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Identifying the Activation of Bimetallic Sites in NiCo2S4@g‐C3N4‐CNT Hybrid Electrocatalysts for Synergistic Oxygen Reduction and Evolution

Hybrid materials composed of transition‐metal compounds and nitrogen‐doped carbonaceous supports are promising electrocatalysts for various electrochemical energy conversion devices, whose activity enhancements can be attributed to the synergistic effect between metallic sites and N dopants. While the functionality of single‐metal catalysts is relatively well‐understood, the mechanism and synergy of bimetallic systems are less explored. Herein, the design and fabrication of an integrated flexible electrode based on NiCo2S4/graphitic carbon nitride/carbon nanotube (NiCo2S4@g‐C3N4‐CNT) are reported. Comparative studies evidence the electronic transfer from bimetallic Ni/Co active sites to abundant pyridinic‐N in underlying g‐C3N4 and the synergistic effect with coupled conductive CNTs for promoting reversible oxygen electrocatalysis. Theoretical calculations demonstrate the unique coactivation of bimetallic Ni/Co atoms by pyridinic‐N species (a Ni, Co–N2 moiety), which simultaneously downshifts their d‐band center positions and benefits the adsorption/desorption features of oxygen intermediates, accelerating the reaction kinetics. The optimized NiCo2S4@g‐C3N4‐CNT hybrid manifests outstanding bifunctional performance for catalyzing oxygen reduction/evolution reactions, highly efficient for realistic zinc–air batteries featuring low overpotential, high efficiency, and long durability, superior to those of physical mixed counterparts and state‐of‐the‐art noble metal catalysts. The identified bimetallic coactivation mechanism will shed light on the rational design and interfacial engineering of hybrid nanomaterials for diverse applications.