Geochemical reactions may alter the permeability of leakage pathways in caprocks, which serve a critical role in confining CO 2 in geologic carbon sequestration. A caprock specimen from a carbonate formation in the Michigan sedimentary Basin was fractured and studied in a high-pressure core flow experiment. Inflowing brine was saturated with CO 2 at 40°C and 10 MPa, resulting in an initial pH of 4.6, and had a calcite saturation index of -0.8. Fracture permeability decreased during the experiment, but subsequent analyses did not reveal calcite precipitation. Instead, experimental observations indicate that calcite dissolution along the fracture pathway led to mobilization of less soluble mineral particles that clogged the flow path. Analyses of core sections via electron microscopy, synchrotron-based X-ray diffraction imaging, and the first application of microbeam Ca K-edge X-ray absorption near edge structure, provided evidence that these occlusions were fragments from the host rock rather than secondary precipitates. X-ray computed tomography showed a significant loss of rock mass within preferential flow paths, suggesting that dissolution also removed critical asperities and caused mechanical closure of the fracture. The decrease in fracture permeability despite a net removal of material along the fracture pathway demonstrates a nonintuitive, inverse relationship between dissolution and permeability evolution in a fractured carbonate caprock.
Invasion percolation with trapping (IPT) and diffusion-limited aggregation (DLA) are simple fractal models, which are known to describe two-phase flow in porous media at well defined, but unphysical limits of the fluid properties and flow conditions. A decade ago, Fernandez, Rangel, and Rivero predicted a crossover from IPT (capillary fingering) to DLA (viscous fingering) for the injection of a zero-viscosity fluid as the injection velocity was increased from zero. [Phys. Rev. Lett. 67, 2958 (1991)]]. We have performed experiments in which air is injected into a glass micromodel to displace water. These experiments clearly demonstrate this crossover as the injection velocity of the air is increased. Furthermore, simulations, using our standard pore-level model, also support the predicted IPT-to-DLA crossover, as well as the predicted power-law behavior of the characteristic crossover length.
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