Xing Chengyu, Xue Yurui, Zheng Xuchen, Gao Yang, Chen Siao, Li Yuliang
Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
Angew Chem Int Ed Engl. 2023 Oct 9;62(41):e202310722. doi: 10.1002/anie.202310722. Epub 2023 Sep 6.
Selective hydrogenation of olefins with water as the hydrogen source at ambient conditions is still a big challenge in the field of catalysis. Herein, the electrocatalytic hydrogenation of purely aliphatic and functionalized olefins was achieved by using graphdiyne based copper oxide quantum dots (Cu O/GDY) as cathodic electrodes and water as the hydrogen source, with high activity and selectivity in aqueous solution at high current density under ambient temperature and pressure. In particular, the sp-/sp -hybridized graphdiyne catalyst allows the selective hydrogenation of cis-trans isomeric olefins. The chemical and electronic structure of the GDY results in the incomplete charge transfer between GDY and Cu atoms to optimize the adsorption/desorption of the reaction intermediates and results in high reaction selectivity and activity for hydrogenation reactions.
在环境条件下以水作为氢源对烯烃进行选择性氢化仍然是催化领域的一大挑战。在此，通过使用基于石墨炔的氧化铜量子点（CuO/GDY）作为阴极电极以及水作为氢源，实现了纯脂肪族烯烃和官能化烯烃的电催化氢化，在室温和常压下的水溶液中，在高电流密度下具有高活性和选择性。特别地，sp-/sp -杂化的石墨炔催化剂能够实现顺反异构烯烃的选择性氢化。石墨炔的化学和电子结构导致石墨炔与铜原子之间的电荷转移不完全，从而优化了反应中间体的吸附/解吸，并导致氢化反应具有高反应选择性和活性。
