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

Abstract

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 one-pot 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 self-sacrificing 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.