Effects of exposure to water and ethanol on silicalite-1 membranes

The effects of long exposures to ethanol, water and 0.1 M aqueous solutions of ammonia, sodium hydroxide, tetrapropyl ammonium hydroxide (TPAOH) and hydrochloric acid on thin TPA-silicalite-1 membranes were studied. Single gas permeation experiments, porosimetry and scanning electron microscopy were used to characterize the membranes. It was found that a short exposure (24 h) will only dissolve synthesis residues and will not affect membrane quality negatively. The only medium that had an effect after 24 h was sodium hydroxide, which almost dissolved the film completely. After exposing TPA-silicalite-1 membranes for 30 days in the various liquids, the membrane quality decreased in the order ethanol <0.1 Mhydrochloric acid< 0.1 M TPAOH < water<0.1 M ammonia<0.1 M sodium hydroxide due to dissolution of the silicalite-1 crystals. This study has shown that prolonged exposure to aqueous solutions will lead to dissolution of silicalite-1 crystals causing an increase in micro and mesopores in the film. The amount and size of the pores will depend on the pH of the aqueous medium. Higher pH gives a higher dissolution and hence more non-zeolitic pores in the silicalite-1 film. Ethanol has no effect on the dissolution of the zeolite film even after 30 days. This finding has an effect in membrane preparation and in several membrane applications such as pervaporation and separation of hydrocarbons isomer mixtures. (C) 2008 Elsevier B.V. All rights reserved.