Cux (x=1-4)团簇在CeO2(111)表面的吸附

doi:10.3866/PKU.WHXB20110405

Abstract

Abstract:

We investigated the adhesion behavior of Cu clusters (Cu_x, x=1-4) on a CeO₂(111) surface using first-principles density functional theory (DFT). We found that small Cu_x 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, Cu_x/CeO₂(111)

MSC2000:

O641

YANG Zong-Xian, XIE Luo-Gang. Adhesion of Small Cu_x (x=1-4) Clusters on a CeO₂(111) Surface[J].Acta Phys. -Chim. Sin., 2011, 27(04): 851-857.

References

(1) Rodríguez, J.; Evans, J.; Graciani, J.; Park, J.; Liu, P.; Hrbek, J.; Sanz, J. J. Phys. Chem. C 2009, 113, 7364.
(2) Rodríguez, J.; Liu, P.; Wang, X.; Wen, W.; Hanson, J.; Hrbek, J.; Pérez, M.; Evans, J. Catal. Today 2009, 143, 45.
(3) Tang, Q.; Liu, Z. J. Phys. Chem. C 2010, 114, 8423.
(4) Feldheim, D. Science 2007, 316, 699.
(5) Wang, X.; Rodriguez, J.; Hanson, J.; Gamarra, D.; Martínez- Arias, A.; Fernández-García, M. J. Phys. Chem. B 2006, 110, 428.
(6) Rodríguez, J.; Liu, P.; Hrbek, J.; Evans, J.; Pérez, M. Angew. Chem. Int. Edit. 2007, 46, 1329.
(7) Park, J.; Graciani, J.; Evans, J.; Stacchiola, D.; Ma, S.; Liu, P.; Nambu, A.; Sanz, J.; Hrbek, J.; Rodriguez, J. Proc. Natl. Acad. Sci. U. S. A. 2009, 106, 4975.
(8) Saito, M.; Murata, K. Catal. Surv. Asia. 2004, 8, 285.
(9) Kresse, G.; Furthmuller, J. Comp. Mater. Sci. 1996, 6, 15.
(10) Kresse, G.; Hafner, J. Phys. Rev. B 1993, 47, 558.
(11) Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865.
(12) Bl?chl, P. E.; Jepsen, O.; Andersen, O. K. Phys. Rev. B 1994, 49, 16223.
(13) Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.; Humphreys, C. J.; Sutton, A. P. Phys. Rev. B 1998, 57, 1505.
(14) Anisimov, V. I.; Zaanen, J.; Andersen, O. K. Phys. Rev. B 1991, 44, 943.
(15) Yang, Z.; Lu, Z.; Luo, G. Phys. Rev. B 2007, 76, 75421.
(16) Yang, Z.; Fu, Z.; Wei, Y.; Lu, Z. J. Phys. Chem. C 2008, 112, 15341.
(17) Nolan, M.; Grigoleit, S.; Sayle, D. C.; Parker, S. C.; Watson, G. W. Surf. Sci. 2005, 576, 217.
(18) Henkelman, G.; Uberuaga, B.; Jónsson, H. J. Chem. Phys. 2000, 113, 9901.
(19) Henkelman, G.; Arnaldsson, A.; Jónsson, H. Comp. Mater. Sci. 2006, 36, 354.
(20) Monkhorst, H. J.; Pack, J. D. Phys. Rev. B 1976, 13, 5188.
(21) Li, B.; Ezekoye, O.; Zhang, Q.; Chen, L.; Cui, P.; Graham, G.; Pan, X. Phys. Rev. B 2010, 82, 125422.
(22) Jug, K.; Zimmermann, B.; Calaminici, P.; Kster, A. J. Chem. Phys. 2002, 116, 4497.
(23) Spasov, V.; Lee, T.; Ervin, K. J. Chem. Phys. 2000, 112, 1713.
(24) Alfonso, D.; Jaffe, J.; Hess, A.; Gutowski, M. Phys. Rev. B 2003, 68, 155411.
(25) Musolino, V.; Selloni, A.; Car, R. Phys. Rev. Lett. 1999, 83, 3242.
(26) Musolino, V.; Dal Corso, A.; Selloni, A. Phys. Rev. Lett. 1999, 83, 2761.
(27) Yang, Z.; He, B.; Lu, Z.; Hermansson, K. J. Phys. Chem. C 2010, 114, 4486.
(28) Jung, K.; Bell, A. Catal. Lett. 2002, 80, 63.
(29) Chen, L.; Johnson, J. K. Phys. Rev. Lett. 2005, 94, 125701.

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

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

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