摘要
采用连续淤浆床反应装置,对比研究了环己烷为溶剂的液-液-固三相体系中成型Ti-MWW分子筛与TS-1分子筛催化环己酮氨肟化反应的性能。结果表明,成型Ti-MWW分子筛催化环己酮氨肟化的性能明显优于TS-1分子筛。催化剂寿命评价以及反应副产物的定性分析结果表明,在催速失活工艺条件下,成型Ti-MWW分子筛在环己烷为溶剂的液-液-固三相体系中稳定运行28.1h,环己酮肟选择性大于99%,反应副产物主要为高沸点极性有机物。通过对新鲜、失活及再生催化剂进行SEM、XRD、N_2物理吸附、UV-Vis和FT-IR等表征,表明成型Ti-MWW分子筛单程失活未见明显骨架硅流失,拓扑结构没有被破坏,失活主要是由反应副产物堵孔造成的。
A continuous slurry reactor was used to study the catalytic performance of shapedTi-MWWand TS1zeolites in the liquidliquidsolid threephase ammoximation,with cyclohexane as the solvent.The results show that the shaped Ti-MWW had better performance than TS1for ammoximation of cyclohexanone.Deactivation behavior of the catalyst was studied and qualitative analysis of the reaction byproducts was carried out.Under the accelerated deactivation condition,the life time of shaped Ti-MWW zeolite reached281hin liquidliquidsolid threephase ammoximation and the selectivity of cyclohexanone oxime was above99%.Byproducts of the reaction were mainly high boiling point polar organic compounds.The fresh,deactivated and regenerated catalysts were characterized by various approaches,including SEM,XRD,N2physisorption,UVVis and FT-IR.The results showed that the dissolution erosion of silicon from the zeolite was negligible and the MWW framework structure did not change obviously.The byproducts blocking of the molecular sieve channels is the primary factor leading to the deactivation of shaped TiMWW zeolite in a single cycle.
作者
王妙
宋仕芋
袁霞
吴剑
WANG Miao;SONG Shiyu;YUAN Xia;WU Jian(School of Chemical Enginering, Xiangtan University, Xiangtan 411105, China)
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
2017年第6期1183-1191,共9页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金项目(21376201)
湖南省高校2011协同创新中心资助项目资助
关键词
成型T-MWW分子筛
氨肟化
环己酮肟
液-液-固三相反应
失活
shaped TiMWW zeolite
ammoximation
cyclohexane oxime
liquidliquidsolid threephase reaction
deactivation
