TS-1分子筛的合成及其催化丙烯环氧化反应工艺条件的优化  

Synthesis of TS-1 Zeolite and Its Optimal Catalytic Conditions for Propylene Epoxidation

作　　者：侯旭 刘猛 温贻强[1] 王向宇[1] HOU Xu;LIU Meng;WEN Yiqiang;WANG Xiangyu(College of Chemistry and Molecular Engineering,Zhengzhou University,Zhengzhou 450001,China)

机构地区：[1]郑州大学化学与分子工程学院

出　　处：《石油学报（石油加工）》2019年第6期1115-1122,共8页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：河南省杰出人才创新基金项目(0221001200);河南省重大科技专项基金项目(131100210900)资助

摘　　要：以纳米硅分子筛(S-1)悬浮液为晶种,在水热体系中合成TS-1分子筛。经过碱后处理和成型,得到成型的TS-1分子筛催化剂。通过XRD、ICP和XPS等表征手段研究了催化剂的性能。采用固定床反应器考察了该催化剂对低n(CH 3OH)/n(H 2O 2)比下丙烯环氧化反应的条件及运行稳定性的影响。结果表明:经过碱后处理的TS-1分子筛表面具有较好的疏水性,且成型前后催化剂的性能不变,进而成型的碱后处理TS-1分子筛,在n(CH 3OH)/n(H 2O 2)=4.9、反应温度为43℃、丙烯的质量空速为0.64 h^-1、反应液pH值为9.10、n(C 3H 6)/n(H 2O 2)=2.1的条件下,H 2O 2的转化率和有效利用率均达到98%,并且此反应过程连续稳定的运行超过了1700 h。TS-1 zeolite was synthesized with using nanosized S-1 suspension as the seed in a hydrothermal system.Then,the extruded TS-1 zeolite was obtained after alkali post-treatment and molding,and the prepared catalyst performance were further studied by different characterization techniques including XRD,ICP,XPS.In addition,with using a fixed-bed reactor,propylene epoxidation with using the prepared TS-1 catalyst under low molar ratio of methanol and hydrogen peroxide was investigated.Experimental results showed that the alkali-treated catalyst surface has good hydrophobicity,and catalyst performance did not change before and after molding.Under the reaction conditions of n(CH 3OH)/n(H 2O 2)=4.9,temperature 43℃,propylene MHSV 0.64 h^-1,pH value of reaction solution 9.10 and n(C 3H 6)/n(H 2O 2)=2.1,the conversion and utilization of H 2O 2 both could reach 98%.Especially,this catalyst demonstrated excellent stability during over 1700 hours test time.

关 键 词：TS-1分子筛 成型 丙烯环氧化 固定床反应器 醇/水摩尔比 

分 类 号：O643.32[理学—物理化学]