Interface dissolution kinetics and porosity formation of calcite and dolomite (110) and (104) planes: An implication to the stability of geologic carbon sequestration.

ABSTRACT

Geologic carbon sequestration (GCS) via injecting CO2 into deep carbonate reservoirs (mainly calcite and dolomite) is a promising strategy to reduce CO2 level. However, the dissolution or precipitation of calcite/dolomite planes on minerals/solution interface during long-term GCS process develops intergranular porosity and thus affects the permeability and stability of reservoirs. To investigate this process, both calcite and dolomite were dissolved in acetic and carbonic acids. A diffusion-controlled process was identified, with greater diffusion rates in acetic acid than that in carbonic acid. Quantified planes activity of both minerals follows (110) > (116) > (101) > (113) > (018) > (104) through density functional theory. Accomplished with preferential dissolution of calcite (110) planes in carbonic acid, calcite crystals precipitated with (104) planes at 423.15 K, under which, more calcite crystals were observed on dolomite surface, producing Ca-deplete surface. Molecular dynamic calculations showed higher dissolution rates of calcite/dolomite (110) planes than (104). In addition, the dissolution coefficients of Ca2+ were approximately triple of that Mg2+. Therefore, this study reveals the interface dissolution mechanisms of calcite and dolomite, especially on (110) and (104) planes at an atomic level, for the first time, providing better understanding for the stability of long-term GCS process.