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Acta Physico-Chimica Sinica  2011, Vol. 27 Issue (05): 1068-1074    DOI: 10.3866/PKU.WHXB20110438
THEORETICAL AND COMPUTATIONAL CHEMISTRY     
Density Functional Theory Study of Atomic and Molecular Oxygen Adsorption on Au Clusters
GUO Xiao-Wei, TENG Bo-Tao, YUAN Jin-Huan, ZHAO Yun, ZHAO Yue, LIU Sha
Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang Province, P. R. China
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Abstract  

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).



Key wordsOxygen atom and molecule      Adsorption      Reaction      Au cluster      Density functional theory     
Received: 04 November 2010      Published: 18 March 2011
MSC2000:  O641  
  O647  
Fund:  

The project was supported by the National Natural Science Foundation of China (20903081) and Natural Science Foundation of Zhejiang Province,China (Y407163).

Corresponding Authors: TENG Bo-Tao     E-mail: tbt@zjnu.cn
Cite this article:

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. Acta Physico-Chimica Sinica, 2011, 27(05): 1068-1074.

URL:

http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/10.3866/PKU.WHXB20110438     OR     http://www.whxb.pku.edu.cn/Jwk_wk/wlhx/Y2011/V27/I05/1068

(1) Haruta, M.; Yamada, N.; Kobayashi, T.; Iijima, S. J. Catal. 1989, 115, 301.
(2) Haruta, M. Catal. Today 1997, 36, 153.
(3) Debeila, M. A.; Coville, N. J.; Scurrell, M. S.; Hearne, G. R. Catal. Today 2002, 72, 11.
(4) Valden, M.; Lai, X.; Goodman, D. W. Science 1998, 281, 1647.
(5) Kozlov, A. I.; Kozlova, A. P.; Asakura, K.; Matsui, Y.; Kogure, T.; Shido, T.; Iwasawa, Y. J. Catal. 2000, 196, 56.
(6) Qian, K.; lv, S. S.; Xiao, X. Y.; Sun, H. X.; Lu, J. Q.; Luo, M. F.; Huang, W. X. J. Mol. Catal. A 2009, 306, 40.
(7) Qian, K.; Fang, J.; Huang, W. X.; He, B.; Jiang, Z. Q.; Ma, Y. S.; Wei, S. Q. J. Mol. Catal. A 2010, 320, 97.
(8) Okumura, M.; Kitagawa, Y.; Haruta, M.; Yamaguchi, K. Appl. Catal. A 2005, 291, 37.
(9) Zhang, C. J.; Michaelides, A.; King, D. A.; Jenkins, S. J. J. Am. Chem. Soc. 2010, 132, 2175.
(10) Okazawa, T.; Fujiwara, M.; Nishimura, T.; Akita, T.; Kohyama, M.; Kido, Y. Surf. Sci. 2006, 600, 1331.
(11) Cheng, D. J.; Lan, J. H.; Wang, W. C.; Cao D. P. Surf. Sci. 2009, 603, 881.
(12) Saliba, N.; Parker, D. H.; Koel, B. E. Surf. Sci. 1998, 410, 270.
(13) Min, B. K.; Wallace, D. W.; Goodman, D. W. Surf. Sci. 2006, 600, 7.
(14) Cox, D. M.; Brockman, R.; Creegan, K.; Kaldor, A.; Z. Phys. D 1991, 19, 353.
(15) Huang, W.; Zhai, H. J.; Wang, L. S. J. Am. Chem. Soc. 2010, 132, 4344.
(16) Mao, H. P.; Wang, H. Y.; Ni, Y.; Xu, G. L.; Ma, M. Z.; Zhu, Z. H.; Tang, Y. J. Acta. Phys. Sin. 2004, 53, 1766.
[毛华平, 王红艳, 倪 羽, 徐国亮, 马美仲, 朱正和, 唐永建. 物理学报, 2004, 53, 1766.]
(17) Zeng, Z. H.; Deng, H. Q.; Li, W. X.; Hu, W. Y. Acta Phys. Sin. 2006, 55, 3157.
[曾振华, 邓辉球, 李微雪, 胡望宇. 物理学报, 2006, 55, 3157.]
(18) Lopez, N.; Janssens, T. V. W.; Clausen, B. S.; Xu, Y.; Mavrikakis, M.; Bligaard, T.; Nørskov, J. K. J. Catal. 2004, 223, 232.
(19) Franceschetti, A.; Pennycook, S. J.; Pantelides, S. T.; Chem. Phys. Lett. 2003, 374, 471.
(20) Mills. G.; Gordon, M. S.; Metiu, H. Chem. Phys. Lett. 2002, 359, 493.
(21) Fernández, E. M.; Ordejón, P.; Balbós, L. C. Chem. Phys. Lett. 2005, 408, 252.
(22) Wang, S.; Wang, W. N.; Lu, J.; Chen, G. H.; Fan, K. N. Acta Chim. Sin. 2007, 65, 2085.
[王 顺, 王文宁, 陆 靖, 陈冠华, 范康年. 化学学报, 2007, 65, 2085.]
(23) Li, J.; Li, X.; Zhai, H. J.; Wang, L. S. Science 2003, 299, 864.
(24) Zhao, L. X.; Lei, Y. M.; Zhang, M.; Feng, X. J.; Luo,Y. H. Physica B 2009, 404, 1705
(25) Fa, W.; Luo, C. F.; Dong, J. M. Phys. Rev. B 2005, 72, 205428.
(26) Delley, B. J. Chem. Phys. 2000, 113, 7756.
(27) Delley, B. J. Chem. Phys. 1990, 92, 508.
(28) Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865.
(29) Xu, Y. L.; Yan, X. L.; Jia, Y. M.; Luo, J. H.; Cao, Q. X.; et al. Introduction to Material Physics; University of Electronic Science and Technology of China: Chengdu, 1994; pp 20-62.
[徐毓龙, 闫西林, 贾宇明, 罗佳慧, 曹全喜. 材料物理导论. 成都: 电子科技大学, 1994: 20-62.]

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