High-Throughput Computational Screening of Metal–Organic Frameworks for Thiol Capture

Abstract

We report high-throughput computational screening of 137 953 hypothetical metal–organic frameworks (hMOFs) and 4764 computation-ready experimental MOFs (CoRE-MOFs) for the capture of thiols (methanethiol and ethanethiol) from air. To minimize the competitive adsorption of moisture, 31 816 hydrophobic MOFs are first identified on the basis of a threshold criterion in the Henry constant of water, and then used to assess the adsorption capacity of thiol (NSH) and the selectivity of thiol over air (SSH/Air). The highest NSH and SSH/Air are predicted to be 70.86 mg/g and 2.6 × 107, respectively. Most of the high-performance MOFs are found to be hMOFs. The structure–property relationships are derived for NSH and SSH/Air with MOF descriptors (including the isosteric heat, the largest cavity diameter, surface area, and void fraction). While the relationship with isosteric heat tends to be monotonic, there exist optimal ranges in the other relationships. Principal component analysis is applied to assess the interr...