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Motivated by CO2 capture and sequestration (CCS) design considerations, weconsider the coupled effects of permeability heterogeneity and background flowon the dissolution of a supercritical CO2 lens into an underlying deep,confined aquifer. We present the results of a large-scale Monte Carlosimulation study examining the interaction of background flow rate and threeparameters describing multi-Gaussian log-permeability fields: mean, variance,and correlation length. Hundreds of high-resolution simulations were performedusing the PFLOTRAN finite volume software to model CO2 dissolution in akilometer-scale aquifer over 1000 y. Predictive dimensionless scalingrelationships relating CO2 dissolution rate to heterogeneity statistics,Rayleigh (Ra) and Peclet (Pe) numbers were developed for both gravitationallydominated free convection to background flow-dominated forced convectionregimes. An empirical criterion, $\rm Pe\ = Ra^{3/4}$, was discovered forregime transition. All simulations converged quickly to a quasi-steady,approximately linear dissolution rate. However, this rate displayed profoundvariability between permeability field realizations sharing the sameheterogeneity statistics, even under mild permeability heterogeneity. Ingeneral, increased heterogeneity was associated with a lower mean and highervariance of dissolution rate, undesirable from a CCS design perspective. Therelationship between dissolution rate and background flow was found to becomplex and nonlinear. Dimensionless scaling relationships were uncovered for anumber of special cases. Results call into question the validity of theBoussinesq approximation in the context of modest-to-high background flow ratesand the general applicability of numerical simulations without background flow.

Impacts of permeability heterogeneity and background flow on supercritical CO2 dissolution in the deep subsurface