The transient, isothermal CO oxidation activity of ceria and Pt/ceria was s
tudied in the temperature range 40-230 degrees C. The influence of oxidativ
e and reductive pre-treatments, at different temperatures, on the low-tempe
rature activity was investigated. Reductive pre-treatment of Pt/ceria was f
ound to-increase the activity; the temperature required to reach a certain
activity was lowered by about 100-140 degrees C by reductive pre-treatment.
The temperature of reduction, 200 degrees C, 300 degrees C or 500 degrees
C, had no dramatic effect on this activity gain. However, for a moderate-di
spersion sample, the activity was higher after reduction at 200 degrees C a
nd 300 degrees C than after reduction at 500 degrees C. XPS measurements sh
owed that Pt was not completely reduced at 200 degrees C. The high activity
obtained after a reductive pre-treatment was almost completely diminished
by a mild oxidation at room temperature. The high activity is discussed in
terms of reduction of ceria in the vicinity of Pt particles.
Isotopically labeled oxygen was used to discriminate between possible react
ion schemes. The isotope distribution indicates that initially, CO mainly r
eacts with oxygen from the catalyst, even on the pre-reduced sample. Howeve
r, it was difficult to draw unambiguous conclusions from the isotope distri
bution, since there is likely also isotope exchange.
The presence of water in the feed had no large influence on the total activ
ity for CO2 formation at low temperatures, but it altered the isotope compo
sition of the CO2 formed, since some CO is oxidized by water instead of by
oxygen. At temperatures above 140 degrees C, water did increase the total C
O oxidation activity by the WGS reaction. (C) 1999 Elsevier Science B.V. Al
l rights reserved.