期刊
SMALL
卷 18, 期 17, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202200730
关键词
atomic coordinates; Co; -N; -C; high-efficiency H; O-2; (2) electrosynthesis; hydrogen peroxide; oxygen reduction
类别
资金
- Natural Science Foundation of China [61971405]
- Zhejiang National Science Fund for Distinguished Young Scholars [LR20B010001]
- Department of Science and Technology
- Ningbo 3315 program
In this study, a novel single-atom electrocatalyst (Co/NC) with a specifically penta-coordinated Co-N-C configuration is reported. The unique atomic structure improves the selectivity and turnover frequency of the catalyst for H2O2 electrosynthesis, outperforming the state-of-the-art carbon-based catalysts.
Atomically dispersed Co-N-C is a promising material for H2O2 selective electrosynthesis via a two-electron oxygen reduction reaction. However, the performance of typical Co-N-C materials with routine Co-N-4 active center is insufficient and needs to be improved further. This can be done by fine-tuning its atomic coordination configuration. Here, a single-atom electrocatalyst (Co/NC) is reported that comprises a specifically penta-coordinated Co-N-C configuration (O-Co-N2C2) with Co center coordinated by two nitrogen atoms, two carbon atoms, and one oxygen atom. Using a combination of theoretical predictions and experiments, it is confirmed that the unique atomic structure slightly increases the charge state of the cobalt center. This optimizes the adsorption energy towards *OOH intermediate, and therefore favors the two-electron ORR relevant for H2O2 electrosynthesis. In neutral solution, the as-synthesized Co/NC exhibits a selectivity of over 90% over a potential ranging from 0.36 to 0.8 V, with a turnover frequency value of 11.48 s(-1); thus outperforming the state-of-the-art carbon-based catalysts.
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