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作 者:Meng Jin Lina Ma Lina Zhou Kaiyue Ji Xiaomeng Xue Bi-Jie Li Haohong Duan
机构地区:[1]Department of Chemistry,Tsinghua University,Beijing 100084,China [2]State Key Laboratory of Chemical Resource Engineering,College of Chemistry,Beijing University of Chemical Technology,Beijing 100029,China [3]State Key Laboratory of Catalytic Materials and Reaction Engineering,Research Institute of Petroleum Processing,SINOPEC,Beijing 100083,China
出 处:《Science China Chemistry》2022年第11期2307-2317,共11页中国科学(化学英文版)
基 金:the National Natural Science Foundation of China(21978147,21935001,22090030,22105015);State Key Laboratory of Catalytic Materials and Reaction Engineering(RIPP,SINOPEC)。
摘 要:Coupling of cathodic H_(2) production with electrosynthesis of organic compounds not only solves the problem of sluggish oxygen evolution reaction(OER) kinetics, but also produces valuable chemicals. However, this strategy has rarely been explored for direct and selective C(sp~3)-H activation to construct C-C bonds, which could significantly enhance the synthetic efficiency in organic synthesis. Here, we report a nickel-iron layered double hydroxide-supported gold catalyst(Au/NiFe-LDH) for efficient electrocatalytic C-C coupling reaction in direct C(sp~3)-H alkynylation of tertiary aliphatic amines with 1-iodoalkynes, which is coupled with H_(2) production. Specifically, triethylamine and 1-iodoalkynes undergo efficient alkynylation to afford propargylamine in high yield(79%) and recycling ability without addition of external oxidants, coupling with 78-fold higher H_(2) productivity compared with water splitting under the same potential. This work may shed light on OER-substituted reaction towards C-C bond formation reactions under mild conditions.
关 键 词:layered double hydroxide ELECTROSYNTHESIS OER-substituted reaction H_(2)production C-C coupling
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