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Constructing multiple active sites in iron oxide catalysts for improving carbonylation reactions.
Liu, Shujuan; Li, Teng; Shi, Feng; Ma, Haiying; Wang, Bin; Dai, Xingchao; Cui, Xinjiang.
Afiliação
  • Liu S; State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou, 730000, China.
  • Li T; State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou, 730000, China.
  • Shi F; State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou, 730000, China.
  • Ma H; State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou, 730000, China.
  • Wang B; University of Chinese Academy of Sciences, No. 19A, Yuquan Road, Beijing, 100049, China.
  • Dai X; State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou, 730000, China.
  • Cui X; State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou, 730000, China.
Nat Commun ; 14(1): 4973, 2023 Aug 17.
Article em En | MEDLINE | ID: mdl-37591841
Surface engineering is a promising strategy to improve the catalytic activities of heterogeneous catalysts. Nevertheless, few studies have been devoted to investigate the catalytic behavior differences of the multiple metal active sites triggered by the surface imperfections on catalysis. Herein, oxygen vacancies induced Fe2O3 catalyst are demonstrated with different Fe sites around one oxygen vacancy and exhibited significant catalytic performance for the carbonylation of various aryl halides and amines/alcohols with CO. The developed catalytic system displays excellent activity, selectivity, and reusability for the synthesis of carbonylated chemicals, including drugs and chiral molecules, via aminocarbonylation and alkoxycarbonylation. Combined characterizations disclose the formation of oxygen vacancies. Control experiments and density functional theory calculations demonstrate the selective combination of the three Fe sites is vital to improve the catalytic performance by catalyzing the elemental steps of PhI activation, CO insertion and C-N/C-O coupling respectively, endowing combinatorial sites catalyst for multistep reactions.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2023 Tipo de documento: Article País de afiliação: China

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2023 Tipo de documento: Article País de afiliação: China