In situ FTIR spectroscopic study of 2-propanol adsorptive and catalytic interactions on metal-modified aluminas

被引:59
|
作者
Zaki, MI [1 ]
Hasan, MA [1 ]
Pasupulety, L [1 ]
机构
[1] Kuwait Univ, Fac Sci, Dept Chem, Safat 13060, Kuwait
关键词
D O I
10.1021/la001810r
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Pure alumina was modified by additives of Ni, Ph, and Pt metal particles by impregnation from aqueous solutions of corresponding precursor compounds sand subsequent reduction in a stream of hydrogen at 400 degreesC for 2 h. The catalysts thus obtained were subjected to N-2, H-2, and O-2 sorptometry, high-resolution electron microscopy, and X-ray photoelectron spectroscopy. Accordingly, the metal reducibility, surface area, dispersion, and particle size were determined. Thin wafers of the catalysts, pretreated in situ in a specially designed IR reactor/cell, were exposed to 2-propanol vapor at various temperatures (room temperature to 400 degreesC) for 10 min, and IR spectra of the gas-phase and adsorbed species were measured. The results indicated that the metal additives provided the surface with dehydrogenation/hydrogenation and cracking (hydrogenolysis) sites. Consequently, the initial alcohol dehydration selectivity of alumina (to give pure propene at 300-400 degreesC) was successfully challenged by a strong activity toward formation of major products of acetone, propane, and methane in the gas phase. A range of relevant adsorbed species were characterized and found to result predominantly from adsorptive interactions of 2-propanol and acetone molecules. Surface reaction pathways were suggested, assuming concerted and sequential interactions of the alcohol (and product) molecules with acid-base and metal sites. It was believed that gas-phase migration of alkene molecules and surface diffusion of hydrogen adatoms facilitate the sequential interactions.
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页码:4025 / 4034
页数:10
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