Study on Catalysts and the Reaction Behaviour of Oxime for Industrial Preparation Methyl Ethyl Ketone Oxime Catalyzed by Titanosilicate/Hydroperoxide System
|School||East China Normal University|
|Course||Physical and chemical|
|Keywords||Titanium silicalite Ti-MWW Pickling Complexing agent Ammonium fluoride Butanone oxime hydrolysis Regeneration Rearrangement|
Butanone oxime, cyclohexanone oxime, etc. oximes is important bulk chemicals containing oxygen, having a scale of tens to hundreds of tons in the international market. Titanium silicalite / H2O2 system catalytic ketones ammoximation generate oxime is environmentally friendly green chemical process. The paper of butanone oxime industrial production process catalysts and oxime reaction behavior of the main line, and further improve the new generation of titanium silicon modified zeolite Ti-MWW catalytic activity analysis the titanium silicalite / H2O2 system production butanone oxime oxime reaction behavior, and to further explore the reasons and regeneration methods in the process of inactivation of titanium silicalite, results achieved very instructive and practical significance. The titanium silicalite to accelerate the industrialization process / H2O2 system catalytic ketones ammoximation provide the basic scientific and technical basis. The Articles Main results are as follows: 1, according to a transition metal Ti with certain complexing agent (EDTA, OX ...) can form a stable complex characteristics, complexing agents auxiliary nitric acid pickling off unless the modified method of the framework titanium, system from complexing agent dosage, temperature, the amount of nitrate, nitric acid and a complexing agent to join the order. The study shows that, EDTA can be used as a suitable complexing agent, to obtain a high catalytic activity of the Ti-MWW zeolite catalyst. Fluoride complexes can be generated according to the system of fluoride ions and transition metal elements into the zeolite frameworks conducive, fluorine modified molecular sieve treatment system from silicon fluoride than processing time. The study showed that the use of ammonium fluoride after-treatment to obtain a highly active catalyst. 2, butanone oxime reaction behavior found in the oxime synthesis-butanone oxime industrial production process based on catalytic butanone ammonia Ti-MWW/H2O2 system directly affect the catalytic system operation stability, design from butanone oxime, affect the of butanone oxime reaction behavior of the factors, including titanium silicalite, H2O2, the titanium silicalite H2O2 together, the titanium silicalite proton acid common role. The study showed that the titanium silicalite with H2O2 joint action of the main factors affecting the stability of the butanone oxime, cyclohexanone oxime having similar properties. Ammoximation process of reaction efficiency and operation laid the foundation for stability. Deactivation of zeolite catalysts Ti-MWW/H2O2 system catalytic butanone ammonia oxime synthesis of butanone oxime industrial production process Deactivation preliminary exploration and study of regeneration method. Deactivation of zeolite catalysts using XRD, SEM, BET, UV-Vis, ICP, TG and other technical analysis. The study showed that the Ti-MWW zeolite catalyst inactivation may be due mainly to plugging the hole and the zeolite framework is destroyed is the organics in the zeolite channels. Try a variety of reproduction method, and was found that the acid treatment with skeletal rearrangement combined best reproduction method.