4.7 Article

Bimetallic CuZn-MOFs derived Cu-ZnO/C catalyst for reductive amination of nitroarenes with aromatic aldehydes tandem reaction

期刊

APPLIED SURFACE SCIENCE
卷 569, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.apsusc.2021.151033

关键词

Metal organic frameworks (MOFs); Hydrogenation-amination tandem reaction; Self-sacrificing template; Amine; Imine

资金

  1. Reform and Development Fund Project of Local University - Central Government, National Natural Science Foundation of China [21801070]

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Tuning of metal-metal/oxide interaction is crucial for enhancing supported catalyst performance. In this study, a Cu/Zn bimetallic MOFs was synthesized and converted into a ZnO/nitrogen-doped carbon composite supported Cu catalyst (Cu-ZnO/NC-BMOFs) for hydrogenation-amination tandem reaction. The developed catalyst exhibited superior performance and stability compared to traditional Cu/ZnO/NC-IWI catalyst, converting nitroarenes into imines or secondary amines with high selectivity.
Tuning of the metal-metal/oxide interaction is a vital route to enhance the performance of the supported catalysts. In this study, a Cu/Zn bimetallic MOFs was synthesized through a simple solvothermal method by using an adenine rigid biomolecule acted as organic linker. Furthermore, a ZnO/nitrogen-doped carbon composite supported Cu catalyst (named as Cu-ZnO/NC-BMOFs) derived from the bimetallic CuZn-MOFs was obtained via onepot pyrolysis method. The developed Cu-ZnO/NC-BMOFs catalyst was tested for hydrogenation-amination tandem reaction. The bimetallic CuZn-MOFs with the uniformly dispersed Cu and Zn centers acted as a selfsacrificing template, which could facilitate the derived catalyst with strengthened Cu-ZnO interaction, high dispersity, and more N species. All of these advantages give the developed Cu-ZnO/NC-BMOFs catalyst with higher performance in hydrogenation-amination tandem reaction compared with traditional Cu/ZnO/NC-IWI (synthesized by incipient wetness impregnation) catalyst. The Cu-ZnO/NC-BMOFs exhibits good stability for the recycling experiments with a negligible loss in its performance. More importantly, the Cu-ZnO/NC-BMOFs catalyst could convert nitroarenes into the corresponding imines or secondary amines with excellent selectivity (>90.0%). This bimetallic MOFs-derived strategy may provide a way for fabricating NC supported catalysts in other tandem reactions.

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