New experimental measurements (at 10 MPa and 323.15 K) and molecular dynamics (MD) simulations (at 10 MPa and 323.15 K, 50 MPa and 344.25 K, and 50 MPa and 375.5 K) are reported in order to measure/predict the aqueous solubilities of the ternary methane–carbon dioxide–water system under two-phase (vapor–liquid) equilibrium conditions. The TIP4P/ice, TraPPE-UA, and OPLS-UA force fields for water, carbon dioxide, and methane, respectively, are used, according to the modifications introduced in the recent study by Michalis et al. (Phys. Chem. Chem. Phys., 2016, 18, 23538–23548) for the binary methane–carbon dioxide hydrate. The MD calculated values for the solubility are in good agreement with the newly available experimental measurements. The molecular dynamics simulations clearly indicate that the solubility of each gas decreases by the addition of the other gas. The particular conclusion is in excellent agreement with the conclusion obtained from the new experimental measurements reported in the current study, as well as the analysis of previously reported experimental measurements. The new experimental solubility measurements are found to be in very good agreement with the limited available experimental data in the literature for the ternary mixture.

中文翻译：

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三元（甲烷+二氧化碳+水）混合物水相中甲烷和二氧化碳的溶解度：实验测量和分子动力学模拟

为了测量/预测水的溶解度，报告了新的实验测量值（在10 MPa和323.15 K下）和分子动力学（MD）模拟（在10 MPa和323.15 K，50 MPa和344.25 K，50 MPa和375.5 K下）两相（汽-液）平衡条件下的三元甲烷-二氧化碳-水系统的组成。根据Michalis等人最近的研究中引入的修改，分别使用了TIP4P / ice，TraPPE-UA和OPLS-UA力场来测量水，二氧化碳和甲烷的力场。（物理学。化学式化学物理。，2016，18（23538-23548）中的甲烷/二氧​​化碳二元水合物。MD的溶解度计算值与新近获得的实验测量值非常吻合。分子动力学模拟清楚地表明，每种气体的溶解度会因添加其他气体而降低。该特定结论与从当前研究中报道的新实验测量以及对先前报道的实验测量的分析得出的结论高度吻合。发现新的实验溶解度测量值与文献中有关三元混合物的有限的可用实验数据非常吻合。