PNNL

Abstract

We present an investigation of oxygen (18O) uptake measurements in 1 ?m thick nanocrystalline ceria films grown on single crystal Al2O3 (0001) by nuclear reaction analysis (NRA). Oxygen uptake measurements were carried out in the temperature range of 200 0C-600 0C at a background 18O pressure of 4.0 x 10-6 Torr. Average grain-size in the as-grown films, synthesized by sol-gel process was ~ 3 nm confirmed by high-resolution transmission electron microscopy (HRTEM) and X-ray diffraction (XRD) measurements. From the diffusion depth profiles, changes in intensity and slopes in surface and interface regions indicate dominating oxygen mobility effects. Oxygen desorption is clearly distinguishable in the film surface region as a result of shift in the oxygen peak intensity. It is argued that high defect density in nanocrystalline ceria which is associated with nano-grain surface combined with intermediate temperature reducing environment triggers multiple processes like diffusion, desorption and exchange interaction. The promising nature of NRA is realized as an effective tool to acquire the depth-dependent information regarding such complex reactions that exists in nanocrystalline environment.