Temperature programmed isotopic exchange (TPIE) of oxygen and pulsed methane combustion experiments were used to investigate the contribution of oxygen from the support in the methane combustion reaction over alumina-and zirconia-supported palladium. TPIE experiments show that PdO is more active than reduced palladium for oxygen exchange between the catalyst and gas phase. Experiments performed on initially reduced catalysts produced a partially oxidized palladium phase containing both oxygen isotopes, suggesting that oxygen exchange between solid phases proceeds simultaneously with Pd oxidation. Reactivity tests performed with labeled reaction mixture pulses showed an important contribution of the support in the overall oxygen balance. Adsorbed oxygen is much more rapidly exchanged on zirconia-supported Pd than on alumina-supported Pd, and the isotopic exchange between the gas phase and the catalyst is strongly accelerated in the presence of methane. This is assigned to an increase in the concentration of oxygen vacancies in the support via oxidation of reaction intermediates on the support.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.