Selective CO2 Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts |
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| Authors: | Dr Shenghua Chen Dr Chengliang Ye Dr Ziwei Wang Dr Peng Li Dr Wenjun Jiang Dr Zechao Zhuang Dr Jiexin Zhu Dr Xiaobo Zheng Dr Shahid Zaman Dr Honghui Ou Lei Lv Dr Lin Tan Dr Yaqiong Su Dr Jiang Ouyang Prof Dingsheng Wang |
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| Institution: | 1. National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, 710049 P. R. China;2. Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084 P. R. China;3. School of Chemistry, Xi'an Key Laboratory of Sustainable Energy Materials Chemistry, State Key Laboratory of Electrical Insulation and Power Equipment, Engineering Research Center of Energy Storage Materials and Devices, Ministry of Education, Xi'an Jiaotong University, Xi'an, 710049 P. R. China;4. Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing, 100094 P. R. China;5. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430070 P. R China;6. Key Laboratory of Energy Conversion and Storage Technologies, Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055 P. R. China;7. School of Biomedical Engineering, Guangzhou Medical University, Guangzhou, 511436 P. R. China |
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| Abstract: | Electrochemical CO2 reduction reaction (CO2RR) over Cu catalysts exhibits enormous potential for efficiently converting CO2 to ethylene (C2H4). However, achieving high C2H4 selectivity remains a considerable challenge due to the propensity of Cu catalysts to undergo structural reconstruction during CO2RR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating the reconstruction of a Cu-based material to a pathway that facilitates CO2 reduction to C2H4 products. An excellent Faraday efficiency (FE) of 63.6 % on C2H4 with a current density of 497.2 mA cm−2 in flow cell was achieved, about 6.5 times higher than the pristine Cu catalyst which mainly produce CH4. The in situ X-ray absorption spectroscopy and Raman studies reveal that the hydroxyl group in TA stabilizes Cuδ+ during the CO2RR. Furthermore, theoretical calculations demonstrate that the Cuδ+/Cu0 interfaces lower the activation energy barrier for *CO dimerization, and hydroxyl species stabilize the *COH intermediate via hydrogen bonding, thereby promoting C2H4 production. Such molecule engineering modulated electronic structure provides a promising strategy to achieve highly selective CO2 reduction to value-added chemicals. |
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| Keywords: | C2H4 CO2RR Cuδ+/Cu0 Hydrogen Bonding TA Molecule |
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