A Zeolitic‐Imidazole Frameworks‐Derived Interconnected Macroporous Carbon Matrix for Efficient Oxygen Electrocatalysis in Rechargeable Zinc–Air Batteries

Nanostructures derived from zeolitic‐imidazole frameworks (ZIFs) gain much interest in bifunctional oxygen electrocatalysis. However, they are not satisfied well for long‐life rechargeable zinc–air batteries due to the limited single particle morphology. Herein, the preparation of an interconnected macroporous carbon matrix with a well‐defined 3D architecture by the pyrolysis of silica templated ZIF‐67 assemblies is reported. The matrix catalyst assembled zinc–air battery exhibits a high power density of 221.1 mW cm−2 as well as excellent stability during 500 discharging/charging cycles, surpassing that of a commercial Pt/C assembled battery. The synergistic effect from the interconnected macroporous structure together with abundant cobalt–nitrogen–carbon active sites justify the excellent electrocatalytic activity and battery performance. Considering the advanced nanostructures and performance, the as‐synthesized hybrid would be promising for rechargeable zinc–air batteries and other energy technologies. This work may also provide significant concept in the view of electrocatalysis design for long‐life battery. An interconnected macroporous carbon matrix is prepared by the pyrolysis of a silica‐templated zeolitic‐imidazole framework assembly. The interconnected macroporous structure with abundant accessible active sites significantly improves the mass transport and accelerates the diffusion of reactants, thus contributing to efficient and robust bifunctionality for oxygen electrocatalysis and achieving long‐life rechargeable zinc–air batteries.