Study On Epoxidation Of Cyclohexene Oxidized By Molecular Oxygen

This dissertation was financially supported by Henan Province Elitist Innovation Fund.In this work, cyclohexene from Shen Ma Group was used as crude material,and molecular oxygen was used as green oxidant. And the synthetic process of 1,2-epoxycyclohexane was studied, which included two main process- one was the preparation of ralative catalysts, the other was optimization of synthetic process.The salen ligands with the ortho- and para-position of hydroxyl having different group and the salophen ligands with different steric and electronic effect were synthesized. Then, the transitional metal complexes were synthesized, and the complexes were used as catalystes in the epoxidation of cyclohexene, and the MnL¹ complex was proved with better activity and selectivity. Thirdly, The selected MnL¹ complex with better activity and selectivity was attached to different molecular sieves by three encapsulation methods. The effection of contents of Mn ion and the repeated use of the catalyst were also investigated .The result showed, the MnL¹ complex attached to ZSM-5 zeolite by ion exchange method exhibited the high activity, and the proper contents of Mn ion were 2.335%. In addition, the catalytic activity was reduceded by 2% after being recycled 3 times.The synthesis conditions were studied when MnL¹ complex attached to ZSM-5 zeolite by ion exchange method was used as catalyst, and effects of many factors were investigated. Then orthognol technique was used to optimize the reaction conditions. And the optimal synthesis conditions were detailed as: temperature 30°C, reaction time 9h, W_{催化剂} :W_{环己 烯}=0.03:1,n_{溶剂乙腈}::n_{环己烯}=11:1, n(C₄H₈O):n(C₆H₁₀)=3.0:1.In such condition, the yield of 1,2-epoxycyclohexane could reach 87.16%.