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首页> 外文期刊>Environmental Science & Technology >Synergistic Coupling of CO_2 and H_2O during Expansion of Clays in Supercritical CO_2-CH_4 Fluid Mixtures
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Synergistic Coupling of CO_2 and H_2O during Expansion of Clays in Supercritical CO_2-CH_4 Fluid Mixtures

机译：CO_2和H_2O在超临界CO_2-CH_4流体混合物中膨胀过程中CO_2和H_2O的协同耦合

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摘要

We used IR and XRD, with supporting theoretical calculations, to investigate the swelling behavior of Na~+-, NH_4~+-, and Cs~+-montmorillonites (SWy-2) in supercritical fluid mixtures of H_2O, CO_2, and CH_4. Building on our prior work with Na-clay that demonstrated that H_2O facilitated CO_2 intercalation at relatively low RH, here we show that increasing CO_2/CH_4 ratios promote H_2O intercalation and swelling of the Na-clay at progressively lower RH. In contrast to the Na-clay, CO_2 intercalated and expanded the Cs-clay even in the absence of H_2O, while increasing fluid CO_2/CH_4 ratios inhibited H_2O intercalation. The NH_4-clay displayed intermediate behavior. By comparing changes in the HOH bending vibration of H_2O intercalated in the Cs-, NH_4-, and Na-clays, we posit that CO_2 facilitated expansion of the Na-clay by participating in outer-sphere solvation of Na~+ and by disrupting the H-bond network of intercalated H_2O. In no case did the pure CH_4 fluid induce expansion. Our experimental data can benchmark modeling studies aimed at predicting clay expansion in humidified fluids with varying ratios of CO_2 and CH_4 in real reservoir systems with implications for enhanced hydrocarbon recovery and CO_2 storage in subsurface environments.
机译：我们使用IR和XRD，支持理论计算，研究H_2O，CO_2和CH_4的超临界流体混合物中Na〜+ - ，NH_4〜+ - 和CS〜+ -Montmorillonites（SWY-2）的溶胀行为。建立在我们与Na-Clay的前面的工作中，证明H_2O促进了相对低RH的CO_2嵌入，在这里，我们表明增加的CO_2 / CH_4比率促进NA-CLAY的H_2O嵌入和溶胀在逐步的下RH。与Na-Clay相反，CO_2嵌入并使CS-粘土膨胀并在不存在H_2O的情况下，同时增加流体CO_2 / CH_4比率抑制H_2O嵌入。 NH_4-CLAY显示中间行为。通过比较CS-，NH_4-和Na-Clays中嵌入H_2O的HOH弯曲振动的变化，我们通过参与NA〜+的外球溶解和破坏嵌入H_2O的H键网络。在任何情况下，纯CH_4流体都会引起扩张。我们的实验数据可以基准建模研究，旨在预测潮湿的流体中的粘土膨胀，其具有实际储层系统中的CO_2和CH_4的不同比例，具有对地下环境中增强的烃恢复和CO_2储存的影响。

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