A replacement strategy for regulating local environment of single-atom Co-SxN4−x catalysts to facilitate CO2 electroreduction

Jiajing Pei, Huishan Shang, Junjie Mao, Zhe Chen, Rui Sui, Xuejiang Zhang, Danni Zhou, Yu Wang, Fang Zhang, Wei Zhu, Tao Wang*, Wenxing Chen*, Zhongbin Zhuang*

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

25 引用 (Scopus)

摘要

The performances of single-atom catalysts are governed by their local coordination environments. Here, a thermal replacement strategy is developed for the synthesis of single-atom catalysts with precisely controlled and adjustable local coordination environments. A series of Co-SxN4−x (x = 0, 1, 2, 3) single-atom catalysts are successfully synthesized by thermally replacing coordinated N with S at elevated temperature, and a volcano relationship between coordinations and catalytic performances toward electrochemical CO2 reduction is observed. The Co-S1N3 catalyst has the balanced COOH*and CO* bindings, and thus locates at the apex of the volcano with the highest performance toward electrochemical CO2 reduction to CO, with the maximum CO Faradaic efficiency of 98 ± 1.8% and high turnover frequency of 4564 h−1 at an overpotential of 410 mV tested in H-cell with CO2-saturated 0.5 M KHCO3, surpassing most of the reported single-atom catalysts. This work provides a rational approach to control the local coordination environment of the single-atom catalysts, which is important for further fine-tuning the catalytic performance.

源语言英语
文章编号416
期刊Nature Communications
15
1
DOI
出版状态已出版 - 12月 2024

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