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1.
Geological storage of carbon dioxide (CO2) is a promising technology for reducing atmospheric emissions. The large discrepancy in the time- and length-scales between up-dip migration of buoyant supercritical CO2 and the sinking fingers of dissolved CO2 poses a challenge for numerical simulations aimed at describing the fate of the plume. Hence, several investigators have suggested methods to simplify the problem, but to date there has been no reference solution with which these simplified models can be compared. We investigate the full problem of Darcy-based two-phase flow with gravity-current propagation and miscible convective mixing, using high-resolution numerical simulations. We build on recent developments of the Automatic Differentiation - General Purpose Research Simulator (AD-GPRS) at Stanford. The results show a CO2 plume that travels for 5000 years reaching a final distance of 14 km up-dip from the injection site. It takes another 2000 years before the CO2 is completely trapped as residual (40%) and dissolved (60%) CO2. Dissolution causes a significant reduction of the plume speed. While fingers of dissolved CO2 appear under the propagating gravity current, the resident brine does not become fully saturated with CO2 anywhere under the plume. The overall mass transfer of CO2 into the brine under the plume remains practically constant for several thousands of years. These results can be used as a benchmark for verification, or improvements, of simplified (reduced-dimensionality, upscaled) models. Our results indicate that simplified models need to account for: (i) reduced dissolution due to interaction with the plume, and (ii) gradual reduction of the local dissolution rate after the fingers begin to interact with the bottom of the aquifer. 相似文献
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3.
Direct atmospheric greenhouse gas emissions can be greatly reduced by CO2 sequestration in deep saline aquifers. One of the most secure and important mechanisms of CO2 trapping over large time scales is solubility trapping. In addition, the CO2 dissolution rate is greatly enhanced if density-driven convective mixing occurs. We present a systematic analysis of the prerequisites for density-driven instability and convective mixing over the broad temperature, pressure, salinity and permeability conditions that are found in geological CO2 storage. The onset of instability (Rayleigh–Darcy number, Ra), the onset time of instability and the steady convective flux are comprehensively calculated using a newly developed analysis tool that accounts for the thermodynamic and salinity dependence on solutally and thermally induced density change, viscosity, molecular and thermal diffusivity. Additionally, the relative influences of field characteristics are analysed through local and global sensitivity analyses. The results help to elucidate the trends of the Ra, onset time of instability and steady convective flux under field conditions. The impacts of storage depth and basin type (geothermal gradient) are also explored and the conditions that favour or hinder enhanced solubility trapping are identified. Contrary to previous studies, we conclude that the geothermal gradient has a non-negligible effect on density-driven instability and convective mixing when considering both direct and indirect thermal effects because cold basin conditions, for instance, render higher Ra compared to warm basin conditions. We also show that the largest Ra is obtained for conditions that correspond to relatively shallow depths, measuring approximately 800 m, indicating that CO2 storage at such depths favours the onset of density-driven instability and reduces onset times. However, shallow depths do not necessarily provide conditions that generate the largest steady convective fluxes; the salinity determines the storage depth at which the largest steady convective fluxes occur. Furthermore, we present a straight-forward and efficient procedure to estimate site-specific solutal Ra that accounts for thermodynamic and salinity dependence. 相似文献
4.
The standard approach for geologic storage of CO2 consists of injecting it as a supercritical CO2 phase. This approach places stringent requirements on the caprock, which must display: (1) high entry pressure to prevent the buoyancy driven upwards escape of CO2; (2) low permeability to minimize the upwards flux of brine displaced by the CO2; and (3) high strength to ensure that pressure build up does not cause caprock failure. We propose an alternative approach for cases when the above requirements are not met. The approach consists of extracting brine from the storage formation and then re-injecting it so that it mixes with CO2 at depth in the injection well. Mixing at depth reduces the pressure required for brine and CO2 at the surface. This CO2-saturated brine will sink to the aquifer bottom because it is denser than resident brine, which eliminates the risk of buoyant escape of CO2. The method is particularly favorable when the aquifer dips, because CO2-saturated brine will tend to flow downslope. We perform two- and three-dimensional numerical simulations to study how far upslope the extraction well needs to be located to ensure a very long operation without CO2 ever breaking through. Several sets of simulations were carried out to evaluate the effect of slope, temperature, pressure and CO2 concentration, which is significantly reduced if flue gas (i.e., without capture) is mixed with the brine. We analyze energy requirements to find that the system requires high permeability to be viable, but its performance is improved by taking advantage of the thermal energy of the extracted brine. 相似文献
5.
Deep saline aquifers are one of the most suitable geologic formations for carbon sequestration. The linear and global stability analysis of the time-dependent density-driven convection in deep saline aquifers is presented for long-term storage of carbon dioxide (CO2). The convective mixing that can greatly accelerate the CO2 dissolution into saline aquifers arises because the density of brine increases upon the dissolution of CO2 and such a density difference may induce instability. The effects of anisotropic permeability on the stability criteria, such as the critical time for the appearance of convective phenomena and the critical wavelength of the most unstable perturbation, are investigated with linear and global stability analysis. The linear stability analysis provides a sufficient condition for instability while the global stability analysis yields a sufficient condition for stability. The results obtained from these two approaches are not exactly the same but show a consistent trend, both indicating that the anisotropic system becomes more unstable when either the vertical or horizontal permeability increases. 相似文献
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The typical shape of a capillary-pressure curve is either convex (e.g., Brooks–Corey model) or S-shaped (e.g., van Genuchten model). It is not universally agreed which model reflects natural rocks better. The difference between the two models lies in the representation of the capillary entry pressure. This difference does not lead to significantly different simulation results for modeling CO2 sequestration in aquifers without considering CO2 dissolution. However, we observe that the van-Genuchten-type capillary-pressure model accelerates CO2 solubility trapping significantly compared with the Brooks–Corey-type model. We also show that the simulation results are very sensitive to the slope of the van-Genuchten-type curve around the entry-pressure region. For the representative examples we study, the differences can be so large as to have complete dissolution of the CO2 plume versus persistence of over 50% of the plume over a 5000-year period.The cause of such sensitivity to the capillary-pressure model is studied. Particularly, we focus on how the entry pressure is represented in each model. We examine the mass-transfer processes under gravity-capillary equilibrium, molecular diffusion, convective mixing, and in the presence of small-scale heterogeneities. Laboratory measurement of capillary-pressure curves and some important implementation issues of capillary-pressure models in numerical simulators are also discussed. Most CO2 sequestration simulations in the literature employ one of the two capillary-pressure models. It is important to recognize that these two representations lead to very different predictions of long-term CO2 sequestration. 相似文献
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V. Shulakova J. Sarout L. Pimienta M. Lebedev S. Mayo M.B. Clennell M. Pervukhina 《Geophysical Prospecting》2017,65(1):251-265
CO2 geosequestration is an efficient way to reduce greenhouse gas emissions into the atmosphere. Carbonate rock formations are one of the possible targets for CO2 sequestration due to their relative abundance and ability to serve as a natural trapping reservoir. The injected supercritical CO2 can change properties of the reservoir rocks such as porosity, permeability, tortuosity, and specific surface area due to dissolution and precipitation processes. This, in turn, affects the reservoir characteristics, i.e., their elastic properties, storage capacity, stability, etc. The tremendous progresses made recently in both microcomputed X‐ray tomography and high‐performance computing make numerical simulation of physical processes on actual rock microstructures feasible. However, carbonate rocks with their extremely complex microstructure and the presence of microporosity that is below the resolution of microcomputed X‐ray tomography scanners require novel, quite specific image processing and numerical simulation approaches. In the current work, we studied the effects of supercritical CO2 injection on microstructure and elastic properties of a Savonnières limestone. We used microtomographic images of two Savonnières samples, i.e., one in its natural state and one after injection and residence of supercritical CO2. A statistical analysis of the microtomographic images showed that the injection of supercritical CO2 led to an increase in porosity and changes of the microstructure, i.e., increase of the average volume of individual pores and decrease in the total number of pores. The CO2 injection/residence also led to an increase in the mean radii of pore throats, an increase in the length of pore network segments, and made the orientation distribution of mesopores more isotropic. Numerical simulations showed that elastic moduli for the sample subjected to supercritical CO2 injection/residence are lower than those for the intact sample. 相似文献
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We suggest that different equations of state (EOS) algorithms can and frequently will provide very different predictions of CO2 migration following injection for sequestration. Rather than carry out an exhaustive examination of all EOS algorithms available, we elected to evaluate this general hypothesis by making detailed comparisons of simulation results of two very common EOS algorithms. We simulated and compared CO2 migration patterns using two fundamentally different EOS algorithms – Modified Redlich-Kwong EOS (MRKEOS) and Span and Wagner EOS (SWEOS). In general, the predictions of thermophysical properties for both algorithms are close, except for a contrast in the predicted fugacity coefficient of CO2, which subsequently propagates to a contrast in predicted solubility in water/brine. Typically, MRKEOS underestimates solubility of CO2 compared to both SWEOS and experimental solubility data. In simulations of CO2 migration, dissolution rates of separate-phase CO2 predicted from the two EOS algorithms were significantly different, even for small contrasts in predicted fluid properties from EOS algorithms, resulting in markedly different migration patterns. 相似文献
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Vertically integrated models are frequently applied to study subsurface flow related to CO2 storage scenarios in saline aquifers. In this paper, we study the impact of capillary-pressure hysteresis and CO2 trapping on the integrated constitutive parameter functions. Our results show that for the initial drainage and a subsequent imbibition, trapping is the dominant contributor to hysteresis in integrated models. We also find that for advective processes like injection and plume migration in a sloped aquifer the correct treatment of the hysteretic nature of the capillary fringe is likely of secondary importance. However, for diffusive/dispersive processes such as a redistribution of the CO2 plume due to buoyancy and capillary forces, the hysteretic nature of the capillary fringe may significantly impact the final distribution of the fluids and the timescale of the redistribution. 相似文献
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Geological heterogeneities affect the dynamics of carbon dioxide (CO2) plumes in subsurface environments in important ways. Previously, we showed how the dynamics of CO2 plumes are influenced by the multiscaled sedimentary architecture in deep brine fluvial-type reservoirs. The results confirm that representing small-scale features and the corresponding heterogeneity in saturation functions, along with hysteresis in saturation functions, are all critical to understanding capillary trapping processes. Here, we show that when heterogeneity and hysteresis are represented, the two conventional approaches for defining saturation functions, Brooks-Corey and van Genuchten, represent fundamentally different physical systems. The Brooks-Corey approach represents heterogeneity in entry pressures, and leads to trapping by capillary pinning. The van Genuchten approach represents a network of pores transporting the nonwetting fluid, across rock types, with negligible capillary entry pressure, and leads to capillary retardation. These differences significantly affect the large-scale characteristics of CO2 plumes (i.e., their mass, shape, and position). 相似文献
11.
Telogenetic epikarst carbon sourcing and transport processes and their associated hydrogeochemical responses are complex and dynamic. Carbon dioxide (CO2) transport rates in the epikarst zone are often driven by hydrogeochemical responses, which influence carbonate dissolution and conduit formation. This study examines the influence of land use on carbon sourcing and carbonate dissolution kinetics through a comparative analysis of separate, but similar, epikarst systems in south-central Kentucky. The use of high-resolution hydrogeochemical data from multiple data loggers and isotope analysis from collected water samples reflects the processes within these epikarst aquifers, which are estimated to contribute significantly to bedrock dissolution. Results indicate that, in an agricultural setting, long-term variability and dissolution is governed by seasonal production of CO2 . In a more urbanized, shallower epikarst system, land cover may affect CO2 transport between the soil and underlying bedrock. This concentration of CO2 potentially contributes to ongoing dissolution and conduit development, irrespective of seasonality. The observed responses in telogenetic epikarst systems seem to be more similar to eogenetic settings, which is suggested to be driven by CO2 transport occurring independent of high matrix porosity. The results of this study indicate site-specific responses with respect to both geochemical and δ13CDIC changes on a seasonal scale, despite regional geologic similarities. The results indicate that further comparative analyses between rural and urban landscapes in other karst settings is needed to delineate the impact of land use and seasonality on dissolution and carbon sourcing during karst formation processes. © 2019 John Wiley & Sons, Ltd. 相似文献
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This study presents the impact of fractures on CO2 transport, capillary pressure and storage capacity by conducting both experimental and numerical studies. A series of laboratory experiment tests was designed with both a homogeneous and a fractured core under CO2 storage conditions. The experimental results reveal a piston-like brine displacement with gravity override effects in the homogeneous core regardless of CO2 injection rates. In the fractured core, however, two distinctive types of brine displacements were observed; one showing brine displacement only in the fracture whereas the other shows brine displacement both in the fracture and matrix with different rates, which were dependent on the magnitude of the pressure build-up in the matrix. The injectivity in the fractured core was twice of the homogeneous core, while the amount of calculated CO2 in the homogeneous core was over 1.5 times greater than the fractured core. Salt precipitation, which is likely to occur near injection wells, was observed in the experiments; X-ray images enabled the observation of salt-precipitation during CO2-flooding tests. Finally, numerical simulations predict free-phase CO2 transfer between fracture and matrix in a fracture-matrix system. Pressure gradients between the fracture and matrix enforced CO2 to transfer from the fracture into matrix at the front of the CO2 plume, whereas, the reversal of pressure gradients at the rear zone of the CO2 plume reversed the transfer process. The variation of CO2 saturation within the fracture was caused by fracture aperture variations, and local variations of fracture permeability control the free-phase CO2 transfer between the fracture and matrix. 相似文献
13.
We present an upscaled model for the vertical migration of a CO2 plume through a vertical column filled with a periodic layered porous medium. This model may describe the vertical migration of a CO2 plume in a perfectly layered horizontal aquifer. Capillarity and buoyancy are taken into account and semi-explicit upscaled flux functions are proposed in the two following cases: (i) capillarity is the main driving force and (ii) buoyancy is the only driving force. In both cases, we show that the upscaled buoyant flux is a bell-shaped function of the saturation, as in the case of a homogeneous porous medium. In the capillary-dominant case, we show that the upscaled buoyant flux is the harmonic mean of the buoyant fluxes in each layer. The upscaled saturation is governed by the continuity of the capillary pressure at the interface between layers. In the capillary-free case, the upscaled buoyant flux and upscaled saturation are determined by the flux continuity condition at the interface. As the flux is not continuous over the entire range of saturation, the upscaled saturation is only defined where continuity is verified, i.e. in two saturation domains. As a consequence, the upscaled buoyant flux is described by a piecewise continuous function. Two analytical approximations of this flux are proposed and this capillary-free upscaled model is validated for two cases of heterogeneity. Upscaled and cell averaged saturations are in good agreement. Furthermore, the proposed analytical upscaled fluxes provide satisfactory approximations as long as the saturation set at the inlet of the column is in a range where analytical and numerical upscaled fluxes are close. 相似文献
14.
The first post‐injection seismic monitor survey at the Ketzin pilot CO2 storage site: results from time‐lapse analysis 
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下载免费PDF全文 Fei Huang Peter Bergmann Christopher Juhlin Monika Ivandic Stefan Lüth Alexandra Ivanova Thomas Kempka Jan Henninges Daniel Sopher Fengjiao Zhang 《Geophysical Prospecting》2018,66(1):62-84
The injection of CO2 at the Ketzin pilot CO2 storage site started in June 2008 and ended in August 2013. During the 62 months of injection, a total amount of about 67 kt of CO2 was injected into a saline aquifer. A third repeat three‐dimensional seismic survey, serving as the first post‐injection survey, was acquired in 2015, aiming to investigate the recent movement of the injected CO2. Consistent with the previous two time‐lapse surveys, a predominantly west–northwest migration of the gaseous CO2 plume in the up‐dip direction within the reservoir is inferred in this first post‐injection survey. No systematic anomalies are detected through the reservoir overburden. The extent of the CO2 plume west of the injection site is almost identical to that found in the 2012 second repeat survey (after injection of 61 kt); however, there is a significant decrease in its size east of the injection site. Assessment of the CO2 plume distribution suggests that the decrease in the size of the anomaly may be due to multiple factors, such as limited vertical resolution, CO2 dissolution, and CO2 migration into thin layers, in addition to the effects of ambient noise. Four‐dimensional seismic modelling based on dynamic flow simulations indicates that a dynamic balance between the newly injected CO2 after the second repeat survey and the CO2 migrating into thin layers and being dissolved was reached by the time of the first post‐injection survey. In view of the significant uncertainties in CO2 mass estimation, both patchy and non‐patchy saturation models for the Ketzin site were taken into consideration. 相似文献
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The vertical stratification of carbon dioxide (CO2) injected into a deep layered aquifer made up of high-permeability and low-permeability layers, such as Utsira aquifer at Sleipner site in Norway, is investigated with a Buckley–Leverett equation including gravity effects. In a first step, we study both by theory and simulation the application of this equation to the vertical migration of a light phase (CO2), in a denser phase (water), in 1D vertical columns filled with different types of porous media: homogeneous, piecewise homogeneous, layered periodic and finally heterogeneous. For each case, we solve the associated Riemann problems and propose semi-analytical solutions describing the spatial and temporal evolution of the light phase saturation. These solutions agree well with simulation results. We show that the flux continuity condition at interfaces between high-permeability and low-permeability layers leads to CO2 saturation discontinuities at these interfaces and, in particular, to a saturation increase beneath low-permeability layers. In a second step, we analyze the vertical migration of a CO2 plume injected into a 2D layered aquifer. We show that the CO2 vertical stratification under each low-permeability layer is induced, as in 1D columns, by the flux continuity condition at interfaces. As the injection takes place at the bottom of the aquifer the velocity and the flux function decrease with elevation and this phenomenon is proposed to explain the stratification under each mudstone layer as observed at Sleipner site. 相似文献
16.
Deep saline aquifers are important geological formations for CO2 sequestration. It has been known that dissolution of CO2 increases brine density, which results in downward density-driven convection and consequently greatly enhances CO2 sequestration. In this study, a continuum-scale lattice Boltzmann model is used to investigate convective mixing of CO2 in saline aquifers. It is found that increasing permeability in either the vertical or horizontal direction accelerates the development of convective mixing. In a heterogeneous aquifer, increasing heterogeneity hampers the onset of convective mixing, because the heterogeneous permeability field results in a large portion of low-velocity region which reduces the instability of the system. The critical time for the onset of instability depends mainly on the coefficient of variation (COV) of the permeability field, and is insensitive to the correlation length. This implies that within the scale of critical time, mass transport is dominated by diffusion, and thus depends mainly on fine-scale heterogeneity controlled by COV. We derived an empirical formula for estimating the critical time, which leads to good estimates for all combinations of COV and correlation length. Fingering, channeling, and dispersion are the three mechanisms for mass transport. In dispersion, dissolved mass is approximately proportional to the square root of time, while in fingering and channeling it is approximately proportional to time. Mass transport by channeling depends significantly on permeability structure, while by fingering it is controlled by gravitational instability. It is also found that larger volumes of CO2 can be stored in heterogeneous aquifers because of higher mass dissolution rates. 相似文献
17.
Predicting and quantifying impacts of potential carbon dioxide (CO2) leakage into shallow aquifers that overlie geologic CO2 storage formations is an important part of developing reliable carbon storage techniques. Leakage of CO2 through fractures, faults or faulty wellbores can reduce groundwater pH, inducing geochemical reactions that release solutes into the groundwater and pose a risk of degrading groundwater quality. In order to help quantify this risk, predictions of metal concentrations are needed during geologic storage of CO2. Here, we present regional-scale reactive transport simulations, at relatively fine-scale, of CO2 leakage into shallow aquifers run on the PFLOTRAN platform using high-performance computing. Multiple realizations of heterogeneous permeability distributions were generated using standard geostatistical methods. Increased statistical anisotropy of the permeability field resulted in more lateral and vertical spreading of the plume of impacted water, leading to increased Pb2+ (lead) concentrations and lower pH at a well down gradient of the CO2 leak. Pb2+ concentrations were higher in simulations where calcite was the source of Pb2+ compared to galena. The low solubility of galena effectively buffered the Pb2+ concentrations as galena reached saturation under reducing conditions along the flow path. In all cases, Pb2+ concentrations remained below the maximum contaminant level set by the EPA. Results from this study, compared to natural variability observed in aquifers, suggest that bicarbonate (HCO3−) concentrations may be a better geochemical indicator of a CO2 leak under the conditions simulated here. 相似文献
18.
George S.H. Pau John B. BellKarsten Pruess Ann S. AlmgrenMichael J. Lijewski Keni Zhang 《Advances in water resources》2010
Simulations are routinely used to study the process of carbon dioxide (CO2) sequestration in saline aquifers. In this paper, we describe the modeling and simulation of the dissolution–diffusion–convection process based on a total velocity splitting formulation for a variable-density incompressible single-phase model. A second-order accurate sequential algorithm, implemented within a block-structured adaptive mesh refinement (AMR) framework, is used to perform high-resolution studies of the process. We study both the short-term and long-term behaviors of the process. It is found that the onset time of convection follows closely the prediction of linear stability analysis. In addition, the CO2 flux at the top boundary, which gives the rate at which CO2 gas dissolves into a negatively buoyant aqueous phase, will reach a stabilized state at the space and time scales we are interested in. This flux is found to be proportional to permeability, and independent of porosity and effective diffusivity, indicative of a convection-dominated flow. A 3D simulation further shows that the added degrees of freedom shorten the onset time and increase the magnitude of the stabilized CO2 flux by about 25%. Finally, our results are found to be comparable to results obtained from TOUGH2-MP. 相似文献
19.
CO2 injection and storage in deep saline aquifers involves many coupled processes, including multiphase flow, heat and mass transport, rock deformation and mineral precipitation and dissolution. Coupling is especially critical in carbonate aquifers, where minerals will tend to dissolve in response to the dissolution of CO2 into the brine. The resulting neutralization will drive further dissolution of both CO2 and calcite. This suggests that large cavities may be formed and that proper simulation may require full coupling of reactive transport and multiphase flow. We show that solving the latter may suffice whenever two requirements are met: (1) all reactions can be assumed to occur in equilibrium and (2) the chemical system can be calculated as a function of the state variables of the multiphase flow model (i.e., liquid and gas pressure, and temperature). We redefine the components of multiphase flow codes (traditionally, water and CO2), so that they are conservative for all reactions of the chemical system. This requires modifying the traditional constitutive relationships of the multiphase flow codes, but yields the concentrations of all species and all reaction rates by simply performing speciation and mass balance calculations at the end of each time step. We applied this method to the H2O–CO2–Na–Cl–CaCO3 system, so as to model CO2 injection into a carbonate aquifer containing brine. Results were very similar to those obtained with traditional formulations, which implies that full coupling of reactive transport and multi-phase flow is not really needed for this kind of systems, but the resulting simplifications may make it advisable even for cases where the above requirements are not met. Regarding the behavior of carbonate rocks, we find that porosity development near the injection well is small because of the low solubility of calcite. Moreover, dissolution concentrates at the front of the advancing CO2 plume because the brine below the plume tends to reach high CO2 concentrations quite rapidly. We conclude that carbonate dissolution needs not to be feared. 相似文献
20.
The nonlinearity of the relationship between CO2 flux and other micrometeorological variables flux parameters limits the applicability of carbon flux models to accurately estimate the flux dynamics. However, the need for carbon dioxide (CO2) estimations covering larger areas and the limitations of the point eddy covariance technique to address this requirement necessitates the modeling of CO2 flux from other micrometeorological variables. Artificial neural networks (ANN) are used because of their power to fit highly nonlinear relations between input and output variables without explaining the nature of the phenomena. This paper applied a multilayer perception ANN technique with error back propagation algorithm to simulate CO2 flux on three different ecosystems (forest, grassland and cropland) in ChinaFLUX. Energy flux (net radiation, latent heat, sensible heat and soil heat flux) and temperature (air and soil) and soil moisture were used to train the ANN and predict the CO2 flux. Diurnal half-hourly fluxes data of observations from June to August in 2003 were divided into training, validating and testing. Results of the CO2 flux simulation show that the technique can successfully predict the observed values with R 2 value between 0.75 and 0.866. It is also found that the soil moisture could not improve the simulative accuracy without water stress. The analysis of the contribution of input variables in ANN shows that the ANN is not a black box model, it can tell us about the controlling parameters of NEE in different ecosystems and micrometeorological environment. The results indicate the ANN is not only a reliable, efficient technique to estimate regional or global CO2 flux from point measurements and understand the spatiotemporal budget of the CO2 fluxes, but also can identify the relations between the CO2 flux and micrometeorological variables.
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