Efficient
separation of hydrogen under steam reforming conditions
is important for the development of clean energy sources. Although
high-temperature and steam-stable membranes with high fluxes and large
separation factors would be valuable for such an application, their
fabrication remains a challenge. Silicon-based ceramic membranes are
particularly promising due to their high temperature resistance and
excellent chemical stability. In this study, we propose a new synthetic
route for fabricating nanoporous, asymmetric membranes via the pyrolysis
of silicon-containing polymer films deposited by initiated chemical
vapor deposition (iCVD) on macroporous silicon carbide supports. Specifically,
we systematically investigated the change in the chemical structure
of poly(2,4,6,8-tetravinyl-2,4,6,8-tetramethyl cyclotetrasiloxane)
films at different pyrolysis temperatures and found that the complete
transition to a silica membrane occurred at ∼1100 °C.
Three different supports composed of silicon carbide powders of varying
sizes were tested for membrane preparation. It was found that membranes
formed with our process were microporous with separation factors several
times above the corresponding Knudsen factors. Our synthetic route,
therefore, offers a scalable and solventless method for producing
silicon-based ceramic membranes for high-temperature separation and
sensor applications.