固定床反应器上TS-1催化丙烯环氧化  

PROPYLENE EPOXIDATION OVER MODIFIED TS-1 CATALYSTS IN FIXED-BED REACTOR

作　　者：刘民[1] 董毅[1] 郭新闻[1] 王祥生[1] 

机构地区：[1]大连理工大学化工学院催化化学与工程系,精细化工国家重点实验室,辽宁大连116012

出　　处：《石油学报（石油加工）》2010年第5期677-683,共7页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：新世纪优秀人才支持计划(NCET-04-0268);“111”计划项目资助

摘　　要：采用四丙基氢氧化铵(TPAOH)稀溶液对TS-1进行改性,考察了不同改性条件对成型后催化剂在丙烯环氧化反应中的催化性能的影响,同时考察了反应条件即反应温度、丙烯空速、双氧水浓度、氨水浓度,以及催化剂床层长/径比、催化剂粒度等对改性TS-1催化丙烯环氧化反应H2O2转化率和环氧丙烷选择性的影响。结果表明,经TPAOH改性的TS-1催化剂在丙烯环氧化反应中的催化性能优异,在反应温度45℃、反应压力3.0 MPa、丙烯空速0.6 h-1、总空速3.5 h-1的条件下,采用摩尔比为3的丙酮和甲醇为溶剂、H2O2浓度1.1 mol/L、氨水浓度0.4 mmol/L、催化剂颗粒度1 mm×1 mm和床层长/径比为11,丙烯环氧化反应的H2O2转化率和环氧丙烷选择性均可以达到且稳定在95%以上。1500 h运转结果表明,催化剂具有高的催化活性、环氧丙烷选择性和稳定性。TS-1 samples were modified with dilute tetrapropyl ammonium hydroxide（TPAOH） aqueous solution.The effects of modification conditions on the catalytic properties of extruded TS-1 samples in propylene epoxidation were investigated.The reaction conditions,such as reaction temperature,space velocity of propylene,concentration of H2O2,concentration of ammonia,length/diameter radio（L/D） of the catalyst bed,particle size of the extruded catalyst,were optimized.The results showed that the suitable reaction conditions were as follows： reaction temperature of 45℃,reaction pressure of 3.0 MPa,total space velocity of 3.5 h-1,propylene space velocity of 0.6 h-1,by using the mixture of acetone and methanol with a mole ratio of 3 as solvent,H2O2concentration of 1.1 mol/L,ammonia concentration of 0.4 mmol/L,particle size of the catalyst 1 mm×1 mm andL/Dof the catalyst bed of 11,under which the conversion of H2O2and the selectivity of propylene oxide reached above 95% and kept stable.A long term of 1500 h reaction showed that the extruded TS-1 catalyst modified with TPAOH exhibited high activity,selectivity of propylene oxide and stability in epoxidation of propylene.

关 键 词：TS-1 四丙基氢氧化铵(TPAOH) 丙烯环氧化 过氧化氢 环氧丙烷 

分 类 号：O643[理学—物理化学]