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The compositing strategy offers great potential in designing bifunctional oxygen electrocatalysts for Zn–air batteries. Recent reports reveal that the couple of RuO2, serving as a benchmark oxygen evolution reaction (OER) catalyst, with other oxygen reduction reaction (ORR) catalysts is a wise choice to build highly efficient bifunctional electrocatalysts. However, the design criteria for ORR and OER activities of RuO2‐based composite catalysts are still unclear. Herein, a series of transition metal (Fe, Co, Mn, and Ni)‐doped spinel oxides are designed to support RuO2 nanorods for exploring the reaction mechanism. Through advanced technology, it is considered that increasing the content and binding energy of Co3+ and enhancing the oxidation state of Ru4+ is an efficient strategy to promote ORR and OER activities for RuO2/Co‐based spinel oxide composite catalysts. It is found that coupling Mn‐doping Co3O4 (CMO) supports with RuO2 can induce the highest catalytic activities in ORR/OER and excellent performance in rechargeable Zn–air batteries. Operando electrochemical impedance spectroscopy and theoretical calculation further prove the synergistic effect between RuO2 and CMO supports originated from the oxygen overflow to overcome the large barrier for oxygen desorption on RuO2 during OER and oxygen adsorption on CMO supports during ORR. [ABSTRACT FROM AUTHOR]

The self‐catalyzed growth of nanostructures on material surfaces is one of the most time‐ and cost‐effective ways to design multifunctional catalysts for a wide range of applications. Herein, the use of this technique to develop a multicomponent composite catalyst with CoSx core encapsulated in an ultrathin porous carbon shell entangled with Co, N‐codoped carbon nanotubes is reported. The as‐prepared catalyst has a superior catalytic activity for oxygen evolution and oxygen reduction reactions, an ultralow potential gap of 0.74 V, and outstanding durability, surpassing most previous reports. Such superiority is ascribed, in part, to the unique 3D electrode architecture of the composite, which is favorable for transporting oxygen species and electrons and creates a synergy between the components with different functionalities. Moreover, the flexible solid Zn–air battery assembled with such an air electrode shows a steady discharge voltage plateau of 1.25 V and a round‐trip efficiency of 70% at 1 mA cm−2. This work presents a simple strategy to design highly efficient bifunctional oxygen electrocatalysts and may pave the way for the practical application of these materials in many energy conversion/storage devices. [ABSTRACT FROM AUTHOR]