Wang Qihao, Yang Chao, Yan Yaqin, Yu Haisheng, Guan Anxiang, Kan Miao, Zhang Quan, Zhang Linjuan, Zheng Gengfeng
Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 200438, Shanghai, China.
Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, 201800, Shanghai, China.
Angew Chem Int Ed Engl. 2023 Jan 26;62(5):e202212733. doi: 10.1002/anie.202212733. Epub 2022 Dec 7.
The electrocatalytic carbon dioxide (CO ) reduction is a promising approach for converting this greenhouse gas into value-added chemicals, while the capability of producing products with longer carbon chains (C >3) is limited. Herein, we demonstrate the Br-assisted electrocatalytic oxidation of ethylene (C H ), a major CO electroreduction product, into 2-bromoethanol by electro-generated bromine on metal phthalocyanine catalysts. Due to the preferential formation of Br over *O or Cl to activate the C=C bond, a high partial current density of producing 2-bromoethanol (46.6 mA⋅cm ) was obtained with 87.2 % Faradaic efficiency. Further coupling with the electrocatalytic nitrite reduction to ammonia at the cathode allowed the production of triethanolamine with six carbon atoms. Moreover, by coupling a CO electrolysis cell for in situ C H generation and a C H oxidation/nitrite reduction cell, the capability of upgrading of CO and nitrite into triethanolamine was demonstrated.
电催化二氧化碳（CO₂）还原是一种将这种温室气体转化为高附加值化学品的有前景的方法，然而生产碳链更长（C>3）产品的能力有限。在此，我们展示了在金属酞菁催化剂上通过电生成的溴将乙烯（C₂H₄）（一种主要的CO₂电还原产物）进行Br辅助电催化氧化为2-溴乙醇。由于Br比*O或Cl更优先形成以活化C=C键，在87.2%的法拉第效率下获得了生产2-溴乙醇的高局部电流密度（46.6 mA·cm⁻²）。进一步在阴极将电催化亚硝酸盐还原为氨，使得能够生产含六个碳原子的三乙醇胺。此外，通过耦合一个用于原位生成C₂H₄的CO₂电解池和一个C₂H₄氧化/亚硝酸盐还原池，展示了将CO₂和亚硝酸盐升级为三乙醇胺的能力。
