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Experimental and ab initio infrared study of χ-, κ- and α-aluminas formed from gibbsite

Type
Articles dans des revues avec comité de lecture
Author
FAVARO, Laurent
1373 Laboratoire d'étude des matériaux hors équilibre [LEMHE]
BOUMAZA, A.
1373 Laboratoire d'étude des matériaux hors équilibre [LEMHE]
300790 centre universitaire de Khenchela
ROY, Pascale
1744 Synchrotron SOLEIL [SSOLEIL]
LÉDION, Jean
469561 ENSAM-LIM
SATTONNAY, Gaël
33665 Institut de Chimie Moléculaire et des Matériaux d'Orsay [ICMMO]
BRUBACH, Jean Blaise
1744 Synchrotron SOLEIL [SSOLEIL]
HUNTZ, Anne Marie
1373 Laboratoire d'étude des matériaux hors équilibre [LEMHE]
33665 Institut de Chimie Moléculaire et des Matériaux d'Orsay [ICMMO]
TÉTOT, Robert
1373 Laboratoire d'étude des matériaux hors équilibre [LEMHE]

URI
http://hdl.handle.net/10985/17901
DOI
10.1016/j.jssc.2010.02.010
Date
2010
Journal
Journal of Solid State Chemistry

Abstract

χ-, κ- and α-alumina phases formed by dehydration of micro-grained gibbsite between 773 and 1573 K are studied using infrared spectroscopy (IR). The structural transitions evidenced by X-ray diffraction (XRD) were interpreted by comparing IR measurements with ab initio simulations (except for the χ form whose complexity does not allow a reliable simulation). For each phase, IR spectrum presents specific bands corresponding to transverse optical (TO) modes of Al-O stretching and bending under 900 cm-1. The very complex χ phase, obtained at 773 K, provides a distinctive XRD pattern in contrast with the IR absorbance appearing as a broad structure extending between 200 and 900 cm-1 resembling the equivalent spectra for γ-alumina phase. κ-alumina is forming at 1173 K and its rich IR spectrum is in good qualitative agreement with ab initio simulations. This complexity reflects the large number of atoms in the κ-alumina unit cell and the wide range of internuclear distances as well as the various coordinances of both Al and O atoms. Ab initio simulations suggest that this form of transition alumina demonstrates a strong departure from the simple pattern observed for other transition alumina. At 1573 K, the stable α-Αl2Ο3 develops. Its IR spectra extends in a narrower energy range as compared to transition alumina and presents characteristics features similar to model α-Αl2Ο3{dot operator} Ab initio calculations show again a very good general agreement with the observed IR spectra for this phase. In addition, for both κ- and α-Αl2Ο3, extra modes, measured at high energy (above 790 cm-1 for κ and above 650 cm-1 for α), can originate from either remnant χ-alumina or from surface modes

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