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Abstract
Copper-based materials are promising electrocatalysts for CO2 reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO2 reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO2 reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C2+ products. We achieve a 40-fold enhancement in the ratio of C2+ to the competing CH4 compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO2 reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier—a rate-limiting step in CO2 reduction to multi-carbon products.
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1 Department of Electrical and Computer Engineering, University of Toronto, Toronto, ON, Canada; Key Laboratory of Luminescence and Optical Information, Beijing Jiaotong University, Ministry of Education, Beijing, China
2 Department of Electrical and Computer Engineering, University of Toronto, Toronto, ON, Canada
3 Department of Electrical and Computer Engineering, University of Toronto, Toronto, ON, Canada; Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, ON, Canada
4 Material and Chemical Research Laboratories, Industrial Technology Research Institute, Hsinchu, Taiwan
5 Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, China
6 Department of Materials Science and Engineering, University of Toronto, Toronto, ON, Canada
7 Canadian Light Source (CLS), Saskatoon, SK, Canada
8 Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu, Taiwan
9 Key Laboratory of Luminescence and Optical Information, Beijing Jiaotong University, Ministry of Education, Beijing, China
10 Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, ON, Canada