The future of electrochemical energy storage spotlights on the designed formation of highly efficient and robust bifunctional oxygen electrocatalysts that facilitate advanced rechargeable metal-air batteries. We introduce a scalable facile strategy for the construction of a hierarchical three-dimensional sulfur-modulated holey C2N aerogels (S-C2NA) as bifunctional catalysts for Zn-air and Li-O2 batteries. The S-C2NA exhibited ultrahigh surface area (~1943 m2g-1), and superb electrocatalytic activities with lowest reversible oxygen electrode index ~0.65 V, outperforms the highly active bifunctional and commercial (Pt/C & RuO2) catalysts. Density functional theory and experimental results reveal that the favorable electronic structure and atomic coordination of holey C-N skeleton enables the reversible oxygen reactions. The resulting Zn-air batteries with liquid electrolytes and the solid-state batteries with S-C2NA air cathodes exhibit superb energy densities (958 and 862 Wh kg-1), low charge-discharge polarizations, excellent reversibility, and ultra-long cycling lives (750 and 460 h) than the commercial Pt/C+RuO2 catalysts, respectively. Notably, Li-O2 batteries with S-C2NA demonstrated an outstanding specific capacity of ~648.7 mA h g-1 and reversible charge-discharge potentials over 200 cycles, illustrating great potential for commercial next-generation rechargeable power sources of flexible electronics.

Hierarchically designed 3D holey C2N aerogels as bifunctional oxygen electrodes for flexible and rechargeable Zn-air batteries

256th National Meeting (2018)

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