Particle Size Effect of Hydride Formation and Surface Hydrogen Adsorption of Nanosized Palladium Catalysts: L3 Edge vs K Edge X-ray Absorption Spectroscopy

The particle size effect oil the formation of palladium hydride and on Surface hydrogen adsorption was studied at room temperature using in situ X-ray absorption spectroscopy at the Pd K and L-3 edges. Hydride formation was indirectly observed by lattice expansion in Pd K edge XANES spectra and by EXAFS analysis. Hydride formation was directly detected in the L-3 edge spectra. A characteristic spectral feature caused by the formation of a Pd-H antibonding state showed strong particle size dependence. The L-3 edge spectra were reproduced using full multiple scattering analysis and density of state calculations, and the contributions of bulk absorbed and surface hydrogen to the XANES spectra could be distinguished. The ratio of hydrogen on the Surface versus that in the bulk increased with decreasing particle size, and smaller particles dissolved less hydrogen.