Eckel Anna-Maria, Rovelli Andrea, Pini Ronny
Department of Chemical Engineering, Imperial College London, LondonSW7 2AZ , U.K.
Environ Sci Technol. 2025 Mar 11;59(9):4618-4630. doi: 10.1021/acs.est.4c10183. Epub 2025 Mar 2.
Free solutal convection refers to the mixing process induced and sustained by local density differences arising from solute dissolution. This process underpins the long-term storage of carbon dioxide (CO) following its injection and dissolution in the formation brine of subsurface rock formations, such as saline aquifers. Direct experimental evidence of free solutal convection in porous rocks is to-date still lacking, leaving large uncertainties on the realized rate of CO dissolution and its contribution toward storage. Using an analogue solute-solvent pair and 4D X-ray computed tomography, we report direct observations of this mixing process in rock core samples, including sandstones and carbonates. The imagery is used to characterize the mixing structures that arise upon solute dissolution and to quantify differences between the rock types. Thus, we compute the temporal evolution of spatial moments of the concentration distribution to derive practical properties, such as the effective transport velocity of the solute plumes. Unlike previous studies on random bead packs, we observe that these measures do not scale well with core-scale rock properties (permeability, porosity, Rayleigh number) and are influenced by microscale rock characteristics (subcore and pore-scale heterogeneities). The latter may need consideration when evaluating the CO storage potential of candidate formations.
自由溶质对流是指由溶质溶解引起的局部密度差异所诱导和维持的混合过程。该过程是二氧化碳(CO)注入并溶解于地下岩层(如盐含水层)的地层卤水中后进行长期储存的基础。迄今为止,多孔岩石中自由溶质对流的直接实验证据仍然缺乏,这使得CO溶解的实际速率及其对储存的贡献存在很大的不确定性。我们使用一对模拟溶质 - 溶剂,并通过四维X射线计算机断层扫描技术,报告了在岩芯样品(包括砂岩和碳酸盐岩)中对这种混合过程的直接观测结果。这些图像用于表征溶质溶解时出现的混合结构,并量化不同岩石类型之间的差异。因此,我们计算浓度分布空间矩的时间演化,以得出实际属性,如溶质羽流的有效传输速度。与之前对随机珠粒填充的研究不同,我们观察到这些测量结果与岩芯尺度的岩石属性(渗透率、孔隙率、瑞利数)的比例关系不佳,并且受到微观尺度岩石特征(亚岩芯和孔隙尺度非均质性)的影响。在评估候选地层的CO储存潜力时,可能需要考虑后者。