Factors affecting MFI membrane quality

Zeolites are crystalline aluminosilicates with molecular sieving properties and are widely used in industrial applications such as catalysis, sorption and ion-exchange. Zeolite membranes are highly interesting due to their capability to continuously separate molecules under severe conditions. The MFI zeolite structure has suitable pore diameter for many applications, and its thermal and chemical stability is high. In order to obtain high performance MFI membranes, a thin and defect free film is needed for high flux and high selectivity. In this thesis, parameters affecting quality of zeolite membranes have been investigated. Different MFI-zeolite membranes were prepared using seed crystals and hydrothermal synthesis. Thereafter, membranes were characterized using scanning electron microscopy, single gas permeation measurements, porosimetry and separation experiments. The effect of grain boundaries was investigated by preparing membranes with small crystal size. It was found that a high amount of grain boundaries reduced the quality of the membranes. In another study, the effect of exposure to aqueous solutions was found to increase the amount of non-zeolitic pores in the membrane, and thus it decreased the quality of the membrane. However, no such effect was found for ethanol that was identified as a safe rinsing media. Membranes with different Si/Al ratio were also prepared and evaluated. It was observed that the Si/Al ratio of a MFI membrane influences the performance of the membrane. It was found that an increase of aluminium makes the membrane more polar which leads to an improved adsorption of, and selectivity for polar molecules. The effect of support invasion was also evaluated and the regularity and extension of the support invasion was observed to affect membrane quality. The effect of heating rate during calcination was investigated and no correlation between heating rate and membrane quality was observed. Calcination of membranes was studied in-situ by high temperature synchrotron radiation and a model for crack formation was postulated. In summary, this work has shown that in order to obtain high quality membranes, the amount of grain boundaries, the film thickness and support invasion should be controlled. To obtain the best performance of the membranes the Si/Al ratio should be chosen with respect to the application. Finally, water exposure affects the lifetime of the MFI membranes in certain applications.Godkänd; 2007; 20071012 (ysko