▎ 摘　　要

Highly efficient and durable multifunctional catalysts with attractive nanoarchitectures remain challenging for next-generation rechargeable metal-air batteries and water splitting devices. Herein, for the first time, a novel copper molybdenum oxynitride anchored nitrogen-doped graphene (CuMo2ON@NG) is synthesized by a simple, scalable, and cost-effective pyrolysis method. The rational design of CuMo2ON encased in NC shells anchored onto the NG matrix to enhance the electroactive sites and boost the electron-transport behaviors for oxygen reduction/evolution reactions (ORR/OER) and hydrogen evolution reaction (HER). The optimal CuMo2ON@NG reveals tremendous trifunctional activities, outperform benchmark Pt/C and IrO2. First-principles calculations demonstrate that the excellent catalytic activity of CuMo2ON@NG is owing to the synergistic electron transfer between the active CuMo2ON nanoparticles, doped N species, and graphitic carbon. Formation of the O* intermediates on CuMo2ON lattice in the core-shell CuMo2ON@NG nanohybrid is an energetic rate-determining step to attain ORR and OER activities. The CuMo2ON@NG air-cathode based rechargeable quasi solid-state zinc-air battery delivers an ultra-high specific capacity of 736 mAh gzn(-1), an exceptional energy density of 800.75 Wh kg(-1), a record power density of 176.3 mW cm(-2), and excellent reversibility (330 h at 10 mA cm(-2)). Furthermore, the CuMo2ON@NG-based water splitting device achieves a cell voltage of 1.49 V at a current density of 10 mA cm(-2) and excellent reversibility of 120 h at a high current density of 100 mA cm(-2), outperforming the benchmark Pt/C parallel to IrO2 (similar to 1.53 V at 10 mA cm(-2)) and reported state-of-the-art catalysts.