The development of nanocomposites with unique structures by combining perovskites (ABO 3 ) is of significant importance for improving oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The introduction of transition metals in active B sites is considered a useful pathway to regulate the chemical and electronic properties of perovskites. In this study, a bifunctional activity-enhanced La(Ni 0.1 )MnO 3 perovskite decorated with N-doped carbon (NC) is developed by a B-site doping strategy. The resulting La(Ni 0.1 )MnO 3 @NC catalyst possesses numerous benefits including unique morphology, controllable synthesis, high conductivity, bifunctional activity, and durability. The enhancement was attributed to the synergistic effect of Ndoped porous carbon and [MnO 6 ] with the incorporation of [NiO 6 ], resulting in the regulated charge redistribution and disorder degree. Remarkably, the rechargeable Zn−air battery assembled with La(Ni 0.1 )MnO 3 @NC in the air cathode also displays satisfactory performance due to the regulation of coordination units when compared with a commercial catalyst. This study shows that the catalytic performance of perovskite oxide-based electrocatalysts can be significantly improved by B-site regulation and allows for the construction of effective cathode catalysts for metal−air batteries.

Rational design of effective non‐precious metal for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is urgently demanded for flexible metal‐air batteries. Engineering heterointerfaces between metal compounds is an attractive strategy for fabricating high‐performance bifunctional electrocatalysts. Herein, a facile spontaneous sulfurization strategy is developed to fabricate the self‐supporting electrode consisting of homogeneous Co3S4 and ZnS on MoS2 with abundant sulfur vacancies, as well as the unique heterointerfaces and conductive carbon skeleton. Owing to the hierarchical structure and more exposed active sites, the optimal Co(Zn0.5)@MoS2/CC electrode exhibits excellent bifunctional catalytic activity with the smaller ΔE value (Ej=10,OER−E1/2,ORR) and durability. Furthermore, Co(Zn0.5)@MoS2/CC based all‐solid‐state zinc‐air and aluminum‐air batteries also deliver high open‐circle voltage, desirable power density and flexibility. This approach offers a novel method to obtain the self‐supporting electrodes with porous structure and highly active metal sulfides.

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