Achieving high selectivity and activity of CO2 electroreduction to formate by in-situ synthesis of single atom Pb doped Cu catalysts

Exploring highly selective and stable electrocatalysts is of great significance for the electrochemical conversion of CO2 into fuel. Herein, a three-dimensional (3D) nanostructure catalyst was developed by doping Pb single-atom (PbSA) in-situ on carbon paper (PbSA100-Cu/CP) through a low-energy and economical method. The designed catalyst exhibited abundant active sites and was beneficial to CO2 adsorption, activation, and subsequent conversion to fuel. Interestingly, PbSA100-Cu/CP showed a prominent Faraday efficiency (FE) of 97 % at –0.9 V versus reversible hydrogen electrode (vs. RHE) and a high partial current density of 27.9 mA·cm−2 for formate. Also, the catalyst remained significantly stable for 60 h during the durability test. The reaction mechanism was investigated by density functional theory (DFT), demonstrating that the doping PbSA induced the electrons redistribution, promoted the formate generation, reduced the rate-determining step (RDS) energy barrier, and inhibited the hydrogen evolution reaction. The study aims to provide a new strategy for developing of single-atom catalysts with high selectivity and stability, which will help reduce environmental pressure and alleviate energy problems.