کد مقاله | کد نشریه | سال انتشار | مقاله انگلیسی | نسخه تمام متن |
---|---|---|---|---|
5424968 | 1395843 | 2008 | 8 صفحه PDF | دانلود رایگان |
The effects of Zr doping on the atomic and electronic properties of the ceria(1Â 1Â 1) surface are studied using first-principles density functional theory with the inclusion of on-site Coulomb interaction. The atomic structures, electronic structure, and the vacancy formation energies of the Zr-doped and undoped ceria(1Â 1Â 1) surfaces are compared. It is found that (i) Zr doping induces a severe distortion of the unreduced surface structure; (ii) at the reduced Zr-doped ceria(1Â 1Â 1) surface, the oxygen anions around the oxygen vacancy show much larger displacements than those on the pure CeO2(1Â 1Â 1) surface; (iii) an oxygen vacancy is more easily formed around the Zr dopant, and the reduction energy is lowered by about 0.5Â eV; (iv) the excess electrons left by the removed oxygen atom localize on the two Ce cations neighboring the vacancy and thus brings about the reduction of the two Ce4+ ions; and (v) the atomic structure modification induced by the Zr doping plays a vital role in facilitating the reduction of the ceria-zirconia solid solution as compared to the pure ceria.
Journal: Surface Science - Volume 602, Issue 6, 15 March 2008, Pages 1199-1206