Abstract

AbstractFine regulation of the physicochemical structure of carbon‐based electrocatalysts to optimize the adsorption energies of oxygen intermediates is critically important to enhance the reaction kinetics of the oxygen evolution/reduction reaction (OER/ORR) but remains a huge challenge. Herein, nano‐space confined growth of Co9S8 nanoparticles (NPs) in porous carbon is realized through an in situ confined growth strategy by using thiol‐chains functionalized COF (COF‐S‐SH) as a confined template. COF‐S‐SH is used as binding sites to immobilize Co ions to improve the interaction between metal nanoparticles (NPs) and carbon skeletons, and simultaneously serves as a confined void to avoid the aggregation metal NPs. Impressively, as an efficient bifunctional catalyst, the resulting Co9S8/COF‐S800 shows significantly enhanced oxygen electrocatalysis with a small OER‐ORR voltage gap of 0.76 V, vastly superior to that of pristine COF‐S800. Furthermore, the assembled Zn–air battery with Co9S8/COF‐S800 catalyst displays a high peak power density of 181.5 mW cm−2 and great durability over 60 h charge–discharge cycles.

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