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Computerized infrared spectroscopic study of surface reactions on selected lanthanide oxides

Thesis/Dissertation ·
OSTI ID:6204630
The natures of adsorption sites on La/sub 2/O/sub 3/, Nd/sub 2/O/sub 3/, and selected praseodymium oxides were investigated by examining surface reactions of probe molecules using computerized transmission ir spectroscopy on unsupported samples. Additionally, the rehydration/dehydration behavior and crystallographic phase transitions of these oxides were examined in pretreatment temperature experiments involving rehydration of the sesquioxides to hydroxides by water exposure. Following rehydration of La/sub 2/O/sub 3/ to La(OH)/sub 3/, the effect of increasing vacuum pretreatment temperature (350 to 1000/sup 0/C) is to gradually remove surface hydroxyl and carbonate entities (up to 650/sup 0/C), and increase the degree of A-type crystallinity. Increasing crystallinity causes a concomitant decrease in surface oxide basicity. The removal of hydroxyl and carbonate species, as well as increases in oxide basicity, strongly correlated to increases in certain catalytic activities. The adsorption of NH/sub 3/, CO/sub 2/, mixtures of NH/sub 3/ and CO/sub 2/, formic acid, acetic acid, acetaldehyde, and ethanol on the oxides was determined to weakly coordinate in Ln/sup 3 +/ sites, and the surface reactions are discussed. Heating was found to desorb the adsorbed compounds and/or causes changes of the originally adsorbed form into other compounds. The effects of temperature on both adsorption and desorption are reported.
Research Organization:
Texas A and M Univ., College Station (USA)
OSTI ID:
6204630
Country of Publication:
United States
Language:
English