mechanisms and estimate the base neutralization capacity（BNC） of the AMD.Detailed explanation of titration curves requires modeling with a hydro-chemical model.In this study the titration curves of water samples from the drainage of the As Pontes mine and the corresponding dumps have been investigated and six buffers are selerted by analyzing those curves.Titration curves have been simulated by a reactive transport model to discover the detailed buffering mechanisms.These simulations show seven regions involving different buffering mechanism.The BNC is primarily from buffers of dissolved Fe,Al and hydrogen sulfate.The BNC can be approximated by：BNC = 3（C_（Fe） ＋ C_（Al）） ＋ 0.05C_（sulfate）,where the units are mol/L.The BNC of the sample from the mine is 9.25×10^（-3） mol/L and that of the dumps sample is 1.28×10^（-2） mol/L
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supported by the National Key R&D Program of China(Grant No.2023YFC3209700)the National Natural Science Foundation of China(Grant Nos.41807194,41902263,41807208).
文摘Earthquake-related hydrochemical changes in thermal springs have been widely observed;however,quantitative modeling of the reactive transport process is absent.In the present study,we apply reactive transport simulation to capture the hydrochemical responses in a thermal spring following the Wenchuan Ms 8.0 and Lushan Ms 7.0 earthquakes.We first constrain deep reservoir geothermal fluid compositions and temperature by multicomponent geothermometry,and then a reactive geochemical transport model is constructed to reproduce the hydrochemical evolution process.The results show that the recharge from the shallow aquifer increases gradually until it reaches a peak because of the permeability enhancement caused by the Lushan earthquake,which may be the mechanism to explain the earthquake-related hydrochemical responses.In contrast to the postseismic effect of the Wenchuan earthquake,the chemical evolution can be considered as hydrochemical anomalies related to the Lushan earthquake.This study proves that the efficient simulation of reactive transport processes is useful for investigating earthquake-related signals in hydrochemical time series.
基金supported by the National Natural Science Foundation of China(Grant Nos.41372245,41272251)
文摘The overestimation of the contaminant concentration is a main issue in simulating the reactive transport using the common advection-dispersion-reaction equation （ADRE）. To solve this problem, a new modeling method is developed. The parameters of the model are identified based on experimental data. The results of the model are compared with previous results in the literature, and the sensitivity of the model is analyzed by examining the model＇s response to changes of the model parameters. Main conclusions are as follows： （1） The numerical modeling approach is feasible with an improved simulating accuracy. The predicted values are in agreement with the experimental measurements. The relative errors of the peak concentration between the simulated and experimental values are less than 2.5%. The errors are greatly reduced as compared with the results （about 67.8% as the maximum） based on a traditional ADRE in the literature. （2） There are three parameters （m, β0 and D ） which can be calibrated on the basis of experimental data in the model. The reactive product concentrations are mainly influenced by the parameters involved in the reactive ratio such as m and β0 The hydrodynamic dispersion coefficient D has almost no influence on the reactive product transport. （3） Our model does not provide better fitting curves for the ＂early arrival＂ and the ＂long tail＂. The ＂early arrival＂ and the ＂long tail＂ are associated with low values of the product AB. Under these conditions, the reaction rate is close to 0, and the model of the ADRE reduces to the advection-dispersion equation （ADE）. Further mechanism study is needed in the future.
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 National Natural Science Foundation of China (12105139 and 42277264)National Key Research and Development Program of China (2021YFC2902104)Education Department of Hunan Province (21B0446).
文摘Porosity,tortuosity,specific surface area(SSA),and permeability are four key parameters of reactive transport modeling in sandstone,which are important for understanding solute transport and geochemical reaction pro-cesses in sandstone aquifers.These four parameters reflect the characteristics of pore structure of sandstone from different perspectives,and the traditional empirical formulas cannot make accurate predictions of them due to their complexity and heterogeneity.In this paper,eleven types of sandstone CT images were firstly segmented into numerous subsample images,the porosity,tortuosity,SSA,and permeability of the subsamples were calculated,and the dataset was established.The 3D convolutional neural network(CNN)models were subse-quently established and trained to predict the key reactive transport parameters based on subsample CT images of sandstones.The results demonstrated that the 3D CNN model with multiple outputs exhibited excellent prediction ability for the four parameters compared to the traditional empirical formulas.In particular,for the prediction of tortuosity and permeability,the 3D CNN model with multiple outputs even showed slightly better prediction ability than its single-output variant model.Additionally,it demonstrated good generalization per-formance on sandstone CT images not included in the training dataset.The study showed that the 3D CNN model with multiple outputs has the advantages of simplifying operation and saving computational resources,which has the prospect of popularization and application.
基金The Joint Funds of the National Natural Science Foundation of China under contract Nos U22A20580 and U2106203the National Natural Science Foundation of China under contract No.41706067the Open Project Program of Key Laboratory of Ecological Warning,Protection&Restoration for Bohai Sea,Ministry of Natural Resources under contract No.2022108.
文摘Naturally occurring radium(^(223)Ra,^(224)Ra,^(226)Ra,and^(228)Ra)isotopes have been widely applied as geochemical tracers in marine environments,especially when estimating the submarine groundwater discharge(SGD).In this sense,the influencing factors and transport mechanism of radium isotope activity in aquifers can be key information for SGD estimation.This work evaluates the adsorption/desorption behavior of^(224)Ra and^(226)Ra in the solid-liquid phase through a leaching experiment and analysis of field data.The results suggested that radium isotope activity was positively correlated with salinity and grain size,in the case of abundant sediments.Through ion analysis,we found that the ions(Na^(+),Ca^(2+),Mg^(2+),and Ba^(2+))exchanged with radium isotopes in the process of transport.A 1-D reactive transport model was established to simulate the transport process of radium isotope in aquifers.The model successfully simulated the variation of radium isotope desorption activity with salinity and was subsequently verified in the field.This study contributes to the understanding of the geochemical behavior of radium isotopes in aquifers and provides guidance for selecting a suitable groundwater endmember in SGD estimation.
基金jointly supported by the National Key R&D Program of China(No.2018YFB1501802)the National Natural Science Foundation of China(No.41902309)funded by the Engineering Research Center of Geothermal Resources Development Technology and Equipment,Ministry of Education,Jilin University。
文摘The Enhanced Geothermal System(EGS) is an artificial geothermal system that aims to economically extract heat from hot dry rock(HDR) through the creation of an artificial geothermal reservoir. Chemical stimulation is thought to be an effective method to create fracture networks and open existing fractures in hot dry rocks by injecting chemical agents into the reservoir to dissolve the minerals. Granite is a common type of hot dry rock. In this paper, a series of chemical stimulation experiments were implemented using acid and alkaline agents under high temperature and pressure conditions that mimic the environment of formation. Granite rock samples used in the experiments are collected from the potential EGS reservoir in the Matouying area, Hebei, China. Laboratory experimental results show that the corrosion ratio per unit area of rock is 3.2% in static acid chemical experiments and 0.51% in static alkaline chemical experiments. The permeability of the core is increased by 1.62 times in dynamic acid chemical experiments and 2.45 times in dynamic alkaline chemical experiments. A scanning electron microscope analysis of the core illustrates that secondary minerals, such as chlorite, spherical silica, and montmorillonite, were formed, due to acid-rock interaction with plagioclase being precipitated by alkaline-rock interactions. Masking agents in alkaline chemical agents can slightly reduce the degree of plagioclase formation. A chemical simulation model was built using TOUGHREACT, the mineral dissolution and associated ion concentration variation being reproduced by this reactive transport model.
文摘Dissolution of fluorite(CaF2)and/or fluorapatite(FAP)[Cas(PO4)3F],pulled by calcite precipitation,is thought to be the dominant mechanism responsible for groundwater fluoride(F)contamination.Here,one dimensional reactive-transport models are developed to test this mechanism using the published dissolution and precipitation rate kinetics for the mineral pair FAP and calcite.Simulation results correctly show positive correlation between the aqueous concentrations of F and CO_(2)and negative correlation between F-and Ca^2+.Results also show that precipitation of calcite,contrary to the present understanding,slows down the FAP dissolution by 10G orders of magnitude compared to the FAP dissolution by hydrolysis.For appreciable amount of fluoride contamination rock-water interaction time must be long and of order 106 years.
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.
基金the funding support from the Ministry of Education,Government of India,under the Prime Minister Research Fellowship programme(Grant Nos.SB21221901CEPMRF008347 and SB22230217CEPMRF008347).
文摘Geomaterials with inferior hydraulic and strength characteristics often need improvement to enhance their engineering behaviors.Traditional ground improvement techniques require enormous mechanical effort or synthetic chemicals.Sustainable stabilization technique such as microbially induced calcite precipitation(MICP)utilizes bacterial metabolic processes to precipitate cementitious calcium carbonate.The reactive transport of biochemical species in the soil mass initiates the precipitation of biocement during the MICP process.The precipitated biocement alters the hydro-mechanical performance of the soil mass.Usually,the flow,deformation,and transport phenomena regulate the biocementation technique via coupled bio-chemo-hydro-mechanical(BCHM)processes.Among all,one crucial phenomenon controlling the precipitation mechanism is the encapsulation of biomass by calcium carbonate.Biomass encapsulation can potentially reduce the biochemical reaction rate and decelerate biocementation.Laboratory examination of the encapsulation process demands a thorough analysis of associated coupled effects.Despite this,a numerical model can assist in capturing the coupled processes influencing encapsulation during the MICP treatment.However,most numerical models did not consider biochemical reaction rate kinetics accounting for the influence of bacterial encapsulation.Given this,the current study developed a coupled BCHM model to evaluate the effect of encapsulation on the precipitated calcite content using a micro-scale semiempirical relationship.Firstly,the developed BCHM model was verified and validated using numerical and experimental observations of soil column tests.Later,the encapsulation phenomenon was investigated in the soil columns of variable maximum calcite crystal sizes.The results depict altered reaction rates due to the encapsulation phenomenon and an observable change in the precipitated calcite content for each maximum crystal size.Furthermore,the permeability and deformation of the soil mass were affected by the simultaneous precipitation of calcium carbonate.Overall,the present study comprehended the influence of the encapsulation of bacteria on cement morphology-induced permeability,biocement-induced stresses and displacements.
文摘The purpose of this paper is to analyze some features of contaminant flow passing through cracked porous medium,such as the influence of fracture network on the advection and diffusion of contaminant species,the impact of adsorption on the overall transport of contaminant wastes.In order to precisely describe the whole process,we firstly build the mathematical model to simulate this problem numerically.Taking into consideration of the characteristics of contaminant flow,we employ two partial differential equations to formulate the whole problem.One is flow equation;the other is reactive transport equation.The first equation is used to describe the total flow of contaminant wastes,which is based on Darcy law.The second one will characterize the adsorption,diffusion and convection behavior of contaminant species,which describes most features of contaminant flow we are interested in.After the construction of numerical model,we apply locally conservative and compatible algorithms to solve this mathematical model.Specifically,we apply Mixed Finite Element(MFE)method to the flow equation and Discontinuous Galerkin(DG)method for the transport equation.MFE has a good convergence rate and numerical accuracy for Darcy velocity.DG is more flexible and can be used to deal with irregular meshes,as well as little numerical diffusion.With these two numerical means,we investigate the sensitivity analysis of different features of contaminant flow in our model,such as diffusion,permeability and fracture density.In particular,we study Kd values which represent the distribution of contaminant wastes between the solid and liquid phases.We also make omparisons of two different schemes and discuss the advantages of both methods.
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 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.
