Affiliation:
1. Guangzhou Key Laboratory for New Energy and Green Catalysis School of Chemistry and Chemical Engineering Guangzhou University Guangzhou 510006 China
2. Joint Institute of Guangzhou University & Institute of Corrosion Science and Technology Guangzhou University Guangzhou 510006 China
Abstract
AbstractFor gas separation and catalysis by metal‐organic frameworks (MOFs), gas diffusion has a substantial impact on the process' overall rate, so it is necessary to determine the molecular diffusion behavior within the MOFs. In this study, an interpretable machine learing (ML) model, light gradient boosting machine (LGBM), is trained to predict the molecular diffusivity and selectivity of 9 gases (Kr, Xe, CH4, N2, H2S, O2, CO2, H2, and He). For these 9 gases, LGBM displays high accuracy (average R2 = 0.962) and superior extrapolation for the diffusivity of C2H6. And this model calculation is five orders of magnitude faster than molecular dynamics (MD) simulations. Subsequently, using the trained LGBM model, an interactive desktop application is developed that can help researchers quickly and accurately calculate the diffusion of molecules in porous crystal materials. Finally, the authors find the difference in the molecular polarizability (ΔPol) is the key factor governing the diffusion selectivity by combining the trained LGBM model with the Shapley additive explanation (SHAP). By the calculation of interpretable ML, the optimal MOFs are selected for separating binary gas mixtures and CO2 methanation. This work provides a new direction for exploring the structure‐property relationships of MOFs and realizing the rapid calculation of molecular diffusivity.
Funder
National Natural Science Foundation of China
Natural Science Foundation of Guangdong Province
China Postdoctoral Science Foundation
Guangzhou Municipal Science and Technology Project
Subject
General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)
Cited by
21 articles.
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