介孔TS-1分子筛微球合成及其催化环己酮氨肟化反应性能  

Synthesis of Mesoporous TS-1 Zeolite Microspheres and Catalytic Property in Cyclohexanone Ammoximation

作　　者：王振东[1] 徐乐[1] 何鸣元[1] 吴鹏[1] 

机构地区：[1]华东师范大学化学系上海市绿色化学与化工过程绿色化重点实验室,上海200062

出　　处：《化学反应工程与工艺》2013年第5期456-461,共6页Chemical Reaction Engineering and Technology

基　　金：国家自然科学基金项目(20925310;U1162102);教育部博士点基金优先发展领域(20120076130001)

摘　　要：采用三嵌段非离子型表面活性剂F127辅助水热晶化制得介孔TS-1分子筛微球,并详细考察了反应温度、氨酮比、双氧水与环己酮之比对TS-1分子筛微球催化液相连续淤浆床环己酮氨肟化反应性能的影响。结果表明:在反应温度75℃,氨与环己酮物质的量之比1.1,双氧水与环己酮物质的量之比1.7,质量空速6.3 h-1的反应条件下,TS-1分子筛微球显示出与常规纳米TS-1分子筛相当的环己酮转化率和环己酮肟的选择性,分别达98%和99%,但前者具有更高的稳定性。Mesoporous TS-1 zeolite microspheres were synthesized by hydrothermal crystallization with the assistance of triblock copolymer F127, and they were employed as the catalysts for the liquid-phase ammoximation of cyclohexanone with ammonia and hydrogen peroxide. The reaction parameters, molar ratio of 1-1202 to cyclohexanone and NH3 to cyclohexanone, which governed the cyclohexanone conversion, oxime selectivity and catalyst deactivation, were investigated by simulating the operating conditions in an industrial process. Under optimized reaction conditions of temperature 75 ℃, molar ratio of H202 to cyclohexanone 1.1, molar ratio of NH3 to cyclohexanone 1.7, WHSV6.3 h^-1, mesoporous TS-1 microspheres exhibited cyclohexanone conversion above 98% and oxime selectivity above 99%. Moreover, the TS-1 microsphere catalyst showed a longer lifetime than conventional nanosized TS-1 particles.

关 键 词：钛硅分子筛 环己酮肟 氨肟化 三嵌段表面活性剂 介孔 

分 类 号：TQ426[化学工程]