Mi. Zaki et al., In situ FTIR spectroscopic study of 2-propanol adsorptive and catalytic interactions on metal-modified aluminas, LANGMUIR, 17(13), 2001, pp. 4025-4034
Pure alumina was modified by additives of Ni, Ph, and Pt metal particles by
impregnation from aqueous solutions of corresponding precursor compounds s
and subsequent reduction in a stream of hydrogen at 400 degreesC for 2 h. T
he 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 particl
e 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 in
dicated that the metal additives provided the surface with dehydrogenation/
hydrogenation and cracking (hydrogenolysis) sites. Consequently, the initia
l alcohol dehydration selectivity of alumina (to give pure propene at 300-4
00 degreesC) was successfully challenged by a strong activity toward format
ion of major products of acetone, propane, and methane in the gas phase. A
range of relevant adsorbed species were characterized and found to result p
redominantly from adsorptive interactions of 2-propanol and acetone molecul
es. Surface reaction pathways were suggested, assuming concerted and sequen
tial 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 interac
tions.