| Article ID | Journal | Published Year | Pages | File Type |
|---|---|---|---|---|
| 62140 | Journal of Catalysis | 2009 | 9 Pages |
Previous study suggested that either high oxygen mobility in layer-structured (La1−ySry)2MnO4 perovskite or high oxygen diffusion through intergrain boundaries is the reason why multiphase La1−xSrxMnO3 samples exhibit a high catalytic activity in high temperature N2O decomposition. The absence of inhibiting effect of oxygen on the reaction rate for these samples allows us to suppose that surface segregation of layered perovskite increases oxygen mobility and facilitates oxygen desorption from the surface. In this paper, we aimed at determining the influence of surface composition on oxygen mobility and catalytic activity in high temperature N2O decomposition. By means of steady-state isotopic transient kinetic analysis (SSITKA) the mechanism and kinetics of oxygen exchange were elucidated for three La1−xSrxMnO3 (x = 0, 0.3, and 0.5) samples considerably differing in phase composition and catalytic activity. The results obtained indicate that inactive single-phase LaMnO3 exhibits both the lowest rate of oxygen exchange on the surface and the lowest rate of oxygen diffusion in the bulk. For La0.3Sr0.7MnO3, the increased values of both rates as compared with LaMnO3 can be interpreted as the appearance of a fast pathway of oxygen transfer through vacancies formed in the perovskite lattice to compensate the reduced cation charge. The highest values of the content of fast-exchangeable oxygen and oxygen diffusion coefficient were found for a multiphase sample containing layered perovskite, thus providing a strong correlation between oxygen mobility and catalytic activity in the reaction of nitrous oxide decomposition.
Graphical abstractMechanism of oxygen exchange in single- and multiphase La–Sr–Mn–O samples was studied by steady-state isotopic transient kinetic analysis (900 °C). Strong correlation between oxygen mobility and the rate of N2O decomposition was found.Figure optionsDownload full-size imageDownload high-quality image (291 K)Download as PowerPoint slide
