Unveil the controls on CO2 diffusivity in saline brines for geological carbon storage

Heng Wang , Yunfei Li , Chengyang Li , Haiyan Zhu , Zhiwu Li , Lei Wang , Bryan X. Medina-Rodriguez
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Abstract

Accurate estimation of the diffusivity of CO2 in formation brine, one of the dominant mass transfer mechanisms, is crucial for characterizing CO2 migration and distribution in Geological Carbon Storage (GCS). However, the effects of pressure, temperature, and the composition and concentration of ions on the CO2 diffusion coefficient in saline aquifers are complex. This study used in-house-designed equipment to determine the diffusion coefficient of supercritical CO2 in synthetic brines, such as deionized water and NaCl, CaCl2, and KCl solutions under different pressure and temperature conditions. First, CO2 solubilities at initial pressure and temperature were measured to provide the initial CO2 concentration at the gas-liquid interface. Then, pressure decay curves were collected for the selected brines and the diffusion coefficients of CO2 molecules were calculated based on Fick's second law. Experimental results show that CO2 solubility increases with increasing pressure and decreasing temperature and ionic strength. Moreover, CO2 solubilities at same pressure, temperature and ionic strength conditions vary in different synthetic brines. We also found that CO2 diffuses faster in brine at higher pressures and temperatures but slows down as ionic strength increases. The type of ions affects the diffusion differently, except at higher pressures, where their impacts balance out due to hydration effects. In addition, a good linear relationship between CO2 diffusion coefficient and solubility was observed, indicating the CO2 diffusion coefficient could be estimated by solubility. The findings in this study shed a light on the CO2 migration during commercial-scale geological storage and enhanced oil recovery processes.
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揭示二氧化碳在盐湖卤水中扩散的控制因素,实现地质碳封存
二氧化碳在地层盐水中的扩散系数是主要的传质机制之一,准确估算这一扩散系数对于确定二氧化碳在地质碳封存(GCS)中的迁移和分布特征至关重要。然而,压力、温度以及离子的成分和浓度对盐类含水层中二氧化碳扩散系数的影响非常复杂。本研究使用内部设计的设备,测定了不同压力和温度条件下超临界二氧化碳在去离子水、NaCl、CaCl2 和 KCl 溶液等合成盐水中的扩散系数。首先,测量初始压力和温度下的二氧化碳溶解度,以提供气液界面上的二氧化碳初始浓度。然后,收集所选盐水的压力衰减曲线,并根据菲克第二定律计算出二氧化碳分子的扩散系数。实验结果表明,二氧化碳的溶解度随压力的增加而增加,随温度和离子强度的降低而降低。此外,在相同压力、温度和离子强度条件下,不同合成盐水中的二氧化碳溶解度也不同。我们还发现,在压力和温度较高时,二氧化碳在盐水中的扩散速度较快,但随着离子强度的增加,扩散速度减慢。离子类型对扩散的影响不同,但在较高压力下,由于水合作用,离子类型对扩散的影响趋于平衡。此外,二氧化碳扩散系数与溶解度之间存在良好的线性关系,这表明二氧化碳扩散系数可以通过溶解度来估算。本研究的发现揭示了商业规模地质封存和提高石油采收率过程中的二氧化碳迁移问题。
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