Pore-scale study of calcite dissolution during CO2-saturated brine injection for sequestration in carbonate aquifers

Abstract

The calcite reaction with carbonate acid is a prerequisite to release cations providing the reactant for mineral trapping, however, the complicated multiple physicochemical processes during calcite dissolution are hardly precisely captured in carbonate aquifers, impeding the CO2 sequestration technology. In this work, a pore-scale numerical study based on the lattice Boltzmann method coupled fluid flow, mass transport, heterogeneous reactions, and calcite structure evolution is implemented to investigate the calcite dissolution process. Firstly, the impact of pressure difference on this reaction is analyzed to identify two characteristic dissolution patterns. Selecting two typical pressure differences, namely 0.036 and 0.36 Pa, the dissolution dynamics under different temperatures from 25 to 85 °C is then investigated by species concentration and solid distributions elucidating that the effect of pressure difference on calcite dissolution will drop with the increment of temperature. Moreover, the regime diagram of calcite dissolution is plotted based on the relation between temperature and pressure. Finally, to upscale the simulation results to the representative element volume scale, the temporal evolution of normalized permeability, the normalized permeability-porosity relationship and the optimal operations are explored to find that the maximum discrepancy of the normalized permeability with the time among all cases is approximately seven times and the best operating conditions promoting the mineral trapping are a high-temperature formation with a high injection rate.