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A primary concern for geologic carbon storage is the potential for leakage of stored carbon dioxide (CO 2 ) into the shallow subsurface where it could degrade the quality of groundwater and surface water. In order to predict and mitigate the potentially negative impacts of CO 2 leakage, it is important to understand the physical processes that CO 2 will undergo as it moves through naturally heterogeneous porous media formations. Previous studies have shown that heterogeneity can enhance the evolution of gas phase CO 2 in some cases, but the conditions under which this occurs have not yet been quantitatively defined, nor tested through laboratory experiments. This study quantitatively investigates the effects of geologic heterogeneity on the process of gas phase CO 2 evolution in shallow aquifers through an extensive set of experiments conducted in a column that was packed with layers of various test sands. Soil moisture sensors were utilized to observe the formation of gas phase near the porous media interfaces. Results indicate that the conditions under which heterogeneity controls gas phase evolution can be successfully predicted through analysis of simple parameters, including the dissolved CO 2 concentration in the flowing water, the distance between the heterogeneity and the leakage location, and some fundamental properties of the porous media. Results also show that interfaces where a less permeable material overlies a more permeable material affect gas phase evolution more significantly than interfaces with the opposite layering.

Hydraulic testing has revealed dramatic underpressures in Paleozoic shales and carbonates at the Bruce nuclear site in Ontario. Although evidence from both laboratory and field studies suggests that a small amount of gas-phase methane could be present in the shale, previous studies examining causal linkages between the gas phase and the underpressure have been inconclusive. To better elucidate processes in such a system, we used a highly simplified 1D representation of the site to test, by using iTOUGH2-EOS7C, the effects of various factors on the evolution of gas-phase methane and pressures within the system. Heterogeneity was represented by three stratigraphic regions with slightly different capillary pressure characteristics and, in one case, three thin distinct zones with very different characteristics. Underpressure occurred only when gas pressures set as an initial condition required it, and even in this case it was geologically short-lived. We conclude that the presence of multiple fluid phases is unlikely to explain the underpressure at the site; we suggest that the influence of gasphase methane on porewater flow is minimal. This is consistent with prior conceptualizations of the underpressured section as a thick aquiclude, in which solute transport occurs extremely slowly, bounded by aquifers of significantly higher permeability.

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