The Baeyer-Villiger Oxidation Of Cyclohexanone Catalyzed By Nitrogen-Doped Carbon Nanotubes And Exploration Of The Feasibility Of Industrialization Production

The catalytic performance of carbon nanotubes（CNTs）are closely related to the structure and surface chemical properties.The heteroatoms doping into the CNTs,especially N doping,could effectively tune the surface property of CNTs,resulting in high specific surface area,high defect density,chemical activity sites etc.In this work,NCNTs was prepared by chemical vapor deposition（CVD）and applied as the catalyst for the Baeyer-Villiger oxidation reaction of cyclohexanone.The main research contents of this paper are listed as follows:（1）For the first time,NCNTs was used as catalyst for the Baeyer-Villiger reaction oxidation of cyclohexanone with benzaldehyde as the sacrificing agent,showing a good catalytic performance and stability.The prioritized condition is 1000 r/min,50 ^oC,2 h,0.8MPa O₂,1,2-dichloroethane as solvent.It was found that NCNTs showed the highest catalytic activity with over 90%ofε-caprolactone selectivity,94.8%conversion of cyclohexanone.NCNTs has showed a good stability after 5 cycles.It was found that the catalytic performance of NCNTs in the Baeyer-Villiger oxidation reaction of cyclohexanone increased with the increase of nitrogen content.Furthermore,oxygen-containing functional groups on the NCNTs surface displayed a negative effect on the Baeyer-Villiger oxidation reaction of cyclohexanone.This study provides a novel metal-free catalytic approach for the Baeyer-Villiger oxidation reaction of cyclohexanone with benzaldehyde as the co-oxidant.（2）Acrolein was used as the co-oxidant in the Baeyer-Villiger oxidation reaction of cyclohexanone to produceε-caprolactone and acrylic acid at the same time.Based on our previous experimental results,a tubular reactor for the produce ofε-caprolactone was designed by using the kinetic parameter extracted from previous data.It was revealed that,for the non-backmixing tubular reactor,the lengths calculated through the regression analysis method and linear fitting method are 6.4m and 11.8m,respectively.For the cycling tubular reactor,the lengths calculated through regression analysis and linear fitting method were 7.1m and 13.5 m,respectively.