Constructing Multiple Active Sites in Iron Oxide Catalysts for Improving Carbonylation Reactions.
Nature communications(2023)
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. Surface engineering of Fe sites was used to improve the carbonylation reaction of aryl halides and amines/alcohols with CO. The elementary steps of phenyl iodide activation, CO insertion and C-N/C-O coupling were catalyzed respectively, leading to improved catalytic activity.
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Key words
Catalyst synthesis,Heterogeneous catalysis,Science,Humanities and Social Sciences,multidisciplinary
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