Synthesis of Silica Membranes by Chemical Vapor Deposition Using a Dimethyldimethoxysilane Precursor

• Main Authors: S. Ted Oyama, Haruki Aono, Atsushi Takagaki, Takashi Sugawara, Ryuji Kikuchi
• Format: Article
• Language: English
• Published: MDPI AG 2020-03-01
• Series: Membranes
• Subjects: silica-alumina membrane; dimethyldimethoxysilane (dmdmos); hydrothermal stability; chemical vapor deposition; gamma-alumina intermediate layers; hydrogen helium separation
• Online Access: https://www.mdpi.com/2077-0375/10/3/50

Silica-based membranes prepared by chemical vapor deposition of tetraethylorthosilicate (TEOS) on γ-alumina overlayers are known to be effective for hydrogen separation and are attractive for membrane reactor applications for hydrogen-producing reactions. In this study, the synthesis of the membranes was improved by simplifying the deposition of the intermediate γ-alumina layers and by using the precursor, dimethyldimethoxysilane (DMDMOS). In the placement of the γ-alumina layers, earlier work in our laboratory employed four to five dipping-calcining cycles of boehmite sol precursors to produce high H₂ selectivities, but this took considerable time. In the present study, only two cycles were needed, even for a macro-porous support, through the use of finer boehmite precursor particle sizes. Using the simplified fabrication process, silica-alumina composite membranes with H₂ permeance > 10^−7 mol m^−2 s^−1 Pa^−1 and H₂/N₂ selectivity >100 were successfully synthesized. In addition, the use of the silica precursor, DMDMOS, further improved the H₂ permeance without compromising the H₂/N₂ selectivity. Pure DMDMOS membranes proved to be unstable against hydrothermal conditions, but the addition of aluminum tri-sec-butoxide (ATSB) improved the stability just like for conventional TEOS membranes.