Infrared spectroscopic characterization of dehydration and accompanying phase transition behaviors in NAT-topology zeolites |
| |
Authors: | Email author" target="_blank">Hsiu-Wen?WangEmail author David?L?Bish |
| |
Institution: | (1) Department of Geological Sciences, Indiana University, 1001 East 10th Street, Bloomington, IN 47405, USA;(2) Present address: Geochemistry and Interfacial Science Group, Chemical Science Division, Oak Ridge National Laboratory, 4100, C350, MS 6110, Oak Ridge, TN 37831, USA |
| |
Abstract: | Relative humidity (
P\textH 2 \textO P_{{{\text{H}}_{ 2} {\text{O}}}} , partial pressure of water)-dependent dehydration and accompanying phase transitions in NAT-topology zeolites (natrolite,
scolecite, and mesolite) were studied under controlled temperature and known
P\textH 2 \textO P_{{{\text{H}}_{ 2} {\text{O}}}} conditions by in situ diffuse-reflectance infrared Fourier transform spectroscopy and parallel X-ray powder diffraction.
Dehydration was characterized by the disappearance of internal H2O vibrational modes. The loss of H2O molecules caused a sequence of structural transitions in which the host framework transformation path was coupled primarily
via the thermal motion of guest Na+/Ca2+ cations and H2O molecules. The observation of different interactions of H2O molecules and Na+/Ca2+ cations with host aluminosilicate frameworks under high- and low-
P\textH 2 \textO P_{{{\text{H}}_{ 2} {\text{O}}}} conditions indicated the development of different local strain fields, arising from cation–H2O interactions in NAT-type channels. These strain fields influence the Si–O/Al–O bond strength and tilting angles within and
between tetrahedra as the dehydration temperature is approached. The newly observed infrared bands (at 2,139 cm−1 in natrolite, 2,276 cm−1 in scolecite, and 2,176 and 2,259 cm−1 in mesolite) result from strong cation–H2O–Al–Si framework interactions in NAT-type channels, and these bands can be used to evaluate the energetic evolution of Na+/Ca2+ cations before and after phase transitions, especially for scolecite and mesolite. The 2,176 and 2,259 cm−1 absorption bands in mesolite also appear to be related to Na+/Ca2+ order–disorder that occur when mesolite loses its Ow4 H2O molecules. |
| |
Keywords: | |
本文献已被 SpringerLink 等数据库收录! |
|