Isolated FeN(4) Sites for Efficient Electrocatalytic CO(2) Reduction

The construction of isolated metal sites represents a promising approach for electrocatalyst design toward the efficient electrochemical conversion of carbon dioxide (CO(2)). Herein, Fe‐doped graphitic carbon nitride is rationally prepared by a simple adsorption method and is used as template to construct isolated FeN(4) sites through a confined pyrolysis strategy, which avoids the agglomeration of metal atoms to particles during the synthesis process and thus provides abundant active sites for the CO(2) reduction reaction. The isolated FeN(4) sites lower the energy barrier for the key intermediate in the CO(2) reduction process, leading to the enhanced selectivity for CO production with a faradaic efficiency of up to 93%.