LAUSR

Engineering transition metal‐nitrogen‐carbon (TM‐N‐C) catalysts with high‐density accessible active sites and optimized electronic structure holds great promise in the context of the electrochemical oxygen reduction reaction (ORR). Herein, a novel modification of a lysozyme‐modified zeolitic imidazolate framework with isolated Co atoms anchored on dominated pyridinic‐N doped carbon (Co‐pyridinic N‐C) is reported. The atomically dispersed Co allows the maximum active site exposure while the introduction of pyridinic N can greatly reduce the electron localization around the Co centers and improve the interaction with oxygenated species, and thus lowering the energy barriers of the intermediates and facilitating the favorable four‐electron ORR pathway. Owing to the synergistic effects of single‐atom Co and coordinated pyridinic N, the Co‐pyridinic N‐C catalyst exhibits an exceptional ORR activity and remarkable stability in both alkaline and more challenging acidic media, representing one of the most active Co‐N‐C catalysts reported. This work may open an avenue for the rational design of TM‐N‐C catalysts to boost their catalytic performance for application in the ORR.