Constructing multiple active sites in iron oxide catalysts for improving carbonylation reactions

Shujuan Liu, Teng Li, Feng Shi, Haiying Ma, Bin Wang, Xingchao Dai and Xinjiang Cui ()
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Shujuan Liu: Chinese Academy of Sciences
Teng Li: Chinese Academy of Sciences
Feng Shi: Chinese Academy of Sciences
Haiying Ma: Chinese Academy of Sciences
Bin Wang: Chinese Academy of Sciences
Xingchao Dai: Chinese Academy of Sciences
Xinjiang Cui: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract 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.

Date: 2023
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DOI: 10.1038/s41467-023-40640-z

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