Citation: ZHAO Wei-Na, LIN Hua-Xiang, LI Yi, ZHANG Yong-Fan, HUANG Xin, CHEN Wen-Kai. Coverage-Dependent Adsorption of X Clusters (X=Pt-Au, Au-Au) on the Defect-Free (3×2) TiO₂(110) Surface[J]. Acta Physico-Chimica Sinica, ;2012, 28(08): 1861-1868. doi: 10.3866/PKU.WHXB201205214 shu

Coverage-Dependent Adsorption of X Clusters (X=Pt-Au, Au-Au) on the Defect-Free (3×2) TiO₂(110) Surface

1.
1. College of Chemistry and Chemical Engineering, Fuzhou University, Fuzhou 350116, P. R. China;
2. Fujian Provincial Key Laboratory of Photocatalysis-State Key Laboratory Breeding Base, Fuzhou University, Fuzhou 350002, Fujian, P. R. China

Received Date: 20 March 2012
Available Online: 21 May 2012
Fund Project: 国家自然科学基金(90922022) (90922022)华中科技大学煤燃烧国家重点实验室开放基金(FSKLCC1110)资助项目 (FSKLCC1110)

Based on spin-polarized density functional theory and generalized gradient approximation (DFT-GGA) calculations, the coverage-dependent adsorption of X bimetallic clusters (X=Pt-Au, Au-Au) on the (3 × 2) TiO₂(110) surface has been investigated utilizing periodic supercell models in the absence of oxygen vacancy sites. Only the ground-state structures corresponding to the given coverage patterns (θ= 1/6-1 ML) for X clusters are discussed in this work. The unambiguous results reveal that the adsorption energies increase with coverage up to 1/2 ML and then decrease except for when saturated coverage is reached. According to the interaction with X clusters, it is more feasible at all coverage levels to create a monolayer film of Pt-Au bimetallic clusters on the TiO₂(110) surface than it is to create a monolayer of Au- Au clusters, even though the adsorption energy of the Pt-Au/TiO₂ adsorption system is smaller in comparison with that of the Au-Au/TiO₂ system. Importantly, especially for the half and saturated coverages, there is a broadening of X peaks overlapping with the TiO₂ state ranging from -3.0 eV to the Fermi level, suggesting a strong interaction between the surface and bimetallic cluster. Also of particular interest is the adsorptive mechanism where the X-TiO₂ interaction is the main driving force at the initial stage of the adsorption process, whereas the X-X interaction controls the process as the coverage increases.
- Density functional theory,
- TiO₂ (110) surface,
- Bimetallic cluster
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Coverage-Dependent Adsorption of X Clusters (X=Pt-Au, Au-Au) on the Defect-Free (3×2) TiO2(110) Surface

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通讯作者: 陈斌, bchen63@163.com

Coverage-Dependent Adsorption of X Clusters (X=Pt-Au, Au-Au) on the Defect-Free (3×2) TiO₂(110) Surface