Catalytic cracking deposition (CCD) of methyldiethoxysilane (MDES) can be used to tune the zeolitic pores over MFI zeolite membranes for H 2 /CO 2 separation. CCD of MDES over MFI zeolite was investigated to reveal the catalytic cracking behavior of silane. The cracking products were found to be strongly influenced by cracking temperature and acid sites. The increases of temperature and acid sites were beneficial to CCD of MDES in the zeolitic pores, which could effectively reduce the pore size of zeolite. H + ion exchange on MFI zeolite membranes has been adopted to increase acid sites in the membrane layer. The membranes were further modified by on-stream CCD of MDES to improve H 2 selectivity. The achieved H 2 selectivity over ion-exchanged membranes was much higher than that for MFI zeolite membranes without ion exchange. Typically, an ionexchanged membrane after CCD modification possessed an H 2 /CO 2 separation factor of 42.6 and H 2 permeance of 2.82 × 10 −7 mol/m 2 •s•Pa at 500 °C.
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