Experimental dissolution of dolomite by CO2-charged brine at 100 °C and 150 bar: Evolution of porosity, permeability, and reactive surface area

•Flow-through experiments on dolomite cores produced a range of dissolution patterns that modified reactive surface area.•XRCT reconstructions illustrate diameter and tortuosity effects of fit parameters in porosity–surface area model.•Elevated recoveries of Ba, Mn, and Sr compared to Ca and Mg indicate dissolution within grains throughout the entire core.•Permeability increases more efficiently per increase in porosity with reaction progress.•A porosity–surface area model is incorporated into a reactive transport model using TOUGHREACT.

Hydrothermal flow experiments of single-pass injection of CO2-charged brine were conducted on nine dolomite cores to examine fluid–rock reactions in dolomite reservoirs under geologic carbon sequestration conditions. Post-experimental X-ray computed tomography (XRCT) analysis illustrates a range of dissolution patterns, and significant increases in core bulk permeability were measured as the dolomite dissolved. Outflow fluids were below dolomite saturation, and cation concentrations decreased with time due to reductions in reactive surface area with reaction progress. To determine changes in reactive surface area, we employ a power-law relationship between reactive surface area and porosity (Luquot and Gouze, 2009). The exponent in this relationship is interpreted to be a geometrical parameter that controls the degree of surface area change per change in core porosity. Combined with XRCT reconstructions of dissolution patterns, we demonstrate that this exponent is inversely related to both the flow path diameter and tortuosity of the dissolution channel. Even though XRCT reconstructions illustrate dissolution at selected regions within each core, relatively high Ba and Mn recoveries in fluid samples suggest that dissolution occurred along the core's entire length and width. Analysis of porosity–permeability data indicates an increase in the rate of permeability enhancement per increase in porosity with reaction progress as dissolution channels lengthen along the core. Finally, we incorporate the surface area–porosity model of Luquot and Gouze (2009) with our experimentally fit parameters into TOUGHREACT to simulate experimental observations.