摘要

High quality pure-silica MFI-type zeolite membranes are successfully prepared by simply controlling the amount of structure directing agent (SDA), i. e., tetrapropylammonium (TPA(+)) in the synthesis solution for seeded growth. The effects of several synthesis parameters such as alkalinity (OH-/Si), TPA(+) concentration (TPA(+)/Si), and crystallization time on the membrane pervaporation performance are investigated in detail. The synthesized MFI-type zeolite membranes are thoroughly characterized by scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, the water contact angle test, X-ray diffraction (XRD), the pervaporation test and gas permeation. The membrane microstructure is very sensitive to the TPA(+)/Si ratio of the synthesis solution. At a high TPA(+)/Si ratio (typically 0.17), parasitic twin crystals are intergrown in the zeolite layer, thus resulting in the formation of membrane defects during SDA removal treatment (calcination at 500 degrees C). When the membrane is prepared with a low TPA(+)/Si ratio (<= 0.05), the appearance of twin crystals can be significantly suppressed and the synthesized dense MFI-type zeolite membranes exhibit pervaporation separation factors higher than 85 for 5 wt% ethanol-water mixtures at 60 degrees C. We demonstrate for the first time that controlling the SDA concentration in the precursor solution is beneficial to the elimination of membrane microstructural defects, showing a pathway to high quality MFI-type zeolite membranes.