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Exploring high-efficiency, low-cost, and long-life bifunctional self-supporting electrocatalysts is of great significance for the practical application of advanced rechargeable Zn-air batteries (ZABs), especially flexible solid-state ZABs. Herein, ultrathin CoFe-layered double hydroxide (CoFe-LDH) nanosheets are strongly coupled on the surface of leaf-like bimetallic metal-organic frameworks (MOFs)-derived hybrid carbon (Co@NC) nanoflake nanoarrays supported by carbon cloth (CC) via a facile and scalable method for rechargeable and flexible ZABs. This interfacial engineering for CoFe-LDHs on Co@NC improves the electronic conductivity of CoFe-LDH nanosheets as well as achieves the balance of oxygen evolution reduction (OER) and oxygen reduction reaction (ORR) activity. The unique three-dimensional (3D) open interconnected hierarchical structure facilitates the transport of substances during the electrochemical process while ensuring adequate exposure of OER/ORR active centers. When applied as an additive-free air cathode in rechargeable liquid ZABs, CC/Co@NC/CoFe-LDH-700 demonstrates high open-circuit potential of 1.47 V, maximum power density of 129.3 mW cm -2 , and satisfactory specific capacity of 710.7 mAh g -1  Zn . Further, the flexible all-solid-state ZAB assembled by CC/Co@NC/CoFe-LDH-700 displays gratifying mechanical flexibility and stable cycling performance over 40 h. More significantly, the series-connected flexible ZAB is further verified as a chain power supply for LED strips and performs well throughout the bending process, showing great application prospects in portable and wearable electronics. This work sheds new light on the design of high-performance self-supporting non-precious metal bifunctional electrocatalysts for OER/ORR and air cathodes for rechargeable ZABs.

polymers

Interfacial Engineering of Leaf-like Bimetallic MOF-Based Co@NC Nanoarrays Coupled with Ultrathin CoFe-LDH Nanosheets for Rechargeable and Flexible Zn-Air Batteries