理想、缺陷和金--促进的金红石TiO2（110）表面：来自PBE +U的结构、能量、动力学和热力学
Ideal, Defective, and Gold--Promoted Rutile TiO2(110) Surfaces: Structures, Energies, Dynamics, and Thermodynamics from PBE+U
摘要：
采用第第一性原理计算对金促进的TiO 2（110）表面进行了结构优化、电子结构分析、表面相图的从头算热力学计算和从头算分子动力学模拟。所有计算都依赖于广义梯度近似（PBE）中的密度泛函理论，并通过包含Hubbard校正PBE+U来解释现场库仑相互作用，其中U是根据线性响应理论计算的。通过研究TiO 2（110）表面与典型探针物种（H，H2O，CO）之间的相互作用，验证了该方法的有效性。松弛的结构和结合能进行比较，从文献和平原PBE结果的数据。研究的主要重点是金促进的二氧化钛表面的性质和它们与CO的相互作用。PBE+U和PBE优化结构的Au吸附原子吸附在化学计量和还原TiO 2表面的计算，以及它们的电子结构。对吸附物在金属/氧化物接触处引起的电荷重排也进行了分析和讨论。通过PBE+U从头算分子动力学模拟，证实了Au原子在化学计量比表面上的扩散是高度各向异性的。金属原子沿着桥接氧行的顶部或这些行之间的区域周围沿着[001]方向从一个桥接位置迁移到下一个桥接位置。近似从头算热力学预测，在富氧条件下，通过用Au原子取代Ti 5c原子获得的结构在宽范围的温度和压力下是热稳定的。
英文摘要：
Extensive first principles calculations are carried out to investigate gold-promoted TiO2(110) surfaces in terms of structure optimizations, electronic structure analyses, ab initio thermodynamics calculations of surface phase diagrams, and ab initio molecular dynamics simulations. All computations rely on density functional theory in the generalized gradient approximation (PBE) and account for on-site Coulomb interactions via inclusion of a Hubbard correction, PBE+U, where U is computed from linear response theory. This approach is validated by investigating the interaction between TiO2(110) surfaces and typical probe species (H, H2O, CO). Relaxed structures and binding energies are compared to both data from the literature and plain PBE results. The main focus of the study is on the properties of gold-promoted titania surfaces and their interactions with CO. Both PBE+U and PBE optimized structures of Au adatoms adsorbed on stoichiometric and reduced TiO2 surfaces are computed, along with their electronic structure. The charge rearrangement induced by the adsorbates at the metal/oxide contact are also analyzed and discussed. By performing PBE+U ab initio molecular dynamics simulations, it is demonstrated that the diffusion of Au adatoms on the stoichiometric surface is highly anisotropic. The metal atoms migrate either along the top of the bridging oxygen rows, or around the area between these rows, from one bridging position to the next along the [001] direction. Approximate ab initio thermodynamics predicts that under O-rich conditions, structures obtained by substituting a Ti5c atom with an Au atom are thermodynamically stable over a wide range of temperatures and pressures.
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