摘要
As a renewable biomass-based compound with wide applications in food additives,fine chemical synthesis and fuels,γ-valerolactone(GVL)has attached much attention.While,pyrrolidones are widely used in pharmaceutical,agrochemical,material industrial and other chemical production.In this research,we demonstrated transformations of biomass-based ethyl levulinate(EL)into GVL and pyrrolidones by using heterogeneous catalysts(CNT-Ru-1)with N-heterocyclic carbene ruthenium(NHC-Ru)complex grafted on multi-walled carbon nanotube(CNT).The Ru catalyst showed high efficiency on EL hydrogenation to GVL with both EL conversion and GVL yield exceeding 99%.Moreover,the Ru catalyst readily promoted reductive amination of EL in the presence of various amines for pyrrolidone synthesis.Finally,the Ru catalyst was also applicable to hydrogenation of various carbonyl compounds for the synthesis of the corresponding alcohols with excellent catalytic performance.The research provides insight for heterogenizing the homogeneous noble metal-based catalysts with high catalytic active for biomass-based transformations.
As a renewable biomass-based compound with wide applications in food additives, fine chemical synthesis and fuels, γ-valerolactone(GVL) has attached much attention. While, pyrrolidones are widely used in pharmaceutical, agrochemical, material industrial and other chemical production. In this research, we demonstrated transformations of biomass-based ethyl levulinate(EL) into GVL and pyrrolidones by using heterogeneous catalysts(CNT-Ru-1) with N-heterocyclic carbene ruthenium(NHC-Ru) complex grafted on multi-walled carbon nanotube(CNT). The Ru catalyst showed high efficiency on EL hydrogenation to GVL with both EL conversion and GVL yield exceeding 99%. Moreover, the Ru catalyst readily promoted reductive amination of EL in the presence of various amines for pyrrolidone synthesis. Finally, the Ru catalyst was also applicable to hydrogenation of various carbonyl compounds for the synthesis of the corresponding alcohols with excellent catalytic performance. The research provides insight for heterogenizing the homogeneous noble metal-based catalysts with high catalytic active for biomass-based transformations.
基金
the financial support from the National Natural Science Foundation of China(U1810111,51872124 and21676116)
Natural Science Foundation of Guangdong Province,China(2018B030311010)
the Fundamental Research Funds for the Central Universities(21617431)
Key Laboratory of Biomass Chemical Engineering of Ministry of Education,Zhejiang University(2018BCE002)
