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The crystallization mechanism of zeolites remains unclarified to date because of lack of effective techniques in characterizing the local structures of amorphous precursors under synthetic conditions. Herein

Small-pore zeolites are gaining increasing attention owing to their superior catalytic performance. Despite being critical for the catalytic activity and lifetime, postsynthetic tuning of bulk Si/Al ratios of small-pore zeolites has not been achieved with well-preserved crystallinity because of the limited mass transfer of aluminum species through narrow micropores. Here, we demonstrate a postsynthetic approach to tune the composition of small-pore zeolites using a previously unexplored strategy named pore-opening migration process (POMP). Acid treatment assisted by stabilization of the zeolite framework by organic cations in pores is proven to be successful for the removal of Al species from zeolite via POMP. Furthermore, the dealuminated AFX zeolite is treated via defect healing, which yields superior hydrothermal stability against severe steam conditions. Our findings could facilitate industrial applications of small-pore zeolites via aluminum content control and defect healing and could elucidate the structural reconstruction and arrangement processes for inorganic microporous materials.

The efficient separation of hydrogen from methane and light hydrocarbons for clean energy applications remains a technical challenge in membrane science. To address this issue, we prepared a graphene-wrapped MFI (G-MFI) molecular-sieving membrane for the ultrafast separation of hydrogen from methane at a permeability reaching 5.8 × 10 6 barrers at a single gas selectivity of 245 and a mixed gas selectivity of 50. Our results set an upper bound for hydrogen separation. Efficient molecular sieving comes from the subnanoscale interfacial space between graphene and zeolite crystal faces according to molecular dynamic simulations. The hierarchical pore structure of the G-MFI membrane enabled rapid permeability, indicating a promising route for the ultrafast separation of hydrogen/methane and carbon dioxide/methane in view of energy-efficient industrial gas separation.