Department of Energy, Environmental and Chemical Engineering, Washington University in St Louis, St Louis, Missouri 63130, United States.
Environ Sci Technol. 2013 Jan 2;47(1):150-8. doi: 10.1021/es302324m. Epub 2012 Sep 28.
Organic compounds in deep saline aquifers may change supercritical CO(2) (scCO(2))-induced geochemical processes by attacking specific components in a mineral's crystal structure. Here we investigate effects of acetate and oxalate on alkali feldspar-brine interactions in a simulated geologic carbon sequestration (GCS) environment at 100 atm of CO(2) and 90 °C. We show that both organics enhance the net extent of feldspar's dissolution, with oxalate showing a more prominent effect than acetate. Further, we demonstrate that the increased reactivity of Al-O-Si linkages due to the presence of oxalate results in the promotion of both Al and Si release from feldspars. As a consequence, the degree of Al-Si order may affect the effect of oxalate on feldspar dissolution: a promotion of ~500% in terms of cumulative Si concentration was observed after 75 h of dissolution for sanidine (a highly disordered feldspar) owing to oxalate, while the corresponding increase for albite (a highly ordered feldspar) was ~90%. These results provide new insights into the dependence of feldspar dissolution kinetics on the crystallographic properties of the mineral under GCS conditions.
在深部盐水含水层中的有机化合物可能通过攻击矿物晶体结构中的特定成分来改变超临界 CO2(scCO2)诱发的地球化学过程。在这里,我们在模拟地质封存(GCS)环境中研究了醋酸盐和草酸盐对碱性长石-盐水相互作用的影响,实验条件为 100 个大气压的 CO2 和 90°C。我们表明,这两种有机物都增强了长石溶解的净程度,草酸盐的影响比醋酸盐更为显著。此外,我们证明了由于草酸盐的存在,Al-O-Si 键的反应性增加,导致长石中 Al 和 Si 的释放都得到了促进。因此,Al-Si 有序度可能会影响草酸盐对长石溶解的影响:在 75 小时的溶解过程中, sanidine(一种高度无序的长石)中观察到的 Si 浓度累积增加了约 500%,而 albite(一种高度有序的长石)的相应增加约为 90%。这些结果为在 GCS 条件下长石溶解动力学对矿物结晶性质的依赖性提供了新的见解。