Changes in caprock integrity due to vertical migration of CO ₂-enriched brine

In geologic carbon sequestration, caprock fractures may act as leakage pathways, threatening the long term sealing ability of the formation. A flow-through experiment was performed to investigate fracture evolution of a fractured carbonate caprock during simulated leakage of CO₂-acidified brine. The initial brine composition represented that of a CO ₂-saturated brine having previously reacted with the injection formation minerals resulting in a starting pH of 4.9. Experimental temperature and pressure conditions were 40°C and 10 MPa, corresponding to injection at a depth of 1 km. A combination of X-ray computed tomography and scanning electron microscopy was used to observe fracture evolution and investigate the mineralogical changes that occurred along the fracture wall. After one week of brine flow, the cross-sectional fracture area increased by an average of 2.7 times that of the initial fracture. The fracture surface was not eroded uniformly, with the largest areas of aperture growth corresponding to direct contact between the acidified brine and calcite. This preferential dissolution of calcite led to a large increase in fracture surface roughness and in some instances, created a silicate mineral-rich microporous coating along the fracture wall. Results from this study suggest that the clay content of low permeability carbonate formations may be an important factor in controlling their long term integrity while in contact with acidified brine and should be considered when selecting appropriate injection sites for geologic CO ₂ sequestration.