Study of Argon Gas Adsorption in Ordered Mesoporous MFI Zeolite Framework

Abstract

An ordered mesoporous MFI zeolite material (Meso-MFI) was prepared by using CMK-type mesoporous carbons as a hard template. The Meso-MFI exhibits both structural and adsorption differences compared to the conventional bulk MFI zeolite. To study the argon (Ar) adsorption process in Meso-MFI, an in situ gas adsorption powder X-ray diffraction (XRD) analysis was performed using synchrotron X-ray source. Structural rearrangement of the mesoporous MFI zeolite upon Ar adsorption at low temperature (83 K) was intensively studied together with Ar adsorption process in Meso-MFI. We observed that a structural transition of the Meso-MFI zeolite framework from monoclinic (P21/n) to orthorhombic (Pnma) occurred at around 126 Pa at 83 K. Positions of Ar atoms are determined as a function of the Ar gas pressure through Rietveld refinement of powder XRD data. Ar atoms are observed at straight channels, sinusoidal channels, and the intersection of these channels at low pressure. As gas pressure increases, Ar atoms in the pore intersection are pulled off from the intersection toward the straight and sinusoidal channels. The pore shape of the straight channel is changed accordingly with the amount of adsorbed Ar atoms within the pores from circular to oval. These results indicate that Ar adsorption induces not only continuous rearrangement of framework atoms but also symmetry change in the Meso-MFI. A molecular simulation study combined with Rietveld refinement of in situ XRD data provided a full understanding of the adsorption process of Ar in Meso-MFI.