Citation: Yongliang Ban, Meng Zhang, Jianya He, Chunfeng Shao, Zhongliao Wang, Wei Zhao, Kai Dai. Atomically dispersed Fe–N₄ sites on g–C₃N₄ enable highly selective CO₂–to–CO electrocatalysis[J]. Chinese Chemical Letters, ;2026, 37(4): 112096. doi: 10.1016/j.cclet.2025.112096 shu

Atomically dispersed Fe–N₄ sites on g–C₃N₄ enable highly selective CO₂–to–CO electrocatalysis

Yongliang Ban ^{a, 1} ,
Meng Zhang ^{b, 1} ,
Jianya He ^b ,
Chunfeng Shao ^{b, *,} ,
Zhongliao Wang ^{b, *,} ,
Wei Zhao ^{c, *,} ,
Kai Dai ^{a, b, *,}

a.
School of Chemistry and Chemical Engineering, Zhoukou Normal University, Zhoukou 466001, China
b.
Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Anhui Province Key Laboratory of Pollutant Sensitive Materials and Environmental Remediation, School of Chemistry and Chemical Engineering, School of Energy Science and Engineering, Huaibei Normal University, Huaibei 235000, China
c.
Songshan Lake Materials Laboratory, Dongguan 523808, China

shaocf@chnu.edu.cn

wangzl@chnu.edu.cn

zhaowei@sslab.org.cn

daikai940@chnu.edu.cn

Received Date: 19 July 2025
Revised Date: 6 November 2025
Accepted Date: 10 November 2025
Available Online: 11 November 2025

Figures(4)

The development of efficient and cost-effective non-precious-metal single-atom catalysts (SACs) is crucial for advancing the practical application of electrocatalytic CO₂ reduction (CO₂RR). However, identifying highly active metal atoms and designing catalysts with uniform active center structures remain significant challenges. To address this, we developed a generic pyrolysis method to synthesize a series of transition metal-based SACs with atomically dispersed metal anchored on carbon nitride support (M-C₃N₄, M = Fe, Ni, Cu). Benefiting from the unique electronic structure of the Fe-N₄ sites supported on C₃N₄, the Fe-C₃N₄ catalyst demonstrated exceptional performance, achieving a CO Faradaic efficiency of 99.6% and maintaining excellent stability. Theoretical calculations indicate that the Fe site exhibits a relatively stronger interaction with the ^*COOH intermediate, thereby helping to lower the energy barrier of the CO₂ protonation process. This study provides valuable theoretical insights and practical synthesis strategies for designing high-performance non-precious-metal SACs for CO₂RR.
- Electrocatalytic CO₂ reduction,
- Single atom catalyst,
- C₃N₄,
- Electron transfer,
- Fe-N₄ sites
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Atomically dispersed Fe–N4 sites on g–C3N4 enable highly selective CO2–to–CO electrocatalysis

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Atomically dispersed Fe–N₄ sites on g–C₃N₄ enable highly selective CO₂–to–CO electrocatalysis