Cognate Cobalt Core‐Shell Structure Decorated Nitrogen‐Doped Hollow Carbon Bowls Triggering Advanced Zinc‐Air Battery

Abstract It is of paramount importance but challenging to construct interface structure in metals with good interfacial compatibility and high conductivity to yield superior bifunctional oxygen electrocatalyst for rechargeable Zn‐air battery (ZAB). In this work, bowl‐like hybrid structures have been designed and fabricated by decorating cognate cobalt core‐shell structure on the N‐doped hollow porous carbon bowls. Such a unique design not only can systematically boost the advantages of hollow porous bowl‐like structure but also demonstrate the universality of synthetic strategy. The experimental and density functional theory calculations elucidate that the excellent bifunctional electrocatalytic activity (ΔE = 0.71 V) of the hybrid catalyst is attributed to the spontaneous integration of a conductive Co metal core with cognate active Co 3 O 4 shell (≈ 4 nm). The core‐shell configuration facilitates the optimization of the desorption/adsorption energy barriers for oxygen‐containing intermediates through efficient electron transfer mediated by the heterogeneous structure. As a flexible ZAB cathode, the cognate cobalt catalyst exhibits long‐term durability (60 h at 1 mA cm −2 ) and excellent bendable stability, demonstrating its promising potential in practical applications.