Hierarchically Designed 3D Holey C<sub>2</sub>N Aerogels as Bifunctional Oxygen Electrodes for Flexible and Rechargeable Zn-Air Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 29262251.
- Also identified by DOI 10.1021/acsnano.7b07473.
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Abstract
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 C<sub>2</sub>N aerogels (S-C<sub>2</sub>NA) as bifunctional catalysts for Zn-air and Li-O<sub>2</sub> batteries. The S-C<sub>2</sub>NA exhibited ultrahigh surface area (∼1943 m<sup>2</sup> g<sup>-1</sup>) and superb electrocatalytic activities with lowest reversible oxygen electrode index ∼0.65 V, outperforms the highly active bifunctional and commercial (Pt/C and RuO<sub>2</sub>) catalysts. Density functional theory and experimental results reveal that the favorable electronic structure and atomic coordination of holey C-N skeleton enable the reversible oxygen reactions. The resulting Zn-air batteries with liquid electrolytes and the solid-state batteries with S-C<sub>2</sub>NA air cathodes exhibit superb energy densities (958 and 862 Wh kg<sup>-1</sup>), low charge-discharge polarizations, excellent reversibility, and ultralong cycling lives (750 and 460 h) than the commercial Pt/C+RuO<sub>2</sub> catalysts, respectively. Notably, Li-O<sub>2</sub> batteries with S-C<sub>2</sub>NA demonstrated an outstanding specific capacity of ∼648.7 mA h g<sup>-1</sup> and reversible charge-discharge potentials over 200 cycles, illustrating great potential for commercial next-generation rechargeable power sources of flexible electronics.