Abstract

Developing highly efficient oxygen electrocatalysts is of vital importance for rechargeable Zn-air batteries (ZABs). Herein, Co/CoOx nano-heterojunctions encapsulated into nitrogen-doped carbon sheets (NCS@Co/CoOx) are fabricated via a dual-template-guided approach by using zeolitic imidazolate frameworks (ZIFs) as templates. The synergistic integration of structural and compositional advantages endows such catalyst with superior catalytic properties to benchmark noble-metal catalysts. To be specific, the hierarchical micro/mesopores affords massive mass transport channels and maximizes the exposure of accessible active sites, whereas the NCS matrix accelerates electron transfer and prevents the self-aggregation of active species during the electrocatalytic reaction. Moreover, abundant and synergistic Co-based active sites (CoO, Co3O4, Co-Nx) greatly promote the catalytic activity. As the cathode of both liquid and flexible solid-state ZABs, excellent device properties are achieved, outperforming those assembled with commercial Pt/C+RuO2 catalyst. This work presents a feasible and cost-effective strategy for developing oxygen electrocatalysts derived from ZIFs templates.

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