Revealing Isolated M−N3C1 Active Sites for Efficient Collaborative Oxygen Reduction Catalysis

Abstract Single atom catalysts (SACs) are of great importance for oxygen reduction, a critical process in renewable energy technologies. The catalytic performance of SACs largely depends on the structure of their active sites, but explorations of highly active structures for SAC active sites are still limited. Herein, we demonstrate a combined experimental and theoretical study of oxygen reduction catalysis on SACs, which incorporate M−N 3 C 1 site structure, composed of atomically dispersed transition metals (e.g., Fe, Co, and Cu) in nitrogenated carbon nanosheets. The resulting SACs with M−N 3 C 1 sites exhibited prominent oxygen reduction catalytic activities in both acidic and alkaline media, following the trend Fe−N 3 C 1 > Co−N 3 C 1 > Cu−N 3 C 1 . Theoretical calculations suggest the C atoms in these structures behave as collaborative adsorption sites to M atoms, thanks to interactions between the d / p orbitals of the M/C atoms in the M−N 3 C 1 sites, enabling dual site oxygen reduction.