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1.
Carbon dioxide (CO2) has been injected in the subsurface permeable formations as a means to cut atmospheric CO2 emissions and/or enhance oil recovery (EOR). It is important to constrain the boundaries of the CO2 plume in the target formation and/or other formations hosting the CO2 migrated from the target formation. Monitoring methods and technologies to assess the CO2 plume boundaries over time within a reservoir of interest are required. Previously introduced methods and technologies on pressure monitoring to detect the extent of the CO2 plume require at least two wells, i.e. pulser and observation wells. We introduce pressure transient technique requiring single well only. Single well pressure transient testing (drawdown/buildup/injection/falloff) is widely used to determine reservoir properties and wellbore conditions. Pressure diagnostic plots are used to identify different flow regimes and determine the reservoir/well characteristics. We propose a method to determine the plume extent for a constant rate pressure transient test at a single well outside the CO2 plume. Due to the significant contrast between mobility and storativity of the CO2 and native fluids (oil or brine), the CO2 boundary causes deviation in the pressure diagnostic response from that corresponding to previously identified heterogeneities. Using the superposition principle, we develop a relationship between the deviation time and the plume boundary. We demonstrate the applicability of the proposed method using numerically generated synthetic data corresponding to homogeneous, heterogeneous, and anisotropic cases to evaluate its potential and limitations. We discuss ways to identify and overcome the potential limitations for application of the method in the field.  相似文献   

2.
A screening and ranking framework (SRF) has been developed to evaluate potential geologic carbon dioxide (CO2) storage sites on the basis of health, safety, and environmental (HSE) risk arising from CO2 leakage. The approach is based on the assumption that CO2 leakage risk is dependent on three basic characteristics of a geologic CO2 storage site: (1) the potential for primary containment by the target formation; (2) the potential for secondary containment if the primary formation leaks; and (3) the potential for attenuation and dispersion of leaking CO2 if the primary formation leaks and secondary containment fails. The framework is implemented in a spreadsheet in which users enter numerical scores representing expert opinions or published information along with estimates of uncertainty. Applications to three sites in California demonstrate the approach. Refinements and extensions are possible through the use of more detailed data or model results in place of property proxies.  相似文献   

3.
The utilization of anthropogenic CO2 for enhanced oil recovery (EOR) can significantly extend the production life of an oil field, and help in the reduction of atmospheric emission of anthropogenic CO2 if sequestration is considered. This work summarizes the prospect of EOR and sequestration using CO2 flooding from an Indian mature oil field at Cambay basin through numerical modelling, simulation and pressure study based on limited data provided by the operator. To get an insight into CO2-EOR and safe storage process in this oil field, a conceptual sector model is developed and screening standard is proposed keeping in mind the major pay zone of the producing reservoir. To construct the geomodel, depth maps, well positions and coordinates, well data and well logs, perforation depths and distribution of petrophysical properties as well as fluid properties provided by the operator, has been considered. Based on the results from the present study, we identified that the reservoir has the potential for safe and economic geological sequestration of 15.04×106 metric ton CO2 in conjunction with a substantial increase in oil recovery of 10.4% of original oil in place. CO2-EOR and storage in this mature field has a bright application prospect since the findings of the present work could be a better input to manage the reservoir productivity, and the pressure field for significant enhancement of oil recovery followed by safe storage.  相似文献   

4.
CO2 geological storage is a transitional technology for the mitigation of climate change. In the vicinity of potential CO2 reservoirs in Hungary, protected freshwater aquifers used for drinking water supplies exist. Effects of disaster events of CO2 escape and brine displacement to one of these aquifers have been studied by kinetic 1D reactive transport modelling in PHREEQC. Besides verifying that ion concentrations in the freshwater may increase up to drinking water limit values in both scenarios (CO2 or brine leakage), total porosity of the rock is estimated. Pore volume is expected to increase at the entry point of CO2 and to decrease at further distances, whereas it shows minor increase along the flow path for the effect of brine inflow. Additionally, electrical conductivity of water is estimated and suggested to be the best parameter to measure for cost-effective monitoring of both worst-case leakage scenarios.  相似文献   

5.
CO2 storage in geological formations is currently being discussed intensively as a technology with a high potential for mitigating CO2 emissions. However, any large-scale application requires a thorough analysis of the potential risks. Current numerical simulation models are too expensive for probabilistic risk analysis or stochastic approaches based on a brute-force approach of repeated simulation. Even single deterministic simulations may require parallel high-performance computing. The multiphase flow processes involved are too non-linear for quasi-linear error propagation and other simplified stochastic tools. As an alternative approach, we propose a massive stochastic model reduction based on the probabilistic collocation method. The model response is projected onto a higher-order orthogonal basis of polynomials to approximate dependence on uncertain parameters (porosity, permeability, etc.) and design parameters (injection rate, depth, etc.). This allows for a non-linear propagation of model uncertainty affecting the predicted risk, ensures fast computation, and provides a powerful tool for combining design variables and uncertain variables into one approach based on an integrative response surface. Thus, the design task of finding optimal injection regimes explicitly includes uncertainty, which leads to robust designs with a minimum failure probability. We validate our proposed stochastic approach by Monte Carlo simulation using a common 3D benchmark problem (Class et al., Comput Geosci 13:451–467, 2009). A reasonable compromise between computational efforts and precision was reached already with second-order polynomials. In our case study, the proposed approach yields a significant computational speed-up by a factor of 100 compared with the Monte Carlo evaluation. We demonstrate that, due to the non-linearity of the flow and transport processes during CO2 injection, including uncertainty in the analysis leads to a systematic and significant shift of the predicted leakage rates toward higher values compared with deterministic simulations, affecting both risk estimates and the design of injection scenarios.  相似文献   

6.
Careful site characterization is critical for successful geologic storage of carbon dioxide (CO2) because of the many physical and chemical processes impacting CO2 movement and containment under field conditions. Traditional site characterization techniques such as geological mapping, geophysical imaging, well logging, core analyses, and hydraulic well testing provide the basis for judging whether or not a site is suitable for CO2 storage. However, only through the injection and monitoring of CO2 itself can the coupling between buoyancy flow, geologic heterogeneity, and history-dependent multi-phase flow effects be observed and quantified. CO2 injection and monitoring can therefore provide a valuable addition to the site-characterization process. Additionally, careful monitoring and verification of CO2 plume development during the early stages of commercial operation should be performed to assess storage potential and demonstrate permanence. The Frio brine pilot, a research project located in Dayton, Texas (USA) is used as a case study to illustrate the concept of an iterative sequence in which traditional site characterization is used to prepare for CO2 injection and then CO2 injection itself is used to further site-characterization efforts, constrain geologic storage potential, and validate understanding of geochemical and hydrological processes. At the Frio brine pilot, in addition to traditional site-characterization techniques, CO2 movement in the subsurface is monitored by sampling fluid at an observation well, running CO2-saturation-sensitive well logs periodically in both injection and observation wells, imaging with crosswell seismic in the plane between the injection and observation wells, and obtaining vertical seismic profiles to monitor the CO2 plume as it migrates beyond the immediate vicinity of the wells. Numerical modeling plays a central role in integrating geological, geophysical, and hydrological field observations.  相似文献   

7.
One of the uncertainties in the field of carbon dioxide capture and storage (CCS) is caused by the parameterization of geochemical models. The application of geochemical models contributes significantly to calculate the fate of the CO2 after its injection. The choice of the thermodynamic database used, the selection of the secondary mineral assemblage as well as the option to calculate pressure dependent equilibrium constants influence the CO2 trapping potential and trapping mechanism. Scenario analyses were conducted applying a geochemical batch equilibrium model for a virtual CO2 injection into a saline Keuper aquifer. The amount of CO2 which could be trapped in the formation water and in the form of carbonates was calculated using the model code PHREEQC. Thereby, four thermodynamic datasets were used to calculate the thermodynamic equilibria. Furthermore, the equilibrium constants were re-calculated with the code SUPCRT92, which also applied a pressure correction to the equilibrium constants. Varying the thermodynamic database caused a range of 61% in the amount of trapped CO2 calculated. Simultaneously, the assemblage of secondary minerals was varied, and the potential secondary minerals dawsonite and K-mica were included in several scenarios. The selection of the secondary mineral assemblage caused a range of 74% in the calculated amount of trapped CO2. Correcting the equilibrium constants with respect to a pressure of 125 bars had an influence of 11% on the amount of trapped CO2. This illustrates the need for incorporating sensitivity analyses into reaction pathway modeling.  相似文献   

8.
Simulation of carbon dioxide (CO2) at hourly/weekly intervals and fine vertical resolution at the continental or coastal sites is challenging because of coarse horizontal resolution of global transport models. Here the regional Weather Research and Forecasting (WRF) model coupled with atmospheric chemistry is adopted for simulating atmospheric CO2 (hereinafter WRF-CO2) in nonreactive chemical tracer mode. Model results at horizontal resolution of 27 × 27 km and 31 vertical levels are compared with hourly CO2 measurements from Tsukuba, Japan (36.05°N, 140.13 oE) at tower heights of 25 and 200 m for the entire year 2002. Using the wind rose analysis, we find that the fossil fuel emission signal from the megacity Tokyo dominates the diurnal, synoptic and seasonal variations observed at Tsukuba. Contribution of terrestrial biosphere fluxes is of secondary importance for CO2 concentration variability. The phase of synoptic scale variability in CO2 at both heights are remarkably well simulated the observed data (correlation coefficient >0.70) for the entire year. The simulations of monthly mean diurnal cycles are in better agreement with the measurements at lower height compared to that at the upper height. The modelled vertical CO2 gradients are generally greater than the observed vertical gradient. Sensitivity studies show that the simulation of observed vertical gradient can be improved by increasing the number of vertical levels from 31 in the model WRF to 37 (4 below 200 m) and using the Mellor–Yamada–Janjic planetary boundary scheme. These results have large implications for improving transport model simulation of CO2 over the continental sites.  相似文献   

9.
The CO2 migrated from deeper to shallower layers may change its phase state from supercritical state to gaseous state (called phase transition). This phase transition makes both viscosity and density of CO2 experience a sharp variation, which may induce the CO2 further penetration into shallow layers. This is a critical and dangerous situation for the security of CO2 geological storage. However, the assessment of caprock sealing efficiency with a fully coupled multi-physical model is still missing on this phase transition effect. This study extends our previous fully coupled multi-physical model to include this phase transition effect. The dramatic changes of CO2 viscosity and density are incorporated into the model. The impacts of temperature and pressure on caprock sealing efficiency (expressed by CO2 penetration depth) are then numerically investigated for a caprock layer at the depth of 800 m. The changes of CO2 physical properties with gas partial pressure and formation temperature in the phase transition zone are explored. It is observed that phase transition revises the linear relationship of CO2 penetration depth and time square root as well as penetration depth. The real physical properties of CO2 in the phase transition zone are critical to the safety of CO2 sequestration. Pressure and temperature have different impact mechanisms on the security of CO2 geological storage.  相似文献   

10.
We present a two-step stochastic inversion approach for monitoring the distribution of CO2 injected into deep saline aquifers for the typical scenario of one single injection well and a database comprising a common suite of well logs as well as time-lapse vertical seismic profiling (VSP) data. In the first step, we compute several sets of stochastic models of the elastic properties using conventional sequential Gaussian co-simulations (SGCS) representing the considered reservoir before CO2 injection. All realizations within a set of models are then iteratively combined using a modified gradual deformation algorithm aiming at reducing the mismatch between the observed and simulated VSP data. In the second step, these optimal static models then serve as input for a history matching approach using the same modified gradual deformation algorithm for minimizing the mismatch between the observed and simulated VSP data following the injection of CO2. At each gradual deformation step, the injection and migration of CO2 is simulated and the corresponding seismic traces are computed and compared with the observed ones. The proposed stochastic inversion approach has been tested for a realistic, and arguably particularly challenging, synthetic case study mimicking the geological environment of a potential CO2 injection site in the Cambrian-Ordivician sedimentary sequence of the St. Lawrence platform in Southern Québec. The results demonstrate that the proposed two-step reservoir characterization approach is capable of adequately resolving and monitoring the distribution of the injected CO2. This finds its expression in optimized models of P- and S-wave velocities, density, and porosity, which, compared to conventional stochastic reservoir models, exhibit a significantly improved structural similarity with regard to the corresponding reference models. The proposed approach is therefore expected to allow for an optimal injection forecast by using a quantitative assimilation of all available data from the appraisal stage of a CO2 injection site.  相似文献   

11.
A new uncertainty quantification framework is adopted for carbon sequestration to evaluate the effect of spatial heterogeneity of reservoir permeability on CO2 migration. Sequential Gaussian simulation is used to generate multiple realizations of permeability fields with various spatial statistical attributes. In order to deal with the computational difficulties, the following ideas/approaches are integrated. First, different efficient sampling approaches (probabilistic collocation, quasi-Monte Carlo, and adaptive sampling) are used to reduce the number of forward calculations, explore effectively the parameter space, and quantify the input uncertainty. Second, a scalable numerical simulator, extreme-scale Subsurface Transport Over Multiple Phases, is adopted as the forward modeling simulator for CO2 migration. The framework has the capability to quantify input uncertainty, generate exploratory samples effectively, perform scalable numerical simulations, visualize output uncertainty, and evaluate input-output relationships. The framework is demonstrated with a given CO2 injection scenario in heterogeneous sandstone reservoirs. Results show that geostatistical parameters for permeability have different impacts on CO2 plume radius: the mean parameter has positive effects at the top layers, but affects the bottom layers negatively. The variance generally has a positive effect on the plume radius at all layers, particularly at middle layers, where the transport of CO2 is highly influenced by the subsurface heterogeneity structure. The anisotropy ratio has weak impacts on the plume radius, but affects the shape of the CO2 plume.  相似文献   

12.
A field facility located in Bozeman, Montana provides the opportunity to test methods to detect, locate, and quantify potential CO2 leakage from geologic storage sites. From 9 July to 7 August 2008, 0.3 t CO2 day−1 were injected from a 100-m long, ~2.5-m deep horizontal well. Repeated measurements of soil CO2 fluxes on a grid characterized the spatio-temporal evolution of the surface leakage signal and quantified the surface leakage rate. Infrared CO2 concentration sensors installed in the soil at 30 cm depth at 0–10 m from the well and at 4 cm above the ground at 0 and 5 m from the well recorded surface breakthrough of CO2 leakage and migration of CO2 leakage through the soil. Temporal variations in CO2 concentrations were correlated with atmospheric and soil temperature, wind speed, atmospheric pressure, rainfall, and CO2 injection rate.  相似文献   

13.
Modeling geological carbon storage represents a new and substantial challenge for the subsurface geosciences. To increase understanding and make good engineering decisions, containment processes and large-scale storage operations must be simulated in a thousand-year perspective. Large differences in spatial and temporal scales make it prohibitively expensive to compute the fate of injected CO2 using traditional 3D simulators. Instead, accurate forecast can be computed using simplified models that are adapted to the specific setting of the bouyancy-driven migration of the light fluid phase. This paper presents a family of vertically integrated models for studying the combined large-scale and long-term effects of structural, residual, and solubility trapping of CO2. The models are based on an assumption of a sharp interface separating CO2 and brine and can provide a detailed inventory of the injected CO2 volumes over periods of thousands of years within reasonable computational time. To be compatible with simulation tools used in industry, the models are formulated in a black-oil framework. The models are implemented in MRST-co2lab, which is an open community software developed especially to study and optimize large-scale, long-term geological storage of CO2. The resulting simulators are fully implicit and handle input from standard geomodeling tools.  相似文献   

14.
A numerical model was developed to investigate the potential to detect fluid migration in a (homogeneous, isotropic, with constant pressure lateral boundaries) porous and permeable interval overlying an imperfect primary seal of a geologic CO2 storage formation. The seal imperfection was modeled as a single higher-permeability zone in an otherwise low-permeability seal, with the center of that zone offset from the CO2 injection well by 1400 m. Pressure response resulting from fluid migration through the high-permeability zone was detectable up to 1650 m from the centroid of that zone at the base of the monitored interval after 30 years of CO2 injection (detection limit = 0.1 MPa pressure increase); no pressure response was detectable at the top of the monitored interval at the same point in time. CO2 saturation response could be up to 774 m from the center of the high-permeability zone at the bottom of the monitored interval, and 1103 m at the top (saturation detection limit = 0.01). More than 6% of the injected CO2, by mass, migrated out of primary containment after 130 years of site performance (including 30 years of active injection) in the case where the zone of seal imperfection had a moderately high permeability (10??17 m2 or 0.01 mD). Free-phase CO2 saturation monitoring at the top of the overlying interval provides favorable spatial coverage for detecting fluid migration across the primary seal. Improved sensitivity of detection for pressure perturbation will benefit time of detection above an imperfect seal.  相似文献   

15.
After more than a decade of multidisciplinary studies of the Central American subduction zone mainly in the framework of two large research programmes, the US MARGINS program and the German Collaborative Research Center SFB 574, we here review and interpret the data pertinent to quantify the cycling of mineral-bound volatiles (H2O, CO2, Cl, S) through this subduction system. For input-flux calculations, we divide the Middle America Trench into four segments differing in convergence rate and slab lithological profiles, use the latest evidence for mantle serpentinization of the Cocos slab approaching the trench, and for the first time explicitly include subduction erosion of forearc basement. Resulting input fluxes are 40–62 (53) Tg/Ma/m H2O, 7.8–11.4 (9.3) Tg/Ma/m CO2, 1.3–1.9 (1.6) Tg/Ma/m Cl, and 1.3–2.1 (1.6) Tg/Ma/m S (bracketed are mean values for entire trench length). Output by cold seeps on the forearc amounts to 0.625–1.25 Tg/Ma/m H2O partly derived from the slab sediments as determined by geochemical analyses of fluids and carbonates. The major volatile output occurs at the Central American volcanic arc that is divided into ten arc segments by dextral strike-slip tectonics. Based on volcanic edifice and widespread tephra volumes as well as calculated parental magma masses needed to form observed evolved compositions, we determine long-term (105 years) average magma and K2O fluxes for each of the ten segments as 32–242 (106) Tg/Ma/m magma and 0.28–2.91 (1.38) Tg/Ma/m K2O (bracketed are mean values for entire Central American volcanic arc length). Volatile/K2O concentration ratios derived from melt inclusion analyses and petrologic modelling then allow to calculate volatile fluxes as 1.02–14.3 (6.2) Tg/Ma/m H2O, 0.02–0.45 (0.17) Tg/Ma/m CO2, and 0.07–0.34 (0.22) Tg/Ma/m Cl. The same approach yields long-term sulfur fluxes of 0.12–1.08 (0.54) Tg/Ma/m while present-day open-vent SO2-flux monitoring yields 0.06–2.37 (0.83) Tg/Ma/m S. Input–output comparisons show that the arc water fluxes only account for up to 40 % of the input even if we include an “invisible” plutonic component constrained by crustal growth. With 20–30 % of the H2O input transferred into the deeper mantle as suggested by petrologic modeling, there remains a deficiency of, say, 30–40 % in the water budget. At least some of this water is transferred into two upper-plate regions of low seismic velocity and electrical resistivity whose sizes vary along arc: one region widely envelopes the melt ascent paths from slab top to arc and the other extends obliquely from the slab below the forearc to below the arc. Whether these reservoirs are transient or steady remains unknown.  相似文献   

16.
Proper characterizations of background soil CO2 respiration rates are critical for interpreting CO2 leakage monitoring results at geologic sequestration sites. In this paper, a method is developed for determining temperature-dependent critical values of soil CO2 flux for preliminary leak detection inference. The method is illustrated using surface CO2 flux measurements obtained from the AmeriFlux network fit with alternative models for the soil CO2 flux versus soil temperature relationship. The models are fit first to determine pooled parameter estimates across the sites, then using a Bayesian hierarchical method to obtain both global and site-specific parameter estimates. Model comparisons are made using the deviance information criterion (DIC), which considers both goodness of fit and model complexity. The hierarchical models consistently outperform the corresponding pooled models, demonstrating the need for site-specific data and estimates when determining relationships for background soil respiration. A hierarchical model that relates the square root of the CO2 flux to a quadratic function of soil temperature is found to provide the best fit for the AmeriFlux sites among the models tested. This model also yields effective prediction intervals, consistent with the upper envelope of the flux data across the modeled sites and temperature ranges. Calculation of upper prediction intervals using the proposed method can provide a basis for setting critical values in CO2 leak detection monitoring at sequestration sites.  相似文献   

17.
In this paper, we focus on the geological storage of CO2 in reservoirs with zones that are cold enough to facilitate CO2 hydrate formation at local pressures. A 2D hydro-chemical mechanical model which has five layers (three layers with aquifers and two layers with cap rock in which we introduced two fractures) is created. We apply a reactive transport reservoir simulator, RetrasoCodeBright (RCB), in which hydrate is treated as a pseudo mineral. Following the recent modifications to account for hydrate dynamics in the code through a kinetic approach (Kvamme et al., Proceedings of the 7th International Conference on Gas Hydrates (ICGH 2011), 2011b), we have further improved the simulator to implement the nonequilibrium thermodynamic calculations. In the present study, we spot the light on the hydrate formation effects on porosity in different regions, as well as on the flow pattern. These simulations are based on classical relationships between porosity and permeability, but the outline of ongoing modifications is presented as well. A critical question in such systems is whether hydrate formation can contribute to stabilizing the storage, given that hydrates are pore filling and cannot be stable toward mineral surfaces. The implications of hydrate formation on the geo-mechanical properties of the model reservoir are other aspects addressed in this study.  相似文献   

18.
The efficiency and sustainability of carbon dioxide (CO2) storage in deep geological formations crucially depends on the integrity of the overlying cap-rocks. Existing oil and gas wells, which penetrate the formations, are potential leakage pathways. This problem has been discussed in the literature, and a number of investigations using semi-analytical mathematical approaches have been carried out by other authors to quantify leakage rates. The semi-analytical results are based on a number of simplifying assumptions. Thus, it is of great interest to assess the influence of these assumptions. We use a numerical model to compare the results with those of the semi-analytical model. Then we ease the simplifying restrictions and include more complex thermodynamic processes including sub- and supercritical fluid properties of CO2 and non-isothermal as well as compositional effects. The aim is to set up problem-oriented benchmark examples that allow a comparison of different modeling approaches to the problem of CO2 leakage.  相似文献   

19.
In the last few decades of industrialization, the concentration of CO2 in the atmosphere had increased rapidly. Different organizations have invested considerable funds in research activities worldwide for CO2 capture and storage. To date, significant work has been done and various technologies have been proposed for CO2 capture and storage. Both adsorption and absorption are promising techniques for CO2 capture, but low-temperature adsorption processes using solid adsorbents are the prevailing technique nowadays. In this review paper, a variety of adsorbents such as carbonaceous materials, dry alkali metal-based sorbents, zeolites, metal–organic frameworks (MOFs) and microporous organic polymers (MOPs) have been studied. Various methods of chemical or physical modification and the effects of supporting materials have been discussed to enhance CO2 capture capacity of these adsorbents. Low-temperature (<100 °C) adsorption processes for CO2 capture are critically analyzed and concluded on the basis of information available so far in the literature. All the information in CO2 adsorption using different routes has been discussed, summarized and thoroughly presented in this review article. The most important comparative study of relatively new material MOFs and MOPs is carried out between the groups and with other sorbent as well.  相似文献   

20.
Deep saline aquifers in sedimentary basins are considered to have the greatest potential for CO2 geological storage in order to reduce carbon emissions. CO2 injected into a saline sandstone aquifer tends to migrate upwards toward the caprock because the density of the supercritical CO2 phase is lower than that of formation water. The accumulated CO2 in the upper portions of the reservoir gradually dissolves into brine, lowers pH and changes the aqueous complexation, whereby induces mineral alteration. In turn, the mineralogical composition could impose significant effects on the evolution of solution, further on the mineralized CO2. The high density of aqueous phase will then move downward due to gravity, give rise to “convective mixing,” which facilitate the transformation of CO2 from the supercritical phase to the aqueous phase and then to the solid phase. In order to determine the impacts of mineralogical compositions on trapping amounts in different mechanisms for CO2 geological storage, a 2D radial model was developed. The mineralogical composition for the base case was taken from a deep saline formation of the Ordos Basin, China. Three additional models with varying mineralogical compositions were carried out. Results indicate that the mineralogical composition had very obvious effects on different CO2 trapping mechanisms. Specific to our cases, the dissolution of chlorite provided Mg2+ and Fe2+ for the formation of secondary carbonate minerals (ankerite, siderite and magnesite). When chlorite was absent in the saline aquifer, the dominant secondary carbon sequestration mineral was dawsonite, and the amount of CO2 mineral trapping increased with an increase in the concentration of chlorite. After 3000 years, 69.08, 76.93, 83.52 and 87.24 % of the injected CO2 can be trapped in the solid (mineral) phase, 16.05, 11.86, 8.82 and 6.99 % in the aqueous phase, and 14.87, 11.21, 7.66 and 5.77 % in the gas phase for Case 1 through 4, respectively.  相似文献   

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