Journal
CATALYSIS TODAY
Volume 73, Issue 1-2, Pages 83-93Publisher
ELSEVIER
DOI: 10.1016/S0920-5861(01)00521-1
Keywords
Na+ and Ba2+ X and Y zeolites; IR spectroscopy of adsorbed CO and CO2
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Sodium and barium forms of X (Si:Al = 1.3) and Y (Si:Al = 3.5) zeolites were studied by IR spectroscopy of adsorbed CO (at low temperature) and CO2 (at room temperature). In BaY, Ba2+ ions substitute almost completely the Na+ ones at sites SIX, and new, stronger Lewis acid sites are formed. In the supercages of X zeolite in sodium form, the Na+ ions are present at both S-II and S-III, sites. After exchange with Ba2+ almost all alkali ions in the supercages are substituted by alkaline-earth ions, which occupy sites S-II only. Also, in this case, Ba2+ ions behave as stronger Lewis acid centres than Na+ ions at such sites. However, their Lewis acidity is weaker than for Ba2+ species at sites S-II in Y zeolite, because of the lower Si:Al ratio. IR spectra of adsorbed CO2 revealed that the Lewis basicity of the framework oxygen atoms of NaX, put in evidence by the formation of carbonate-like species, is strongly decreased by exchanging Na+ with Ba2+, as in BaX CO2 is linearly polarised on the cations only. Calculation of the partial negative charge on the framework oxygens (carried out on the basis of the Sanderson's electronegativity equalisation method) confirmed this effect for X systems, and indicated that the exchange of Na+ with Ba2+ resulted in a decrease in basicity in the case of Y zeolite also, (which even in the sodium form was unable to give rise to carbonate-like species by interaction with CO2). (C) 2002 Elsevier Science B.V. All rights reserved.
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