4.8 Article

Catalytic Oxidation of K2S via Atomic Co and Pyridinic N Synergy in Potassium-Sulfur Batteries

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 41, 页码 16902-16907

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c06255

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  1. Australian Research Council (ARC) [FL170100154]

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This study reports the catalytic oxidation of K2S on a sulfur host with Co single atoms immobilized on nitrogen-doped carbon. The potassium-sulfur battery exhibited high capacities under high current densities, providing atomic-scale insights for the rational design of highly efficient sulfur hosts.
Potassium-sulfur batteries hold practical promise for next-generation batteries because of their high theoretical gravimetric energy density and low cost. However, significant impediments are the sluggish K2S oxidation kinetics and a lack of atomic-level understanding of K2S oxidation. Here, for the first time, we report the catalytic oxidation of K2S on a sulfur host with Co single atoms immobilized on nitrogen-doped carbon. On the basis of combined spectroscopic characterizations, electrochemical evaluation, and theoretical computations, we show a synergistic effect of dynamic Co-S and N-K interactions to catalyze K2S oxidation. The resultant potassium-sulfur battery exhibited high capacities of 773 and 535 mAh g(-1) under high current densities of 1 and 2 C, respectively. These findings provide atomic-scale insights for the rational design of highly efficient sulfur hosts.

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