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

Abstract

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.

Recent progress of theoretical studies on electro- and photo-chemical conversion of CO2with single-atom catalysts

“…21 Hai et al found that, for some MOFs, the selectivity of HCOOH depended on the adsorption energy difference between *HCOO and *COOH by DFT calculations. 98 Thus, the biggest obstacle is that HER would severely inhibit eCO 2 RR. 99 Graphite carbonitride (g-C 3 N 4 ) contains unique chemical composition, p-conjugated electronic structure and strong nucleophilic ability.…”

“… 21 Hai et al found that, for some MOFs, the selectivity of HCOOH depended on the adsorption energy difference between *HCOO and *COOH by DFT calculations. 98 Thus, the biggest obstacle is that HER would severely inhibit eCO 2 RR. 99 …”

A Multiobjective Closed-loop Approach Towards Autonomous Discovery of Electrocatalysts for Nitrogen Reduction

“…Our approach here can be contrasted with multiobjective filtering approaches where hard thresholds are defined for each metric based on prior knowledge to screen materials [31][32][33][34].…”

Ligand leaching enabling improved electrocatalytic oxygen evolution performance

“…27 Recently, various MOF candidates were systematically screened through a multiple-step high-throughput screening protocol for high-performance electrocatalysts. 29 Overall, comprehensively regulating the intrinsic activity and the number of accessible active sites in MOFs is expected to break the bottleneck of their electrocatalytic activity, thereby promoting their practical applications.…”