Confined Water Determines Transport Properties of Guest Molecules in Narrow Pores

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• 作者：Anh Phan ; David R. Cole ; R. Gregor Weiß ; Joachim Dzubiella ; Alberto Striolo
• 刊名：ACS Nano
• 出版年：2016
• 出版时间：August 23, 2016
• 年：2016
• 卷：10
• 期：8
• 页码：7646-7656
• 全文大小：878K
• 年卷期：0
• ISSN：1936-086X

文摘

We computed the transport of methane through 1 nm wide slit-shaped pores carved out of solid substrates. Models for silica, magnesium oxide, and alumina were used as solid substrates. The pores were filled with water. The results show that the methane permeability through the hydrated pores is strongly dependent on the solid substrate. Detailed analysis of the simulated systems reveals that local properties of confined water, including its structure, and more importantly, evolution of solvation free energy and hydrogen bond structure are responsible for the pronounced differences observed. The simulations are extended to multicomponent systems representative of natural gas, containing methane, ethane, and H₂S. The results show that all pores considered have high affinity for H₂S, moderate affinity for methane, and low affinity for ethane. The H₂S/methane transport selectivity through the hydrated alumina pore is comparable, or superior, to that reported for existing commercial membranes. A multiscale approach was then implemented to demonstrate that a Smoluchowski one-dimensional model is able to reproduce the molecular-level results for short pores when appropriate values for the local self-diffusion coefficients are used as input parameters. We propose that the model can be extended to predict methane transport through uniform hydrated pores of macroscopic length. When verified by experiments, our simulation results could have important implications in applications such as natural gas sweetening and predictions of methane migration through hydraulically fractured shale formations.