A bifunctional heterogeneous catalyst was designed and synthesized,denoted DMEDA/IL–NH2-MIL-101.The structure and physical-chemical characterization of DMEDA/IL–NH2-MIL-101 and its precursors were characterized by S...A bifunctional heterogeneous catalyst was designed and synthesized,denoted DMEDA/IL–NH2-MIL-101.The structure and physical-chemical characterization of DMEDA/IL–NH2-MIL-101 and its precursors were characterized by SEM,N2 adsorption-desorption,XPS,FT-IR,PXRD,elemental analysis,and TGA techniques.The date showed that the two catalytic components of N,N-dimethylethylenediamine(DMEDA)and 1-butyl-3-methylimidazolium bromide(BmimBr)were chemically immobilized in NH2-MIL-101 nanocages.The amine of DMEDA was grafted onto carrier NH2-MIL-101 by N–Cr coordinate covalent bonds and the ionic liquid of BmimBr(IL(Br-))was anchored in the NH2-MIL-101 nanocages by'ship-in-a-bottle'method,in which the amidogen of NH2-MIL-101 condensed with N,N-carbonyldiimidazole(CDI)firstly,and then alkylated with 1-bromo butane.This novel heterogeneous catalyst with two different active sites can efficiently catalyze the synthesis of N-aryl oxazolidin-2-ones from carbon dioxide(CO2),epoxides,and anilines in one-pot under mild solvent-free conditions.It not only showed good stability and recoverability after five cycles but also exhibited shape selectivity for the substrate due to the synergic catalysis of amine,ionic liquid,and NH2-MIL-101.This novel bifunctional material is a promising solid catalyst for the green synthesis of N-aryl oxazolidin-2-ones.展开更多
基金Support of this work by the National Natural Science Foundation of China(21573016)is gratefully acknowledged.
文摘A bifunctional heterogeneous catalyst was designed and synthesized,denoted DMEDA/IL–NH2-MIL-101.The structure and physical-chemical characterization of DMEDA/IL–NH2-MIL-101 and its precursors were characterized by SEM,N2 adsorption-desorption,XPS,FT-IR,PXRD,elemental analysis,and TGA techniques.The date showed that the two catalytic components of N,N-dimethylethylenediamine(DMEDA)and 1-butyl-3-methylimidazolium bromide(BmimBr)were chemically immobilized in NH2-MIL-101 nanocages.The amine of DMEDA was grafted onto carrier NH2-MIL-101 by N–Cr coordinate covalent bonds and the ionic liquid of BmimBr(IL(Br-))was anchored in the NH2-MIL-101 nanocages by'ship-in-a-bottle'method,in which the amidogen of NH2-MIL-101 condensed with N,N-carbonyldiimidazole(CDI)firstly,and then alkylated with 1-bromo butane.This novel heterogeneous catalyst with two different active sites can efficiently catalyze the synthesis of N-aryl oxazolidin-2-ones from carbon dioxide(CO2),epoxides,and anilines in one-pot under mild solvent-free conditions.It not only showed good stability and recoverability after five cycles but also exhibited shape selectivity for the substrate due to the synergic catalysis of amine,ionic liquid,and NH2-MIL-101.This novel bifunctional material is a promising solid catalyst for the green synthesis of N-aryl oxazolidin-2-ones.
