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Abstract Effective integration of multiple active moieties and strategic engineering of coordinated interfacial junctions are crucial for optimizing the reaction kinetics and intrinsic activities of heterogeneous electrocatalysts. Herein, a simple integrated heterostructure of biphasic Co 0.7 Fe 0.3 /Fe 3 C embedded on in situ grown N‐doped carbon sheets is constructed. Rationally designed CoFe/Fe 3 C‐T 2 owns more accessible active sites and interfacial junction effects, cooperatively boosting the electron and mass transfer, needed for multifunctional electrocatalysis. Leveraging the synergistic effect of dual active sites, CoFe/Fe 3 C‐T 2 demonstrates outstanding oxygen electrocatalytic activity in alkaline medium with an ultra‐low potential gap of 0.58 V, surpassing the recently available state‐of‐the‐art catalysts. Moreover, CoFe/Fe 3 C‐T 2 air‐electrode achieves a high peak power density of 249 mW cm −2 , a large specific capacity of 808 mAh g −1 and excellent cycling stability for aqueous Zn‐air batteries. Remarkably, the solid‐state flexible ZAB also exhibits satisfactory performance, showcasing an open‐circuit voltage of 1.43 V and a peak power density of 66 mW cm −2 . These outstanding results push this catalyst to the top of the list of non‐noble metal‐based electrode materials. This work offers a viable method for using the active‐site‐uniting strategy to create double‐active‐site catalysts, which may find real‐time applications in energy conversion/storage devices.
Das et al. (Sun,) studied this question.