Synthesis and New Characterization Method of Silicalite-1 Membranes for Gas Separation

Abstract

Zeolite membranes have great potential in gas separation applications because of their unique selective properties. The main challenge is in synthesizing defect-free zeolite membranes. In this study, we synthesized silicalite-1 zeolite membranes on ceramic supports composed of Al2O3 and TiO2 using the pore-plugging method. We investigated the effect of the fill-level in the autoclave during the synthesis on the membrane performance. In particular, we were interested in determining the conditions at which the defects' contribution to the total transport is minimized. We adopted and further developed the approach proposed by Carter (2019) to quantify the permeance contribution through defects. Comparing the membrane performance before and after calcination, we proposed several modifications to the original analysis of Carter (2019). Knowing the defect transport contribution, we determined the corrected diffusivity, an intrinsic property of zeolite crystals at a given temperature, of several adsorbed gases on silicalite-1 crystals. The defect's contribution decreased as the autoclave fill-level increased from 94 to 98%. A further increase in the autoclave fill-level introduced more defects and caused the autoclave lid to rupture. Despite the differences in the membranes' performance arising from the autoclave fill-level, the corrected diffusivities of CO2, CH4, and N2 in silicalite-1 showed minimal variation from membrane to membrane. This proves the validity of the proposed characterization method. Moreover, the reported corrected diffusivities are comparable to the literature's values, found using other characterization methods. However, none of the previously used methods is as simple and straightforward as the one we further developed in this study.