Computer-Aided Discovery of MOFs with Calixarene-Analogous Microenvironment for Exceptional SF<sub>6</sub> Capture
Jiahao Ren, Miao Chang, Wenjiang Zeng, Yuanhua Xia, Dahuan Liu, Guillaume Maurin, Qingyuan Yang
Abstract
Finding optimal adsorbents to achieve an efficient capture and recovery of sulfur hexafluoride (SF6) from SF6/N2 mixture is of great industrial importance. To address this key challenge, here we present a materials-genomics-accelerated strategy by integrating high-throughput computational screening with subsequent synthesis and adsorption/separation testing of the identified promising material. From over 10140 metal–organic frameworks (MOFs), those with calixarene-analogous pore feature were computationally identified as optimal adsorbents with exceptional SF6/N2 selectivity and SF6 uptake. The separation mechanism was revealed to be thermodynamically driven owing to the synergistic contribution of multiple hydrogen-bond and van der Waals-type SF6/MOF pore wall interactions. As a proof-of-concept, one of the discovered MOFs was further synthesized, and equilibrium adsorption measurements demonstrated both record SF6 adsorption capacity as a single component at 0.1 bar (3.39 mmol g–1) and SF6/N2 IAST-predicted selectivity (∼266) under ambient conditions. Besides its excellent regeneration and cycling performance, dynamic breakthrough experiments further confirmed the attractiveness of this MOF for SF6 capture under working conditions.