Electronic Origin of the Surface Reactivity of Transition-Metal-Doped TiO2(110)

详细信息    查看全文

• 作者：M贸nica Garc铆a-Mota ; Aleksandra Vojvodic ; Frank Abild-Pedersen ; Jens K. N酶rskov
• 刊名：The Journal of Physical Chemistry C
• 出版年：2013
• 出版时间：January 10, 2013
• 年：2013
• 卷：117
• 期：1
• 页码：460-465
• 全文大小：293K
• 年卷期：v.117,no.1(January 10, 2013)
• ISSN：1932-7455

文摘

We investigate the surface reactivity of doped rutile M-TiO₂(110) (M = V, Cr, Mo, W, Mn, Fe, Ru, Co, Ir, and Ni) using density functional theory (DFT) and Hubbard-U corrected DFT calculations (DFT+U method). The oxygen adsorption bond, used as the surface reactivity measure, is stronger on the doped TiO₂ surfaces as compared with that on the undoped TiO₂ surface. We relate this increase in reactivity of the doped TiO₂ surfaces to the presence of localized surface resonances and surface states in the vicinity of the Fermi level. We find that the center of these localized states on doped TiO₂ is a good descriptor for the oxygen adsorption energy. The inclusion of the Hubbard-U correction to DFT barely modifies the oxygen adsorption energy on undoped TiO₂, whereas it destabilizes the oxygen adsorption energies on doped TiO₂ when compared with results from standard DFT. Nevertheless, we find that the oxygen adsorption energy trends predicted by a standard GGA-DFT functional are reproduced when the Hubbard-U correction is applied.