Density Functional Theory Calculations of Oxygen Vacancy Formation and Subsequent Molecular Adsorption on Oxide Surfaces
Density Functional Theory Calculations of Oxygen Vacancy Formation and Subsequent Molecular Adsorption on Oxide Surfaces
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DOI：
10.1021/acs.jpcc.8b11279
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发表时间：
2018-12-27
影响因子：
3.7
通讯作者：
Shimizu, Ken-ichi
中科院分区：
文献类型：
--
作者：
Hinuma, Yoyo;Toyao, Takashi;Shimizu, Ken-ichi
表面氧空位形成能（E-Ovac）是衡量金属氧化物催化活性的重要参数。因此，估计这些能量可以导致有希望的催化剂候选物的数据驱动设计。在本研究中，我们确定各种绝缘和半导体氧化物的E-Ovac。统计调查表明，带隙，体形成能，和电子亲和力的因素，强烈影响E-Ovac。在O脱附之后，电子进入缺陷态，并且这些状态可以在价带、中间带隙或导带中。随后的吸附O-2，NO，CO，CO2，和H-2分子上的O-缺乏表面也进行了研究。这些分子成为优先吸附在缺陷部位，和E-Ovac被确定为决定的吸附模式，以及一个描述符，表现出良好的相关性与吸附能的主导因素。
The surface oxygen vacancy formation energy (E-Ovac) is an important parameter in determining the catalytic activity of metal oxides. Estimating these energies can therefore lead to data-driven design of promising catalyst candidates. In the present study, we determine E-Ovac for various insulating and semiconducting oxides. Statistical investigations indicate that the band gap, bulk formation energy, and electron affinity are factors that strongly influence E-Ovac. Electrons enter defect states after O desorption, and these states can be in the valence band, mid-gap, or in the conduction band. Subsequent adsorption of O-2, NO, CO,CO2, and H-2 molecules on an O-deficient surface is also investigated. These molecules become preferentially adsorbed at the defect sites, and E-Ovac is identified as the dominant factor that determines the adsorption mode as well as a descriptor that shows good correlation with the adsorption energy.