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SO2 与 CO2 共注入地质封存中的溶解电势。

Dissolution potential of SO2 Co-injected with CO2 in geologic sequestration.

机构信息

Department of Civil & Environmental Engineering, Princeton University, Princeton, New Jersey 08540, USA.

出版信息

Environ Sci Technol. 2010 Jan 1;44(1):349-55. doi: 10.1021/es902612m.

Abstract

Sulfur dioxide is a possible co-injectant with carbon dioxide in the context of geologic sequestration. Because of the potential of SO2 to acidify formation brines, the extent of SO2 dissolution from the CO2 phase will determine the viability of co-injection. Pressure-, temperature-, and salinity-adjusted values of the SO2 Henry's Law constant and fugacity coefficient were determined. They are predicted to decrease with depth, such that the solubility of SO2 is a factor of 0.04 smaller than would be predicted without these adjustments. To explore the potential effects of transport limitations, a nonsteady-state model of SO2 diffusion through a stationary cone-shaped plume of supercritical CO2 was developed. This model represents an end-member scenario of diffusion-controlled dissolution of SO2, to contrast with models of complete phase equilibrium. Simulations for conditions corresponding to storage depths of 0.8-2.4 km revealed that after 1000 years, 65-75% of the SO2 remains in the CO2 phase. This slow release of SO2 would largely mitigate its impact on brine pH. Furthermore, small amounts of SO2 are predicted to have a negligible effect on the critical point of CO2 but will increase phase density by as much as 12% for mixtures containing 5% SO2.

摘要

二氧化硫是地质封存中与二氧化碳共同注入的一种可能性物质。由于 SO2 具有酸化地层盐水的潜力,因此从 CO2 相中溶解的 SO2 程度将决定共同注入的可行性。确定了压力、温度和盐度调整后的 SO2 亨利定律常数和逸度系数值。预测这些值随深度降低,使得 SO2 的溶解度比没有这些调整时预测的溶解度小 0.04 倍。为了探索传输限制的潜在影响,开发了一个通过超临界 CO2 固定锥形羽流扩散的 SO2 非稳态模型。该模型代表了扩散控制溶解 SO2 的极端情况,与完全相平衡模型形成对比。针对对应于存储深度 0.8-2.4 km 的条件的模拟表明,在 1000 年后,65-75%的 SO2 仍保留在 CO2 相中。SO2 的这种缓慢释放将在很大程度上减轻其对盐水 pH 值的影响。此外,预测少量的 SO2 对 CO2 的临界点几乎没有影响,但对于含有 5%SO2 的混合物,将使相密度增加高达 12%。

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