Home Physical Sciences PH₂O-dependent structural phase transitions in the zeolite mesolite: Real- and reciprocal-space crystal structure refinements
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PH₂O-dependent structural phase transitions in the zeolite mesolite: Real- and reciprocal-space crystal structure refinements

  • Hsiu-Wen Wang EMAIL logo , David L. Bish and Hongwei Ma
Published/Copyright: April 2, 2015
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Abstract

The response of the mesolite crystal structure (Na16Ca16Al48Si72O240·64H2O) to dehydration was evaluated as a function of temperature and partial pressure of water (i.e., PH₂O or relative humidity, RH) using laboratory X-ray powder diffraction (XRD; CuKα radiation) and synchrotron X-ray pair distribution function (PDF) methods. At 425 °C under low-PH₂O conditions (PH₂O ≤ ~1.3 mbar), dehydrated mesolite preserved the long-range ordered aluminosilicate framework structure, which has not been previously observed. This new dehydrated phase, x-metamesolite, has unit-cell parameters [a = 16.731(3) Å, b = 17.822(2) Å, c = 6.312(1) Å, V = 1882.5(5) Å3, and possible space group Fdd2] similar to those of other dehydrated natrolite phases (either α1- or α2-metanatrolite). Conversely, under high-PH₂O conditions (PH₂O > ~1.3 mbar), dehydrated mesolite became amorphous (amorphous T5O10) at 425 °C. The local structure of amorphous T5O10 was characterized by PDF analyses, which showed the formation of twisted T5O10 nano-fibers [with dimensions (LWH) of ~6.9 × 6.9 × 6.3 Å] resulting from breakage of the mesolite aluminosilicate framework. The two distinct high-temperature PH₂O-dependent phase transition paths illustrate the importance of considering the combined effects of temperature and PH₂O in mesolite. In addition, the low-temperature phase transition in mesolite, involving order-disorder of the extraframework cations, also showed a PH₂O-dependent transition temperature. Although, there is no path dependence on PH₂O for this transition, the local arrangement of Na, Ca, and vacancies in disordered metamesolite (formed through the extraframework cation order-disorder phase transition) likely influences the thermal stability of the aluminosilicate framework during further heating.

Received: 2009-11-3
Accepted: 2010-1-2
Published Online: 2015-4-2
Published in Print: 2010-5-1

© 2015 by Walter de Gruyter Berlin/Boston

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