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When CO2 is injected in saline aquifers, dissolution causes a local increase in brine density that can cause Rayleigh-Taylor-type gravitational instabilities. Depending on the Rayleigh number, density-driven flow may mix dissolved CO2 throughout the aquifer at fast advective time-scales through convective mixing. Heterogeneity can impact density-driven flow to different degrees. Zones with low effective vertical permeability may suppress fingering and reduce vertical spreading, while potentially increasing transverse mixing. In more complex heterogeneity, arising from the spatial organization of sedimentary facies, finger propagation is reduced in low permeability facies, but may be enhanced through more permeable facies. The connectivity of facies is critical in determining the large-scale transport of CO2-rich brine. We perform high-resolution finite element simulations of advection-diffusion transport of CO2 with a focus on facies-based bimodal heterogeneity. Permeability fields are generated by a Markov Chain approach, which represent facies architecture by commonly observed characteristics such as volume fractions. CO2 dissolution and phase behavior are modeled with the cubic-plus-association equation-of-state. Our results show that the organization of high-permeability facies and their connectivity control the dynamics of gravitationally unstable flow. We discover new flow regimes in both homogeneous and heterogeneous media and present quantitative scaling relations for their temporal evolution.

A field-scale carbon dioxide (CO2) injection pilot project was conducted as part of the Southeast Regional Sequestration Partnership (SECARB) at Cranfield, Mississippi. We present higher-order finite element simulations of the compositional two-phase CO2-brine flow and transport during the experiment. High-resolution static models of the formation geology in the Detailed Area Study (DAS) located below the oilwater contact (brine saturated) are used to capture the impact of connected flow paths on breakthrough times in two observation wells. Phase behavior is described by the cubic-plus-association (CPA) equation of state, which takes into account the polar nature of water molecules. Parameter studies are performed to investigate the importance of Fickian diffusion, permeability heterogeneity, relative permeabilities, and capillarity. Simulation results for the pressure response in the injection well and the CO2 breakthrough times at the observation wells show good agreement with the field data. For the high injection rates and short duration of the experiment, diffusion is relatively unimportant (high Péclet numbers), while relative permeabilities have a profound impact on the pressure response. High-permeability pathways, created by fluvial deposits, strongly affect the CO2-transport and highlight the importance of properly characterizing the formation heterogeneity in future carbon sequestration projects.

The geologic architecture in sedimentary reservoirs affects the behavior of density-driven flow and the dispersion of CO-rich brine. The spatial organization and connectivity of facies types play an important role. Low-permeability facies may suppress fingering and reduce vertical spreading, but may also increase transverse mixing. This is more pronounced when geologic structures create preferential flow pathways through connected facies types. We perform high-resolution simulations of three-dimensional (3D) heterogeneous formations whose connectivity cannot be represented in two-dimensional models consistent with percolation theory. This work focuses on the importance of 3D facies-based heterogeneity and connectivity on advection-diffusion transport of dissolved CO. Because the dissolution of CO and the subsequent density increase of brine are the driving force for gravitational instabilities, we model the phase behavior with the accurate cubic-plus-association equation-of-state, which accounts for the self-association of polar water molecules and the cross-association between CO and water. Our results elucidate how the spatial organization of facies affects the dynamics of CO convective mixing. Scaling relations for the evolution of a global dispersion-width provide insights that can be universally applied. The results suggest that the long-term evolution and scaling of dispersion are surprisingly similar for homogeneous and (binary and multiscale) heterogeneous porous media.

We numerically examine solutal convection in porous media, driven by the dissolution of carbon dioxide (CO2) into water-an effective mechanism for CO2 storage in saline aquifers. Dissolution is associated with slow diffusion of free-phase CO2 into the underlying aqueous phase followed by density-driven convective mixing of CO2 throughout the water-saturated layer. We study the fluid dynamics of CO2 convection in the single aqueous-phase region. A comparison is made between two different boundary conditions in the top of the formation: (i) a constant, maximum aqueous-phase concentration of CO2, and (ii) a constant, low injection-rate of CO2, such that all CO2 dissolves instantly and the system remains in single phase. The latter model is found to involve a nonlinear evolution of CO2 composition and associated aqueous-phase density, which depend on the formation permeability. We model the full nonlinear phase behavior of water-CO2 mixtures in a confined domain, consider dissolution and fluid compressibility, and relax the common Boussinesq approximation. We discover new flow regimes and present quantitative scaling relations for global characteristics of spreading, mixing, and a dissolution flux in two-and three-dimensional media for both boundary conditions. We also revisit the scaling behavior of Sherwood number (Sh) with Rayleigh number (Ra), which has been under debate for porous-media convection. Our measurements from the solutal convection in the range 1, 500 Ra 135, 000 show that the classical linear scaling Sh ∼ Ra is attained asymptotically for the constant-concentration case. Similarly linear scaling is recovered for the constant-flux model problem. The results provide a new perspective into how boundary conditions may affect the predictive powers of numerical models, e.g., for both the short-term and long-term dynamics of convective mixing rate and dissolution flux in porous media at a wide range of Rayleigh numbers.

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