摘 要: 利用水热合成法在 α-Al 2 O 3 陶瓷管表面制备了连续完整的钛硅(TS-1)沸石膜, 并且利用该膜催化剂催化丙烯 直接环氧化合成环氧丙烷(PO)。采用 SEM、XRD、FT-IR 和 UV-Vis 等表征手段及丙烯环氧化反应测试, 详细研究 了合成液中 Ti/Si 比对 TS-1 沸石膜形貌、 结构及催化性能的影响。 结果表明, 合成液中 Ti/Si 比在 0.01~0.04 范围内, 所合成的 TS-1 沸石膜均具备典型 MFI 型拓扑结构。但当 Ti/Si 比>0.02 时, 随着 Ti/Si 比升高, TS-1 沸石膜表面沸 石颗粒排列变得杂乱, 且 TS-1 沸石沉积量逐渐减少, 沸石晶间缺陷增多, 丙烯渗透速率增大。而且, 当 Ti/Si 比= 0.03、0.04 时, 由于所合成的 TS-1 沸石膜中存在大量非骨架钛, 导致在丙烯环氧化反应中 PO 选择性和 PO 生成速 率明显降低。当 Ti/Si 比为 0.02 时, 合成的 TS-1 沸石膜骨架钛含量最高, 其催化性能最佳, H 2 O 2 转化率、PO 选择 性和生成速率分别为 12.43%、95.80%和 15.78 mmol/(h·g)。TS-1 沸石膜在丙烯环氧化反应中重复使用 8 次, 其催化 性能保持相对稳定。 关 键 词: 钛硅沸石; 沸石膜; 水热合成; 环氧丙烷 中图分类号: TQ174 文献标识码: AAbstract: Titanium silicalite-1(TS-1) zeolite membranes were successfully prepared on porous α-Al 2 O 3 tubes using hydrothermal synthesis method for epoxidation of propylene to propylene oxide (PO). SEM, XRD, FT-IR, and UV-vis spectroscopy were used to investigate the effects of Ti/Si molar ratio on surface morphology and structure of the TS-1 zeolite membrane. When the Ti/Si molar ratio was set between 0.01 and 0.04, continuous and compact TS-1 zeolite membranes were deposited on the porous support. The obtained TS-1 membranes displayed typical characteristics diffraction peaks of MFI structure. With the increase of the Ti/Si molar ratio, the deposition amounts of the TS-1 zeolites decreased. As a result, some intercrystalline defects were formed and the propylene permeance increased. For the TS-1 membranes prepared with the Ti/Si molar ratio of 0.03~0.04, poor PO selectivity and low PO formation rate were observed in the epoxidation reaction of propylene. This was at-tributed to the formation of extra-framework TiO 2 in the TS-1 membranes that could catalyze the decomposition