CO Oxidation to CO on Uranium Dioxide Molecules through Intermediate OU(η-CO).

Investigations on the reactions of uranium oxide molecules with CO offer new inspiration for the design of promising high-efficiency catalysts for CO activation using actinide materials. Herein, we contribute a combined matrix-isolation infrared spectroscopic and theoretical study of CO oxidation to CO on uranium dioxide (UO) molecules in solid argon. The reaction intermediate OU(η-CO) is generated spontaneously at the bands of 1893.0, 870.6, and 801.3 cm during codeposition and annealing. Upon the following irradiation, CO is substantially produced by the consumption of OU(η-CO), indicating the catalytic conversion of CO to CO through the intermediate OU(η-CO). In CO isotopic substitution experiments, the yields of OCO convincingly confirm that one of the oxygen atoms in CO derives from UO. The reaction pathways are discussed based on the theoretical and experimental results.