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Directing the Selectivity of CO Electrolysis to Acetate by Constructing Metal-Organic Interfaces |
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| Authors: | Youwen Rong Dr. Tianfu Liu Jiaqi Sang Dr. Rongtan Li Dr. Pengfei Wei Dr. Hefei Li Dr. Aiyi Dong Prof. Dr. Li Che Prof. Dr. Qiang Fu Prof. Dr. Dunfeng Gao Prof. Dr. Guoxiong Wang |
| Affiliation: | 1. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China School of Science, Dalian Maritime University, 116026 Dalian, China These authors contributed equally to this work.;2. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China;3. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China University of Chinese Academy of Sciences, 100049 Beijing, China;4. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023 Dalian, China School of Science, Dalian Maritime University, 116026 Dalian, China;5. School of Science, Dalian Maritime University, 116026 Dalian, China |
| Abstract: | Electrochemically converting CO2 to valuable chemicals holds great promise for closing the anthropogenic carbon cycle. Owing to complex reaction pathways and shared rate-determining steps, directing the selectivity of CO2/CO electrolysis to a specific multicarbon product is very challenging. We report here a strategy for highly selective production of acetate from CO electrolysis by constructing metal-organic interfaces. We demonstrate that the Cu-organic interfaces constructed by in situ reconstruction of Cu complexes show very impressive acetate selectivity, with a high Faradaic efficiency of 84.2 % and a carbon selectivity of 92.1 % for acetate production, in an alkaline membrane electrode assembly electrolyzer. The maximum acetate partial current density and acetate yield reach as high as 605 mA cm−2 and 63.4 %, respectively. Thorough structural characterizations, control experiments, operando Raman spectroscopy measurements, and density functional theory calculation results indicate that the Cu-organic interface creates a favorable reaction microenvironment that enhances *CO adsorption, lowers the energy barrier for C−C coupling, and facilitates the formation of CH3COOH over other multicarbon products, thus rationalizing the selective acetate production. |
| Keywords: | Acetate CO Electrolysis Metal-Organic Interface Reaction Microenvironment Selectivity Control |