Crafting a robust, high-performance, non-precious metal-based flexible air electrode is crucial for realizing flexible zinc-air batteries (ZABs). Herein, hierarchical MoO2 and MoS2 heterojunction nanosheets grown on carbon cloth (CC) are prepared through a simple hydrothermal reaction followed by calcination. Afterward, through self-assembly and high-temperature carbonization of zeolitic imidazolate framework-67 (ZIF-67) and Materials of Institute Lavoisier-101 (MIL-101) on the heterojunction nanosheets, a hierarchical structure of nitrogen-doped carbon (NC) encapsulated CoFe alloy nanoparticles (NPs) supported on MoO2@MoS2 heterojunction nanosheets (CC/MoS2@MoO2@CoFe) is obtained. It exhibits remarkable activity and durability for both bifunctional oxygen evolution and reduction reactions (OER/ORR), attributed to the ternary heterojunction formed by NC-coated CoFe alloy NPs uniformly dispersed among the MoO2@MoS2 nanosheets, along with oxygen vacancies at heterogeneous interfaces between MoS2, MoO2, and Co0.72Fe0.28 alloy. As a binder-less self-supporting electrode, the assembled aqueous ZAB demonstrates a maximum power density of 113.6 mW cm–2, surpassing that of Pt/C + RuO2 (75.2 mW cm–2), along with excellent cycling stability. Furthermore, the CC/MoS2@MoO2@CoFe-based flexible ZABs achieve a maximum power density of 54.1 mW cm–2, exhibit good cycling stability for up to 120 cycles, and show outstanding flexibility. This study paves the way for the practical integration of flexible ZABs into wearable electronic devices, heralding a new era of portable power solutions.
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