Linear Correlations between Adsorption Energies and HOMO Levels for the Adsorption of Small Molecules on TiO2 Surfaces
Linear Correlations between Adsorption Energies and HOMO Levels for the Adsorption of Small Molecules on TiO2 Surfaces
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DOI：
10.1021/acs.jpcc.9b05707
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发表时间：
2019-08
期刊：
影响因子：
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通讯作者：
T. Kamachi;Toshinobu Tatsumi;Takashi Toyao;Y. Hinuma;Z. Maeno;S. Takakusagi;S. Furukawa;Ichigaku Takigawa;K. Shimizu
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文献类型：
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作者：
T. Kamachi;Toshinobu Tatsumi;Takashi Toyao;Y. Hinuma;Z. Maeno;S. Takakusagi;S. Furukawa;Ichigaku Takigawa;K. Shimizu
吸附是固体表面催化的基本步骤，因此，理解它对于解释其行为非常重要。这项工作利用周期密度研究了各种小分子，包括 H2、N2、CO、CO2、CH4、NH3、H2O、H2S、二甲亚砜、烷烃、烯烃、炔烃、芳香族化合物、醇、醛、酮、腈、羧酸、酰胺和胺在 TiO2 锐钛矿 (101) 和金红石 (110) 表面上的吸附泛函理论计算和统计方法。吸附能是在相同的理论水平上计算的，以获得干净且一致的数据集。这些分子的吸附能与其最高占据分子轨道（HOMO）能级之间观察到线性关系，而最低未占据分子轨道能级则没有明显的相关性。通过将这些分子分为两个子组，可以改善吸附能和 HOMO 水平之间的相关性：氢...
Adsorption is a fundamental step in catalysis on a solid surface, and therefore, its understanding is important for explaining its behavior. This work investigated the adsorption of various small molecules, including H2, N2, CO, CO2, CH4, NH3, H2O, H2S, dimethyl sulfoxide, alkanes, alkenes, alkynes, aromatic compounds, alcohols, aldehydes, ketones, nitriles, carboxylic acids, amides, and amines, on the anatase (101) and rutile (110) surfaces of TiO2, using periodic density functional theory calculations and statistical methods. Adsorption energies were computed at the same level of theory to obtain a clean and consistent data set. A linear relationship was observed between the adsorption energies of these molecules and their highest occupied molecular orbital (HOMO) levels, whereas no obvious correlation was evident for the lowest unoccupied molecular orbital levels. Improved correlations between the adsorption energies and HOMO levels were generated by dividing these molecules into two subgroups: hydroca...