Ammoximation Of Cyclohexanone To Cyclohexanone Oxime Over Titanium Silicon Molecular Sieve (TS-1) And Its Modified Catalysts

Cyclohexanone omixe is one of the most important intermediate in the production of Caprolactam. Conventionally it is synthesized in the cyclohexanone-hydroxylamine way. In the middle of 1980's Montedipe S.P.A of Italy successfully developed a new technology in which the ammoxidation of cyclohexanone was catalyzed by titanium silicalite-1. It is a new way to produce Caprolactam that was paid attention by investigators for its moderate reaction conditions,the use of cheaper and safe diluted hydrogen peroxide solution for oxidants,high conversion rate and seletivity,non-poluting process and no vice-thiamin merits. But the expensive production cost and harsh conditions limit its large-scale industrial applications. For the catalytic reaction system over TS-1,the development of lower cost of synthetic technology of TS-1 and better performance of catalytic-oxidation of TS-1 are the direction of future efforts. At the same time, the grain of the TS-1 that made from organic titanium-silicon materials is too small to separate from the reaction system. And TS-1 can be dissolved and eroded in the reaction system that using t-Butanol for solvent. These problems are also in the need of further research.On the basis of former studies,TS-1 original powder was produced by inorganic titanium-silicon materials and homemade templates.TS-1 contained silver was also produced by deposition-precipitation method(DP method) and hydrothermal synthesis method. And the influence factors during synthetic procedure of the two methods are investigated. TS-1 was dealed with acid in accordance with documentation. The TS-1 that both dealed with and non were applied to the reaction of ammoximation of cyclohexanone. The laws of ammonia oxidation process catalyted by TS-1,TS-1 that was treated and TS-1 that was loaded with silver were studied. And the reaction conditions were optimized and improved. Experimental results indicate that: 1)Both treating the TS-1 with acid and resetting TS-1 by adding stencil-plate can enhance the catalytic performance of TS-1.Moreover,the effect of combining this two methods is much more better. The cyclohexanone conversion rate is 20 percent higher than that not treated .2)the use of silver of hydrothermal synthesis method is more efficient than the DP method. The TS-1 loaded with silver does not show high catalytic reactive. The effect of the samples contain 2.0% silver is better than that contain 1.5% and 2.5% silver. The effect of the samples that loaded silver at 45℃are better than the other two temperature. 3)Under the experiment conditions that using water for solvent,reacting at 75...