Gaining molecular insights into structure-performance relations of MOFs via high-throughput computational screening

Abstract

High-throughput computational screening (HTCS) has emerged as a powerful tool for gaining molecular-level insights into the complex structure-performance relationships of metal-organic frameworks (MOFs) in gas separation applications. In this mini-review, we examined how HTCS has advanced our understanding of adsorption-based separation performance of MOFs by systematically evaluating large number of materials using molecular simulations. We first visited the fundamental principles of HTCS workflows, including the selection of databases and the performance metrics used to rank materials. Pioneering and representative studies that explicitly correlate structural descriptors with performance metrics were then reviewed, highlighting how statistically meaningful trends derived from large MOF datasets enable the identification of top materials. Emphasis was given to emerging HTCS investigations targeting gas separations such as H2 purification, CO separation, NH3 capture, and air separation. Finally, we discussed the current opportunities and limitations of HTCS in deriving robust structure-performance relations that can guide the selection of existing materials and the rational design of new MOFs.