Citation: GUO Xiao-Wei, TENG Bo-Tao, YUAN Jin-Huan, ZHAO Yun, ZHAO Yue, LIU Sha. Density Functional Theory Study of Atomic and Molecular Oxygen Adsorption on Au Clusters[J]. Acta Physico-Chimica Sinica, ;2011, 27(05): 1068-1074. doi: 10.3866/PKU.WHXB20110438 shu

Density Functional Theory Study of Atomic and Molecular Oxygen Adsorption on Au Clusters

1.
Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang Province, P. R. China

Received Date: 4 November 2010
Available Online: 18 March 2011
Fund Project: 国家自然科学基金(20903081) (20903081)浙江省自然科学基金(Y407163)资助项目 (Y407163)

The adsorption behaviors of O and O₂ on charged and neutral Au₁₉ and Au₂₀ clusters were systematically investigated by density functional theory (DFT) with Dmol³ program. Our results indicate that the adsorption energies of O on the hollow sites of Au₁₉ are higher than those on Au₂₀; while those on the side-bridge sites of the Au₁₉ and Au₂₀ clusters are similar. For negatively charged clusters, the adsorption energies of O and O₂ are higher than those for neutral and positive clusters. The O―O bond lengths of the adsorbed O₂ on the Au₁₉ and Au₂₀ clusters with different charges show a similar trend to the adsorption energy, that is, the O―O bond lengths on Au₁₉^- are longer than those on the Au₁₉ and Au₁₉⁺ clusters. Population analysis shows that more electrons transfer to the adsorbed O and O₂ from the Au₁₉^- and Au-20 clusters, which indicates stronger interactions compared with the neutral or positive clusters. Charge density difference (CDD) analysis for O₂ on the Au₁₉ and Au₂₀ clusters suggests that electrons of the Au₁₉ and Au₂₀ clusters transfer to the π^* orbital of O₂, upon which the O―O bonds are activated. The dissociation reaction barrier of O₂ on Au₁₉^- is 1.33 eV, which is lower than those on Au₁₉ (1.86 eV) and Au₁₉⁺ (2.27 eV).
- Oxygen atom and molecule,
- Adsorption,
- Reaction,
- Au cluster,
- Density functional theory
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1.
沈阳化工大学材料科学与工程学院沈阳 110142