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Abstract Rechargeable Zn‐air batteries (ZAB) represent a promising avenue for sustainable energy storage, boasting high energy density, cost‐effectiveness, scalability, and environmental friendliness. However, the sluggish redox kinetics and limited cycle life of bifunctional oxygen evolution/reduction (OER/ORR) electrocatalysts impede the further practical development of ZABs. In this study, homogenic boundary effect within α/β‐NiMoO 4 is introduced as a superior electrocatalyst for ZAB. Through in situ poikilothermic X‐ray diffraction, X‐ray absorption spectroscopy, and theoretical investigations, the active Ni atoms exhibit more effective electron transfer at α/β‐NiMoO 4 due to the homogenic boundary effect is unveiled. Furthermore, the presence of oxygen vacancies and lattice distortions at these boundaries significantly reduces the thermodynamic barrier of OER to a mere 0.46 V. Consequently, α/β‐NiMoO 4 demonstrates a remarkably low overpotential of 270 mV at 10 mA cm −2 for the bottlenecked OER, along with prolonged durability (150 h) and a high specific capacity (745 mAh g −1 at 5 mA cm −2 ) for ZAB. This study underscores the efficacy of homogenic boundary effects in enhancing electrocatalytic activities, offering great promise for the advancement of sustainable energy systems.
Zhu et al. (Tue,) studied this question.