Excess-Entropy Scaling for Gas Diffusivity in Nanoporous Materials

Journal Article · Thu Sep 26 04:00:00 EDT 2013 · Langmuir

DOI:https://doi.org/10.1021/la403082q· OSTI ID:1126535

Liu, Yu ^[1]; Fu, Jia ^[1]; Wu, Jianzhong ^[1]

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1. Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering and Dept. of Mathematics

Here, we present an efficient computational procedure for the rapid prediction of the self-diffusivity of gas molecules in nanoporous materials by a combination of the Knudsen model, Rosenfeld’s excess-entropy scaling method, and a classical density functional theory (DFT). The self-diffusivity conforms to the Knudsen model at low density, and the effects of intermolecular interactions at higher densities are accounted for by Rosenfeld’s excess-entropy scaling method. The classical DFT provides a convenient way to calculate the excess entropy used in the scaling analysis. The hybrid computational procedure has been calibrated with MD simulation for the adsorption of H₂, He, Ne, and Ar gases in several nanoporous materials over a broad range of pressure. It predicts adsorption isotherms and different types of diffusion behavior in excellent agreement with the simulation results. Although the simulation of gas diffusion in nanoporous materials is extremely time-consuming, the new procedure is computationally very efficient because it uses only single molecular and thermodynamic parameters.

• Research Organization: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
• DOE Contract Number: AC05-00OR22725
• OSTI ID: 1126535
• Journal Information: Langmuir, Journal Name: Langmuir Journal Issue: 42 Vol. 29; ISSN 0743-7463
• Publisher: American Chemical Society
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE