Abstract
Structure of gold nanoparticles formed by physical vapor deposition onto thin ceria films was studied by scanning tunneling microscopy (STM). Gold preferentially nucleates on point defects present on the terraces of the well-ordered, fully oxidized films to a low density. The nucleation expands to the terrace step edges, providing a large variety of low-coordinated sites. Only at high coverage, the Au particles grow homogeneously on the oxygen-terminated CeO2(111) terraces. The morphology of Au particles was further examined by STM in situ and ex situ at elevated (up to 20 mbar) pressures of O2, CO, and CO + O2 at 300 K. The particles are found to be stable in O2 ambient up to 10 mbar, meanwhile gold sintering emerges at CO pressures above ∼1 mbar. Sintering of the Au particles, which mainly proceeds along the step edges of the CeO2(111) support, is observed in CO + O2 (1:1) mixture at much lower pressure (∼10−3 mbar), thus indicating that the structural stability of the Au/ceria catalysts is intimately connected with its reactivity in the CO oxidation reaction.
Similar content being viewed by others
References
G. Bond, C. Lois and D. Thompson, Catalysis by Gold (World Scientific, 2006)
Fu Q., Weber A., Flytzani-Stephanopoulos M. (2001) Catal. Lett. 77:87
Andreeva D., Idakiev V., Tabakova T., Ilieva L., Falares P., Bourlinos A., Travlos A. (2002) Catal. Today 72:51
Sakurai H., Akita T., Tsubota S., Kiuchi M., Haruta M. (2005) Appl. Catal. A 291:179
Carrettin S., Concepción P., Corma A., López Nieto J.M., Puntes V.F. (2004) Angew. Chem. Int. Ed. 43:2538
Guzman J., Carrettin S., Corma A. (2005) J. Am. Chem. Soc. 127:3286
Lai S.-Y., Qiu Y., Wang S. (2006) J. Catal. 237:303
Centeno M.A., Portales C., Carrizosa I., Odrizola J.A. (2005) Catal. Lett. 102:289
Pillai U.R., Deevi S. (2006) Appl. Catal. A 299:266
Fu Q., Saltsburg H., Flytzani-Stephanopoulos M. (2003) Science 301:935
Campbell C.T. (1997) Surf. Sci. Rep. 27:1
Henry C. (1998) Surf. Sci. Rep. 31:231
Goodman D.W. (1995) Chem. Rev. 95:523
Freund H.-J. (2002) Surf. Sci. 500:271
Meyer R., Lemire C., Shaikhutdinov S., Freund H.-J. (2004) Gold Bull. 37:72
J. Guzman and B.C. Gates, J. Am. Chem. Soc. 126 (2004) 2672; J. Phys. Chem. B 106 (2002) 7659
Henao J.D., Caputo T., Yang J.H., Kung M.C., Kung H.H. (2006) J. Phys. Chem. B 110:8689
Wang X., Rodriguez J.A., Hanson J.C., Perez M., Evans J. (2005) J. Chem. Phys. 1213:21101
Overbury S.H., Schwartz V., Mullins D., Yan W., Dai S. (2006) J. Catal. 241:56
Weiher N., et al. (2006) J. Catal. 240:100
Hutchings G., et al. (2006) J. Catal. 242:71
Valden M., Lai X., Goodman D.W. (1998) Science 281:1647
Kolmakov A., Goodman D.W. (2000) Catal. Lett. 70:93
Starr D.E., Shaikhutdinov S.K., Freund H.-J. (2005) Top. Catal. 36:33
Mullins D.R., Radulovic P.V., Overbury S.H. (1999) Surf. Sci. 429:186
J.-L. Lu, H.-J.Gao, S. Shaikhutdinov and H.-J. Freund, Surf. Sci. (corrected proof available online)
Nörenberg H., Briggs G.A.D. (1999) Surf. Sci. 424:L352
Eck S., Castellarin-Cudia C., Surnev S., Ramsey M.G., Netzer F.P. (2002) Surf. Sci. 520:173
Castellarin-Cudia C., Surnev S., Schneider G., Podlucky R., Ramsey M.G., Netzer F.P. (2004) Surf. Sci. 554:L120
Esch F., Fabris S., Zhou L., Montini T., Africh C., Fornasiero P., Comelli G., Rosei R. (2005) Science 309:752
T. Akita, M. Okumura, K. Tanaka, M. Kohyama, S. Tsubota and M. Haruta, J. Electron Microsc. 54 (2005) 81; J. Mat. Sci. 40 (2005) 3101
Sayle T.X.T., Parker S.C., Catlow C.R.A. (1994) Surf. Sci. 316:329
Acknowledgments
The authors gratefully acknowledge financial support from the Fonds der Chemischen Industrie and Deutsche Forschungsgemeinschaft (DFG). J.L. thanks International Max-Planck Research School “Complex Surfaces in Materials Science” for the fellowship.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Lu, JL., Gao, HJ., Shaikhutdinov, S. et al. Gold supported on well-ordered ceria films: nucleation, growth and morphology in CO oxidation reaction. Catal Lett 114, 8–16 (2007). https://doi.org/10.1007/s10562-007-9039-3
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10562-007-9039-3