Regulating the Microenvironment of Zn‐Based Metal‐Organic Framework for Enhanced CO2 Electroreduction to Formate

Abstract Electrocatalytic CO 2 reduction (ECR) has emerged as one of the most promising strategies to alleviate the energy crisis and CO 2 pollution, for which a wide variety of catalysts are under development. Metal‐organic frameworks (MOFs) with clear and designable structures are an excellent platform for ECR. In this study, two isostructural N, O‐coordinated Zn‐MOFs, FJU‐126‐4F, and FJU‐126‐CH 3 , based on terephthalic acid ligand with different groups (one is ─4F and the other is ─CH 3 ) on the benzene ring, have been constructed for ECR catalysts. Significantly, the different functional groups make the performance difference of ECR. The maximum Faraday efficiency of formate (FE formate ) for FJU‐126‐4F is 60.5% with the partial current density of formate ( j formate ) of −19.35 mA cm −2 at −1.47 V, while the optimum FE formate of FJU‐126‐CH 3 is 50.2% with the j formate of −10.04 mA cm −2 at −1.57 V. This work provides an insight into the rational design of MOF catalysts for ECR.