High-Throughput Computational Screening of Metal–Organic Frameworks as High-Performance Electrocatalysts for CO2RR

Metal–organic frameworks (MOFs) are considered as promising electrocatalytic materials for the carbon dioxide reduction reaction (CO2RR) due to their various excellent properties. Here, through multistep high-throughput screening of the Computation-Ready, Experimental (CoRE) MOF database, including structural rationality check, pore size screening, adsorption capacity prediction, open metal site identification, CO2 molecular activation capacity, and reaction path calculation, MOFs named GAFRUD, CAJQEL, and cg400449c are identified as potential catalysts for electrocatalytic CO2RR. Furthermore, based on density functional theory calculations, we propose that the polarity of the coordination bonds between the metal atoms and the coordination atoms in ligands has a significant impact on the activation of CO2 molecules, and the selectivity of HCOOH mainly depends on the adsorption energy difference between *HCOO and *COOH. This principle is further validated by the experimental results, which will provide guidelines for the rational design of MOF-based electrocatalysts for CO2RR.