Acta Phys. -Chim. Sin. ›› 2011, Vol. 27 ›› Issue (04): 851-857.doi: 10.3866/PKU.WHXB20110405

• THEORETICAL AND COMPUTATIONAL CHEMISTRY • Previous Articles     Next Articles

Adhesion of Small Cux (x=1-4) Clusters on a CeO2(111) Surface

YANG Zong-Xian1,2, XIE Luo-Gang1   

  1. 1. College of Physics and Information Engineering, Henan Normal University, Xinxiang 453007, Henan Province, P. R. China;
    2. Henan Key Laboratory of Photovoltaic Materials, Xinxiang 453007, Henan Province, P. R. China
  • Received:2010-12-20 Revised:2011-01-14 Published:2011-03-29
  • Contact: YANG Zong-Xian E-mail:yzx@henannu.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (10674042) and Innovation Scientists and Technicians Troop Construction Projects of Henan Province, China (104200510014).

Abstract:

We investigated the adhesion behavior of Cu clusters (Cux, x=1-4) on a CeO2(111) surface using first-principles density functional theory (DFT). We found that small Cux clusters (x=2, 3) tended to adhere as two dimensional (2D) planar structures on the CeO2(111) surface. For the Cu4 cluster, a three dimensional (3D) tetrahedral structure is preferred and the 3D Cu4 particle is positively charged because of charge transfer from Cu 3d to Ce 4f. The transition from a 2D planar structure to 3D particles occurs with a transition barrier of 1.05 eV and the favorable route consists of one Cu atom hopping directly from the interface site to the hollow site above the Cu triangle. Because the Cu-O interactions are comparable with the Cu-Cu intra-cluster interactions, their competition determines the morphologies of the eventual Cu clusters on CeO2. The 3D positively charged Cu4 particle obtained on CeO2 is expected to result in distinct catalytic performance compared to the unsupported Cu4 cluster for water dissociation, and thus the water gas shift reactions.

Key words: Density functional theory, Cu cluster, Adhesion, Cux/CeO2(111)

MSC2000: 

  • O641