Abstract
Rational design of oxygen reduction reaction (ORR) electrocatalysts with indestructible active sites for high-performance Zn-air batteries (ZABs) remains a significant challenge. Herein, we achieve an innovative active site design by encaging Co nanoparticles within the Co−N4 atomic sites-dispersed graphite nanopocket (CoSAs-NPs/NC), leading to outstanding alkaline ORR activity and stability, and consequently ultra-high power density of 193.8 mW cm–2 and specific capacity of 819.1 mAh gZn–1 at 10 mA cm–2 of a primary ZAB assembled, along with impressive power density of 73.4 mW cm–2 and charging/discharging stability up to 110 cycles of a flexible solid-state ZAB. Theoretical calculations unveil the enhanced ORR kinetics can be traced to the significantly optimized local electronic structure of Co−N4 sites with upshifted d-band center and reduced energy barrier of rate-limiting step by the encaged Co nanoparticle. This study showcases a creative conformational design for guiding the construction of valid synergy in hybridized metal/single-atom catalysts.
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