The isothermal isotopic exchange reaction of O-18(2) with O-16 of chro
mium(VI) oxide supported on zirconia, alumina, and titania has been in
vestigated with in situ laser Raman spectroscopy. The isotopic exchang
e reaction is dependent on the support type, the Cr loading, and the r
eaction temperature. Complete isotopic exchange of chromium(VI) oxide
with O-18(2) is difficult to achieve and requires several successive b
utane reduction-O-18(2) oxidation cycles at relatively high temperatur
es. The efficiency of the isothermal isotopic exchange reaction increa
ses from alumina over titania to zirconia and with increasing Cr loadi
ng and reduction temperature. The observed Raman shifts upon isotopic
labeling are consistent with a mono-ore surface chromium oxide(VI) spe
cies.