Gas Permeation of SiC Membrane Coated on Multilayer γ-Al2O3 with a Graded Structure for H2 Separation

Abstract

A promising candidate material for a <TEX>$H_2$</TEX> permeable membrane is SiC due to its many unique properties. A hydrogen-selective SiC membrane was successfully fabricated on the outer surface of an intermediate multilayer <TEX>$\gamma-Al_2O_3$</TEX> with a graded structure. The <TEX>$\gamma-Al_2O_3$</TEX> multilayer was formed on top of a macroporous <TEX>$\alpha-Al_2O_3$</TEX> support by consecutively dipping into a set of successive solutions containing boehmite sols of different particle sizes and then calcining. The boehmite sols were prepared from an aluminum isopropoxide precursor and heated to <TEX>$80^{\circ}C$</TEX> with high speed stirring for 24 hrs to hydrolyze the precursor. Then the solutions were refluxed at <TEX>$92^{\circ}C$</TEX> for 20 hrs to form a boehmite precipitate. The particle size of the boehmite sols was controlled according to various experimental parameters, such as acid types and acid concentrations. The topmost SiC layer was formed on top of the intermediate <TEX>$\gamma-Al_2O_3$</TEX> by pyrolysis of a SiC precursor, polycarbosilane, in an Ar atmosphere. The resulting amorphous SiC-on-<TEX>$Al_2O_3$</TEX> composite membrane pyrolyzed at <TEX>$900^{\circ}C$</TEX> possessed a high <TEX>$H_2$</TEX> permeability of <TEX>$3.61\times10^{-7}$</TEX> <TEX>$mol{\cdot}m^{-2}{\cdot}s^{-1}{\cdot}Pa^{-1}$</TEX> and the <TEX>$H_2/CO_2$</TEX> selectivity was much higher than the theoretical value of 4.69 in all permeation temperature ranges. Gas permeabilities through a SiC membrane are affected by Knudsen diffusion and a surface diffusion mechanism, which are based on the molecular weight of gas species and movement of adsorbed gas molecules on the surface of the pores.