Combining Machine Learning and Molecular Simulations to Unlock Gas Separation Potentials of MOF Membranes and MOF/Polymer MMMs

[Image: see text] Due to the enormous increase in the number of metal-organic frameworks (MOFs), combining molecular simulations with machine learning (ML) would be a very useful approach for the accurate and rapid assessment of the separation performances of thousands of materials. In this work, we combined these two powerful approaches, molecular simulations and ML, to evaluate MOF membranes and MOF/polymer mixed matrix membranes (MMMs) for six different gas separations: He/H(2), He/N(2), He/CH(4), H(2)/N(2), H(2)/CH(4), and N(2)/CH(4). Single-component gas uptakes and diffusivities were computed by grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations, respectively, and these simulation results were used to assess gas permeabilities and selectivities of MOF membranes. Physical, chemical, and energetic features of MOFs were used as descriptors, and eight different ML models were developed to predict gas adsorption and diffusion properties of MOFs. Gas permeabilities and membrane selectivities of 5249 MOFs and 31,494 MOF/polymer MMMs were predicted using these ML models. To examine the transferability of the ML models, we also focused on computer-generated, hypothetical MOFs (hMOFs) and predicted the gas permeability and selectivity of 1000 hMOF/polymer MMMs. The ML models that we developed accurately predict the uptake and diffusion properties of He, H(2), N(2), and CH(4) gases in MOFs and will significantly accelerate the assessment of separation performances of MOF membranes and MOF/polymer MMMs. These models will also be useful to direct the extensive experimental efforts and computationally demanding molecular simulations to the fabrication and analysis of membrane materials offering high performance for a target gas separation.