Finding high-performance MOFs for effective SF₆/N₂ separation through high-throughput computational screening and machine learning

Abstract Given the rapidly expanding pool of synthesized and hypothetical metal–organic frameworks (MOFs), testing every single material for SF 6 /N 2 separation by iterative experimental methods or computationally demanding molecular simulations is not practical. In this study, we integrated high-throughput computational screening and machine learning (ML) approaches to evaluate SF 6 /N 2 mixture adsorption and separation performances of over 25 000 different types of synthesized and hypothetical MOFs (hypoMOFs), representing the largest set of structures studied for SF 6 /N 2 separation to date. SF 6 /N 2 mixture adsorption data that we produced for synthesized MOFs using molecular simulations were utilized to develop ML models to accurately and quickly predict SF 6 and N 2 uptakes, SF 6 /N 2 selectivities, SF 6 working capacities, adsorbent performance scores, and regenerabilities of both synthesized and hypoMOFs. Results showed the MOF space that we studied exhibits very high SF 6 /N 2 selectivities in the range of 1.8–4204 at 1 bar in addition to high SF 6 working capacities between 0.04–5.68 mol kg −1 at an adsorption pressure of 1 bar and desorption pressure of 0.1 bar at room temperature. The top-performing MOF adsorbents for SF 6 /N 2 mixture separation were identified to have Zn, Cu, Ni metals; terphenyl, pyridine, naphthalene linkers; and medium pore sizes. Our comprehensive computational approach offers a highly efficient alternative to brute-force computer simulations by enabling the rapid assessment of the MOF adsorbents for SF 6 /N 2 separation and provides molecular insights into the key structural features of the most promising adsorbents.