Abstract

Converting CO2 into valuable chemicals using electrocatalysis is an attractive approach for sustainable energy storage and artificial carbon cycle. In this study, atomically dispersed Ir species (Ad-Ir) that are supported on three-dimensional (3D) porous carbon networks are proposed as electrocatalysts for highly efficient CO2 conversion. The resulting catalysts can preferentially and rapidly produce CO with a high Faradaic efficiency of 95.6 % and a very high turnover frequency (TOF) value of 33,365 h−1. Furthermore, it shows no obvious decay in both FE for CO and current density over 20 h of continuous operation. Based on detailed experimental studies and density functional theory (DFT) calculations, such outstanding catalytic performance for CO2 conversion to CO production can be attributed to the structural advantages of 3D network of porous carbon and atomically dispersed Ir species on the 3D carbon support.

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