环己酮氨肟化及贝克曼重排反应研究-化学工艺专业论文.docxVIP

环己酮氨肟化及贝克曼重排反应研究 STUDY ON THE REACTION OF CYCLOHEXANONE AMMOXIDATION AND BECKMANN REARRANGEMENT ABSTRACT The one-step synthesis of ε-caprolactam (CPL) from cyclohexanone ammoxidation is one of the novel routes in green chemistry. The pillared montmorillonite is a novel synthetic catalytic material, which have application prospect in the catalytic field. In this thesis, titanium pillared montmorillonite, silicon titanium pillared montmorillonite and earth metal doped silicon- titanium pillared montmorillonite were synthesized and their physicochemical properties were characterized thoroughly, the catalytic performance for cyclohexanone ammoximation was investigated. ε-caprolactam was synthesized by microwave assisted to improve the catalytic performance of P2O5 catalyst towards cyclohexanone oxime liquid phase Beckmann rearrang- ement. Then, the one-pot synthesis of ε-caprolactam from cyclohexanone ammoxidation was studied. Titanium pillared-reagent, silicon-titanium pillared-reagent and rare metal doped silicon– titanium pillared-reagent were prepared by sol-gel method, and pillared montmorillonite catalysts were prepared by ion exchange method. The prepared pillared montmorillonite were determined by XRD, FT-IR, TG-DSC, SEM-EDX and BET. The catalytic performance of the catalysts for cyclohexanone ammoximation was investigated. The results show that when Ti : MMT ratio is 6 : 1(mmol/g), OH-: H+ for pillared-reagent molar ratio is 3:1, Si : Ti molar ratio is 1:2, hydrothermal cross-linking method, calcinations temperature is 450℃, the spacing of layers of silicon-titanium pillared montmorillonite increase from 0.98 nm of the sodium montmori- llomite to 1.02 nm, the specific surface area of silicon-titanium pillared montmorillonite increase from 35.9 m2 /g of the sodium montmorillomite to 138.3 m2 /g. The silicon-titanium pillared montmorillonite show good thermal stability, when the temperature arrives at about 900℃, the weight loss is only 2.27 %. Eu3+ doped