Engineered Atom-Particle Coupling in Dice-Like Hollow Carbon Cages Accelerates Oxygen Electrocatalysis for Efficient Zinc-Air Batteries.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41974614.
- Also identified by DOI 10.1021/acs.nanolett.6c00844 and PMC identifier 13133904.
- Licence recorded as CC BY-NC-ND.
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Abstract
Sluggish oxygen electrocatalytic kinetics and diffusion limitations remain key barriers to high-performance zinc-air batteries (ZABs). Herein, we report a dice-like Co/N codoped hollow carbon cage catalyst (Co/N-HCC) featuring efficient atom-particle coupled Co single atoms and nanoparticles (Co<sub>SA</sub>&Co<sub>NP</sub>) confined within a hierarchically porous framework via a self-templated surface-confinement strategy. Calculations and in situ spectroelectrochemical experiments suggest that the atom-particle electronic coupling triggers substantial interfacial charge redistribution and tunes the d-band center of Co-N<sub>4</sub> moieties, thereby regulating oxygenated intermediate adsorption and accelerating interfacial electron transfer. Remarkably, the tailored Co/N-HCC achieved superior bifunctional electrocatalytic activity with a low potential gap of 0.63 V in alkaline media. Furthermore, the Co/N-HCC-based ZAB delivers a high peak power density of 269.1 mW cm<sup>-2</sup>, a specific capacity of 813.6 mAh g<sup>-1</sup>, and robust cycling durability. This work elucidates a mechanistic paradigm for integrating atom-particle electronic coupling with hierarchical porosity toward advanced oxygen electrocatalysts.