High-Pressure Phase Transition, Pore Collapse, and Amorphization in the Siliceous 1D Zeolite, TON

Abstract

The siliceous zeolite TON with a 1-D pore system was studied at high pressure by X-ray diffraction, infrared spectroscopy, and DFT calculations. The behavior of this material was investigated using nonpenetrating pressure-transmitting media. Under these conditions, a phase transition from the Cmc21 to a Pbn21 structure occurs at close to 0.6 GPa with doubling of the primitive unit cell based on Rietveld refinements. The pores begin to collapse with a strong increase in their ellipticity. Upon decreasing the pressure below this value the initial structure was not recovered. DFT calculations indicate that the initial empty pore Cmc21 phase is dynamically unstable. Irreversible, progressive pressure-induced amorphization occurs upon further increases in pressure up to 21 GPa. These changes are confirmed in the mid- and far-infrared spectra by peak splitting at the Cmc21 to Pbn21 phase transition and strong peak broadening at high pressure due to amorphization.