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(111) Facet-oriented Cu2Mg Intermetallic Compound with Cu3-Mg Sites for CO2 Electroreduction to Ethanol with Industrial Current Density |
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| Authors: | Dr Chen Peng Jiaxing Ma Dr Gan Luo Shuai Yan Junbo Zhang Yangshen Chen Dr Ning Chen Dr Zhiqiang Wang Prof Wei Wei Prof Tsun-Kong Sham Prof Yao Zheng Prof Min Kuang Prof Gengfeng Zheng |
| Institution: | 1. Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
School of Chemical Engineering, The University of Adelaide, Adelaide, SA, 5005 Australia These authors contributed equally: Chen Peng and Jiaxing Ma;2. Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China These authors contributed equally: Chen Peng and Jiaxing Ma;3. Henan Engineering Center of New Energy Battery Materials, Henan D&A Engineering Center of Advanced Battery Materials, College of Chemistry and Chemical Engineering, Shangqiu Normal University, Shangqiu, 476000 China;4. Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China;5. Canadian Light Source Inc., University of Saskatchewan, Saskatoon, SK, S7 N 2 V3 Canada;6. Department of Chemistry, University of Western Ontario, London, ON, N6 A 5B7 Canada;7. School of Chemical Engineering, The University of Adelaide, Adelaide, SA, 5005 Australia;8. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 China |
| Abstract: | The efficient ethanol electrosynthesis from CO2 is challenging with low selectivity at high CO2 electrolysis rates, due to the competition with H2 and other reduction products. Copper-based bimetallic electrocatalysts are potential candidates for the CO2-to-ethanol conversion, but the secondary metal has mainly been focused on active components (such as Ag, Sn) for CO2 electroreduction, which also promote selectivity of ethylene or other reduction products rather than ethanol. Limited attention has been given to alkali-earth metals due to their inherently active chemical property. Herein, we rationally synthesized a (111) facet-oriented nano Cu2Mg (designated as Cu2Mg(111)) intermetallic compound with high-density ordered Cu3-Mg sites. The in situ Raman spectroscopy and density function theory calculations revealed that the Cu3− −-Mg− + active sites allowed to increase *CO surface coverage, decrease reaction energy for *CO−CO coupling, and stabilize *CHCHOH intermediates, thus promoting the ethanol formation pathway. The Cu2Mg(111) catalyst exhibited a high FEC2H5OH of 76.2±4.8 % at 600 mA⋅cm−2, and a peak value of |jC2H5OH| of 720±34 mA⋅cm−2, almost 4 times of that using conventional Cu2Mg with (311) facets, comparable to the best reported values for the CO2-to-ethanol electroreduction. |
| Keywords: | CO2 electroreduction alkali-earth metal Cu2Mg intermetallic compound electron localization (111) facets |