Surface Immobilization of Transition Metal Ions on Nitrogen‐Doped Graphene Realizing High‐Efficient and Selective CO2 Reduction

Electrochemical conversion of CO2 to value‐added chemicals using renewable electricity provides a promising way to mitigate both global warming and the energy crisis. Here, a facile ion‐adsorption strategy is reported to construct highly active graphene‐based catalysts for CO2 reduction to CO. The isolated transition metal cyclam‐like moieties formed upon ion adsorption are found to contribute to the observed improvements. Free from the conventional harsh pyrolysis and acid‐leaching procedures, this solution‐chemistry strategy is easy to scale up and of general applicability, thus paving a rational avenue for the design of high‐efficiency catalysts for CO2 reduction and beyond. A feasible ion‐adsorption strategy is highlighted to bring unprecedentedly efficient and selective CO2 reduction activity to nitrogen‐doped graphene. Free from high‐temperature pyrolysis and acid leaching, this solution‐chemistry route incorporating molecular‐catalyst moieties into a highly conductive carbon matrix provides a practical approach to design high‐efficiency electrocatalysts for CO2 reduction and related catalytic reactions.