Preparation of Al-Containing ZSM-58 Zeolite Membranes Using Rapid Thermal Processing for CO₂/CH₄ Mixture Separation

Abstract

The synthesis of DDR-type zeolite membranes faces the problem of cracks that occur on the zeolite membrane due to differences in the thermal expansion coefficient between zeolite and the porous substrate during the detemplating process. In this study, Al-containing ZSM-58 zeolite membranes with DDR topology were prepared by rapid thermal processing (RTP), with the aim of developing a reproducible method for preparing DDR zeolite membrane without cracks. Moreover, we verified the influence of RTP before performing conventional thermal calcination (CTC) on ZSM-58 membranes with various silica-to-aluminum (Si/Al) molar ratios. Using the developed method, an Al-containing ZSM-58 membrane without cracks was obtained, along with complete template removal by RTP, and it had higher CO2/CH4 selectivity. An all-silica ZSM-58 membrane without cracks was obtained by only using the ozone detemplating method. ZSM-58 crystals and membranes with various Si/Al molar ratios were analyzed by using Fourier-transform infrared (FTIR) spectroscopy to confirm the effects of RTP treatment. Al-containing ZSM-58 zeolites had higher silanol concentrations than all-silica zeolites, confirming many silanol condensations by RTP. The condensation of silanol forms results in the formation of siloxane bonds and stronger resistance to thermal stress; therefore, RTP caused crack suppression in Al-containing ZSM-58 membranes. The results demonstrate that Al-containing ZSM-58 zeolite membranes with high CO2 permeance and CO2/CH4 selectivity and minimal cracking can be produced by using RTP.

Keywords

• DDR
• ZSM-58
• rapid thermal processing
• zeolite membrane
• CO₂ separation