Abstract

Substituting costly Pt-based oxygen reduction reaction (ORR) catalysts with highly active and stable non-precious metal catalysts is a great challenge in zinc-air batteries. Herein, we fabricated Co/Co9S8 nanoparticles decorated nitrogen, sulfur dual-doped carbon leaves (Co/Co9S8-NCL) with outstanding ORR performance by pyrolysis of dithiooxamide (DTO) molecule modified two-dimensional (2D) leaf-shaped zeolitic imidazolate framework (ZIF-L). The functionality of DTO simultaneously optimizes 2D nanostructure and component (S doping) by the confinement effect due to the coordination interaction between S atoms of DTO and Co2+ in ZIF-L. Benefiting from the synergistic effect between Co-Nx sites and Co/Co9S8 species coupled with unique two-dimensional N, S-codoped carbon leaves, the resulting Co/Co9S8-NCL-30 exhibits a remarkable ORR activity with a half-wave potential of 0.852 V comparable to Pt/C (0.843 V) and outstanding long-term stability. Impressively, the Zn-air battery with Co/Co9S8-NCL-30 achieves high power density of 112 mW cm−2 and specific capacity of 799 mAh g−1Zn. This work will present a new pathway to prepare highly active and durable 2D transition metal-based carbon nanomaterials in zinc-air batteries.

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