Browsing by Author "Rouxhet, Paul G."

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    Evolution of the Acidic Properties of Silica—Alumina Gels as a Function of Chemical Composition: Infrared Approach
    (Journal of the Chemical Society : Faraday Transaction - I. The Chemical Society, London. 1977, 73 (2), 1977) Scokart, Paul O.; Declerck, Francois D.; Sempels, Raymond E.; Rouxhet, Paul G.
    The adsorption of pyridine and CD3CN on silica–alumina gels covering the whole composition range (0–100 % Al2O3) has been studied by infrared spectroscopy, the amount adsorbed being measured by an electrobalance. The measurement of the maximum intensity reached by the bands of strongly adsorbed species has allowed us to sketch the evolution of the surface Brönsted sites and various types of Lewis sites as a function of the chemical composition of the adsorbant. The overall concentration of Lewis sites increases smoothly from 0 to 75 % Al2O3; the sharper increase in the high Al2O3 range is mainly due to weak sites which are revealed by a pyridine band at 1615 cm–1 while pyridine coordinated with strong Lewis sites gives a band at 1625 cm–1. The concentration of acid sites associated with the mixed silica–alumina phase corresponds to the more acidic sites observed by titration in non aqueous media. A high proportion of them are strongly acidic hydroxlys which are detected by absorption of H bond acceptors. The mixed phase develops as the Al2O3 content increases from 0 to 25 %; above 50 % Al2O3 it is progressively diluted in a mixture with other phases and is no longer observed above 85 % Al2O3.
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    Hydrogen Bond Strengths and Acidities of Hydroxyl Groups on Silica-Alumina Surfaces and in Molecules in Solution
    (Journal of the Chemical Society : Faraday Transaction - I. The Chemical Society, London. 1974, 70 (11), 1974) Rouxhet, Paul G.; Sempels, Raymond E.
    The properties of hydroxyl groups on mixed silica–alumina gels (0–50 % Al2O3) have been studied by adsorbing weak H bond accepting molecules onto the gels and recording the OH stretching infrared band. Additional measurements on silica gel and compilation of numerous literature data have shown that frequency shift measurements, or series of ΔvOH measurements condensed into BHW (Bellamy, Hallam and Williams) slopes, provide a reliable estimate of the OH acidity. The resulting scale is independent of the atom to which the hydroxyl is attached; it may be used for surfaces of solids as well as for solutions. The results obtained for silica–alumina show that two distinct populations of hydroxyl groups are present. Hydroxyl groups of type 1 are identical with those present on the surface of silica. The spectra show the presence of hydroxyl groups of a second type, the proportion of which increases as the Al content of the gel rises; their acidity corresponds to a pKa between –4 and –8 and they are presumably the sites responsible for the protonation observed upon adsorption of pyridine or ammonia.