Kinetics and Mechanisms of CO Oxidation on Nd1-xSrxCoO3-y Catalysts with Static and Flow Methods

Perovskite-type Nd1-xSrxCoO3-y catalysts with various Sr mole fraction were prepared and investigated for the effect of Sr substitution on their catalytic activities in the oxidation of carbon monoxide. Utilizing the static and flow methods, kinetic studies have been carried out between 373 and 523 K. The initial reaction was investigated by the static reactor system using a differential photoacoustic cell, and for the study of reaction stage showing a constant catalytic activity after an initial stage characterized by high reaction rates, the flow reactor system using on-line gas chromatography was employed. The catalytic activity increased with increasing amounts of Sr substitution for Nd in NdCoO3 compounds, and it also increased with higher reaction temperature within the range of 373-523 K. Kinetic data obtained in an initial reaction stage by CO2 photoacoustic spectroscopy showed that the reaction partial orders to CO and O2 were 0.8-0.9 and 0, respectively. In the reaction stage showing a constant catalytic activity after an initial stage, the oxidation was found to be first order with respect to CO and 0.5 order with respect to O2. The concentration of oxygen vacancy in the solid catalyst was shown to be the controlling factor for the oxidation of carbon monoxide. According to the experimental results, the mechanisms of the CO oxidation processes are discussed, and it is believed that O2 adsorbs on the oxygen vacancies (Vo x ) formed by Sr substitution while CO adsorbs on the lattice oxygens during the reaction process.