Oxygen‐Substituted Porous C<sub>2</sub>N Frameworks as Efficient Electrocatalysts for Carbon Dioxide Electroreduction
The electrochemical carbon dioxide reduction reaction (CO<sub>2</sub>RR) provides a green avenue for decarbonizing the conventional chemical industries. Here, a structure-selectivity relationship of catalysts is pivotal for the control of a highly selective and active CO<sub>2</sub>RR pathway. We report the fabrication of an oxygen-substituted C<sub>2</sub>N as metal-free catalyst (O─C<sub>2</sub>N) for electrochemical CO<sub>2</sub>─to─CO conversion with tunable O microenvironment. Combined spectroscopic analysis reveals a fine tailored N─C─O moiety in O─C<sub>2</sub>N, where C─O─C species (e.g., ring in-plane ether) become the dominant oxygen configurations at higher pyrolysis temperatures. Based on experimental observations, a correlation between the exocyclic O-substituted N─C─O─C moieties and CO selectivity is established, giving clear chemical tools for active structure design. The optimized O─C<sub>2</sub>N electrocatalysts with the dominant appearance of C─O─C moieties exhibit an outstanding 2e<sup>-</sup> CO<sub>2</sub>RR performance with a CO selectivity up to 94.8%, which can be well maintained in a practical flow-cell reactor with an adjustable syngas feature.
Authors
- Nana Gao
- Tianxi X. Liu (ORCID: https://orcid.org/0000-0002-5592-7386)
- Qingran Zhang (ORCID: https://orcid.org/0000-0002-9939-8383)
- Yinguang Chen (ORCID: https://orcid.org/0000-0002-6463-5895)
- Josh Leverett (ORCID: https://orcid.org/0000-0001-7718-1792)
- Xunyu Lu (ORCID: https://orcid.org/0000-0003-4802-5269)
- Rahman Daiyan (ORCID: https://orcid.org/0000-0002-3543-3944)
- Yingtang Zhou (ORCID: https://orcid.org/0000-0002-8678-295X)
- Yufei Zhao (ORCID: https://orcid.org/0000-0002-5325-8991)
- Zhihong Tian (ORCID: https://orcid.org/0000-0002-6377-376X)
- Rose Amal (ORCID: https://orcid.org/0000-0001-9561-4918)
- Zhipeng Ma (ORCID: https://orcid.org/0000-0002-0719-7710)
- Markus Antonietti (ORCID: https://orcid.org/0000-0002-8395-7558)
- Shuai Wang (ORCID: https://orcid.org/0000-0002-8139-6515)
- Qiang Liu (ORCID: https://orcid.org/0000-0002-1625-6436)
- Xiaofeng Zhu (ORCID: https://orcid.org/0000-0002-1928-7107)
- Yihao Shan
Institutions
- Jiangnan University (CN)
- Shanghai University (CN)
- University of Technology Sydney (AU)
- Tongji University (CN)
- Southwest University of Science and Technology (CN)
- Henan University (CN)
- UNSW Sydney (AU)
- State Key Laboratory of Pollution Control and Resource Reuse (CN)
- Max Planck Institute of Colloids and Interfaces (DE)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-03-29
- DOI
- https://doi.org/10.1002/anie.202501896
- Citations
- 10
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 3.63