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      Thermodynamically Consistent Methodology for Estimation of Diffusivities of Mixtures of Guest Molecules in Microporous Materials

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      ACS Omega
      American Chemical Society

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          Abstract

          The Maxwell–Stefan (M–S) formulation, that is grounded in the theory of irreversible thermodynamics, is widely used for describing mixture diffusion in microporous crystalline materials such as zeolites and metal–organic frameworks (MOFs). Binary mixture diffusion is characterized by a set of three M–S diffusivities: Đ 1, Đ 2, and Đ 12. The M–S diffusivities Đ 1 and Đ 2 characterize interactions of guest molecules with pore walls. The exchange coefficient Đ 12 quantifies correlation effects that result in slowing-down of the more mobile species due to correlated molecular jumps with tardier partners. The primary objective of this article is to develop a methodology for estimating Đ 1, Đ 2, and Đ 12 using input data for the constituent unary systems. The dependence of the unary diffusivities Đ 1 and Đ 2 on the pore occupancy, θ, is quantified using the quasi-chemical theory that accounts for repulsive, or attractive, forces experienced by a guest molecule with the nearest neighbors. For binary mixtures, the same occupancy dependence of Đ 1 and Đ 2 is assumed to hold; in this case, the occupancy, θ, is calculated using the ideal adsorbed solution theory. The exchange coefficient Đ 12 is estimated from the data on unary self-diffusivities. The developed estimation methodology is validated using a large data set of M–S diffusivities determined from molecular dynamics simulations for a wide variety of binary mixtures (H 2/CO 2, Ne/CO 2, CH 4/CO 2, CO 2/N 2, H 2/CH 4, H 2/Ar, CH 4/Ar, Ne/Ar, CH 4/C 2H 6, CH 4/C 3H 8, and C 2H 6/C 3H 8) in zeolites (MFI, BEA, ISV, FAU, NaY, NaX, LTA, CHA, and DDR) and MOFs (IRMOF-1, CuBTC, and MgMOF-74).

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          Molecular simulations of zeolites: adsorption, diffusion, and shape selectivity.

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            Ethene/ethane separation by the MOF membrane ZIF-8: Molecular correlation of permeation, adsorption, diffusion

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              Zeolite membranes – Recent developments and progress

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                Author and article information

                Journal
                ACS Omega
                ACS Omega
                ao
                acsodf
                ACS Omega
                American Chemical Society
                2470-1343
                02 August 2019
                20 August 2019
                : 4
                : 8
                : 13520-13529
                Affiliations
                Van ’t Hoff Institute for Molecular Sciences, University of Amsterdam , Science Park 904, 1098 XH Amsterdam, The Netherlands
                Author notes
                Article
                10.1021/acsomega.9b01873
                6705243
                31460481
                ad76defe-73ba-4d78-bc35-dba40f91d547
                Copyright © 2019 American Chemical Society

                This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License, which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.

                History
                : 23 June 2019
                : 26 July 2019
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                Custom metadata
                ao9b01873
                ao-2019-01873a

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