Oxygen‐Substituted Porous C<sub>2</sub>N Frameworks as Efficient Electrocatalysts for Carbon Dioxide Electroreduction
Abstract
AbstractThe electrochemical carbon dioxide reduction reaction (CO2RR) 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 CO2RR pathway. We report the fabrication of an oxygen‐substituted C2N as metal‐free catalyst (O─C2N) for electrochemical CO2─to─CO conversion with tunable O microenvironment. Combined spectroscopic analysis reveals a fine tailored N─C─O moiety in O─C2N, 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─C2N electrocatalysts with the dominant appearance of C─O─C moieties exhibit an outstanding 2e− CO2RR 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.
Article Details
Authors (17)
Shuai Wang
Shujie Zhou
School of Chemical Engineering
Zhipeng Ma
Nana Gao
Engineering Research Center For Nanomaterials Henan University Kaifeng P.R. China
Rahman Daiyan
Joshua Leverett
Particles and Catalysis Research Group School of Chemical Engineering University of New South Wales Sydney 2052 Australia
Yihao Shan
School of Chemical Engineering
Xiaofeng Zhu
Yufei Zhao
State Key Laboratory of Chemical Resource Engineering
Qiang Liu
Rose Amal
School of Chemical Engineering
Xunyu Lu
Tianxi Liu
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering
Markus Antonietti
Department of Colloid Chemistry
Yinguang Chen
State Key Laboratory of Pollution Control and Resources Reuse School of Environmental Science and Engineering Tongji University 1239 Siping Road Shanghai 200092 P.R. China
Qingran Zhang
State Key Laboratory of Pollution Control and Resources Reuse School of Environmental Science and Engineering Tongji University 1239 Siping Road Shanghai 200092 P.R. China
Zhihong Tian
Engineering Research Center for Nanomaterials Henan University Kaifeng P. R. China