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An Organic Molecular Mimetic Metal-Free Heterogeneous Catalyst for Electrocatalytic Alkyne Semihydrogenation.
Song, Ziyang; Yang, Rong; Liu, Xinyu; Zhang, Bin; Wu, Yongmeng.
Afiliación
  • Song Z; Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
  • Yang R; Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
  • Liu X; Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
  • Zhang B; Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
  • Wu Y; Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Frontiers Science Center for Synthetic Biology (Ministry of Education), Tianjin University, Tianjin, 300072, China.
Angew Chem Int Ed Engl ; 63(42): e202410200, 2024 Oct 14.
Article en En | MEDLINE | ID: mdl-39008407
ABSTRACT
The direct construction of metal-free catalysts on conductive substrates for electrocatalytic organic hydrogenation reactions is significant but still unexplored. Here, learning from the homogeneous molecular catalysts, an organic molecular mimetic metal-free heterogeneous catalyst is designed and constructed in situ on a graphite flake electrode via a mild electrochemical oxidation-reduction relay strategy. The as-prepared -COOH- and -OH-functionalized metal-free catalyst exhibits an electrocatalytic alkyne semihydrogenation performance with a 72 % Faradaic efficiency, 99 % selectivity and 96 % yield of the alkene product, which is comparable to that of noble metal catalysts. The removal of these oxygen-containing groups leads to negligible activity. The experimental and calculation results reveal that the origin of the high activity can be assigned to the -COOH and -OH groups on graphite. A flow electrolytic cell delivers ten grams of hydrogenated products with 81 % Faradaic efficiency. This metal-free catalyst is also suitable for gas-phase acetylene semihydrogenation and other electrocatalytic hydrogenation reactions.
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Texto completo: 1 Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China

Texto completo: 1 Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China