首页|Integrating Homogeneous and Heterogeneous Catalysis in a Copper Nanocluster with Lewis Acid-Base Sites for Chemical Conversion of CO2 and Propargylamine
Integrating Homogeneous and Heterogeneous Catalysis in a Copper Nanocluster with Lewis Acid-Base Sites for Chemical Conversion of CO2 and Propargylamine
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It remains a significant challenge to develop a cata-lyst that merges the advantages of homogeneous and heterogeneous catalysis with high reactivity and great recyclability.Herein,an atomically precise Cu6-NH2 nanocluster with distorted octahedral Cu6 core and NH2-functionalized ligands has been devel-oped as the first homo/heterogeneous catalyst to catalyze the cyclization reaction of propargylic amines with carbon dioxide(CO2)under mild condi-tions.As a homogeneous catalyst,Cu6-NH2 shows excellent catalytic activity with high turnover fre-quency due to highly accessible active sites.The definite coordination geometry and homogeneity nature of active centers make it convenient to inves-tigate the structure-activity relationship at the atom-ic level through experiments and theory calculations.In addition,the nanocluster exhibits excellent stabili-ty,great recrystallizability,and reusability in five catalytic cycles,in which its catalytic performance has no obvious decrease.Moreover,Cu6-NH2 incor-porates Lewis acid and base sites in metal and ligand,respectively,which can promote catalytic efficiency in a synergistic effect in the absence of any cocatalysts.Importantly,Cu6-NH2 can realize direct conversion of CO2 in simulated flue gas into oxazo-lidinones with high efficiency.The metal-ligand co-operative effect and integrated advantages of homogeneous and heterogeneous catalysis would provide new perspectives to achieve advanced metal nanocluster catalysts for CO2 conversion.
Henan Key Laboratory of Crystalline Molecular Functional Materials,Henan International Joint Laboratory of Tumor Theranostical Cluster Materials,Green Catalysis and College of Chemistry,Zhengzhou University,Zhengzhou 450001
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