Boosting Oxygen Reduction for High-Efficiency H2O2 Electrosynthesis on Oxygen-Coordinated Co-N-C Catalysts

Hangjia Shen*, Nianxiang Qiu, Liu Yang, Xuyun Guo, Kun Zhang, Tiju Thomas, Shiyu Du, Qifu Zheng, J. Paul Attfield, Ye Zhu, Minghui Yang

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract / Description of output

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-N4 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.

Original languageEnglish
Article number2200730
JournalSmall
Volume18
Issue number17
Early online date24 Apr 2022
DOIs
Publication statusE-pub ahead of print - 24 Apr 2022

Keywords / Materials (for Non-textual outputs)

  • atomic coordinates
  • Co -N -C
  • high-efficiency H O electrosynthesis
  • hydrogen peroxide
  • oxygen reduction

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