期刊
ENERGY STORAGE MATERIALS
卷 59, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.ensm.2023.102790
关键词
Single atom; N-enriched; Submicron carbon spheres; Oxygen reduction reaction; Zn-air battery
Fe single atoms anchored on N-enriched porous submicron carbon spheres (FeSA/ N-PSCS) were fabricated by a N-rich heterocycle regulated supramolecular coordination self-assembly strategy, exhibiting ultra-high N-dopant content and optimized FeNx configuration, leading to the highest level of catalytic activity in oxygen reduction reaction (ORR).
Nitrogen-doped carbon supported metal single-atom catalysts (M-N-C SACs), especially Fe-N-C SACs appear as very promising catalysts for oxygen reduction reaction (ORR). However, precisely modulating of the Fe-Nx configuration and geometric microenvironment in Fe-N-C SACs to achieve the highest level of catalytic activity remains grand challenges. Herein, we describe a N-rich heterocycle regulated supramolecular coordination selfassembly strategy to fabricate Fe single atoms anchored on N-enriched porous submicron carbon spheres (FeSA/ N-PSCS), with ultra-high N-dopant content (14.81 at.%) for facilitating the formation of atomically dispersed FeN4. Density functional theory calculations validate that N-doping at the periphery of the Fe-N4 active sites optimizes the adsorption of oxygen-containing intermediates and significantly reduces the ORR overpotential. Benefitting from the localized N-enriched atomic configuration, highly microporous, and regular submicronspherical structure, FeSA/N-PSCS exhibit enhanced ORR performance. More importantly, FeSA/N-PSCS catalyzed Zn-air battery (ZAB) outperforms Pt/C+RuO2-based ZAB in the aspects of maximum power density, specific capacity and cycling stability.
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