Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA.
Phys Chem Chem Phys. 2012 Dec 28;14(48):16595-602. doi: 10.1039/c2cp42288c. Epub 2012 Aug 28.
The interaction of atomic hydrogen with the majority (101) surface of anatase TiO(2) is studied using density functional theory calculations both with a standard semi-local functional and with the inclusion of on-site Coulomb repulsion terms. We investigate the energetics of different adsorption configurations at surface and subsurface sites and different coverages, from low to one monolayer, as well as diffusion pathways among the different sites and recombinative H(2) desorption barriers. While H(2) desorption is the energetically most favorable process, the diffusion of H into the subsurface is found to be at least equally favorable kinetically. It is further shown that subsurface oxygen vacancies on reduced anatase are favorable adsorption sites for hydrogen atoms.
采用密度泛函理论计算方法，使用标准局域泛函和包含局域库仑排斥项两种方法，研究了原子氢与锐钛矿 TiO(2)（101）面的相互作用。我们研究了在表面和次表面位置以及不同覆盖度（从低至单层）下不同吸附构型的能量，以及不同位置之间的扩散途径和复分解 H(2)脱附势垒。虽然 H(2)脱附是能量上最有利的过程，但氢进入次表面的扩散在动力学上至少同样有利。进一步表明，还原锐钛矿中的次表面氧空位是氢原子的有利吸附位。
