Zeolite membranes are thermally, chemically, and mechanically stable. They also have tunable molecular sieving and catalytic ability. These unique properties make zeolite membrane an excellent candidate for use in catalytic membrane reactor applications related to coal conversion and gasification, which need high temperature and high pressure range separation in chemically challenging environment where existing technologies are inefficient or unable to operate. Small pore, good quality, and thin zeolite membranes are needed for highly selective H{sub 2} separation from other light gases (CO{sub 2}, CH{sub 4}, CO). However, zeolite membranes have not been successful for H{sub 2} separation from light gases because the zeolite pores are either too big or the membranes have a large number of defects. The objective of this study is to develop zeolite membranes that are more suitable for H{sub 2} separation. In an effort to tune the size of zeolite pores and/or to decrease the number of defects, medium-pore zeolite B-ZSM-5 (MFI) membranes were synthesized and silylated. Silylation on B-ZSM-5 crystals reduced MFI-zeolite pore volume, but had little effect on CO{sub 2} and CH{sub 4} adsorption. Silylation on B-ZSM-5 membranes increased H{sub 2} selectivity both in single component and in mixtures with CO{sub 2}CO{sub 2}, CH{sub …