Citation: HU Jian-Ping, WANG Jun, TANG Dian-Yong, FU Qin-Chao, ZHANG Yuan-Qin. Reaction Mechanisms of CO Oxidation Catalyzed by Binary Copper Group Cluster Anions[J]. Acta Physico-Chimica Sinica, ;2011, 27(02): 329-336. doi: 10.3866/PKU.WHXB20110226 shu

Reaction Mechanisms of CO Oxidation Catalyzed by Binary Copper Group Cluster Anions

  • Received Date: 25 August 2010
    Available Online: 5 January 2011

    Fund Project: 教育部科学技术研究重点项目(210189) (210189) 四川省自然科学基金(2008JY0119) (2008JY0119)四川省教育厅(07ZA158)资助 (07ZA158)

  • The detailed mechanisms of CO oxidation catalyzed by AuAg-, AuCu-, and AgCu- were investigated using density functional theory at the B3LYP level. The computational results indicate that the adsorption site of CO onto the mixed clusters decreases as follows: Cu>Au>Ag. Copper is the preferred adsorption site for O2 on the binary clusters. The adsorption of O2 onto ld was found to be the weakest. Three reaction pathways exist for CO oxidation catalyzed by AuAg-, AuCu-, and AgCu-. The most feasible pathway for CO oxidation catalyzed by AuAg- is CO insertion into the Ag―O bond of AuA 2- to produce the [Au―AgC(O―O)O]- intermediate, which then decomposes into CO2 and AuA -, or another CO molecule attacks [Au―AgC(O―O)O]- to form two CO2 molecules and AuAg- anion. A feasible pathway for CO oxidation catalyzed by AuCu- or AgCu- is initiated by the co-absorption of CO and O2 onto the clusters followed by the formation of a four-membered ring intermediate to produce the corresponding products. The cooperation effect of the second CO is very weak. The catalytic activities of AuAg- and AuCu- toward CO oxidation are stronger than that of Au2- . Doping the Au clusters with Ag and Cu increases the catalytic activity. These results are in agreement with the previous experimental results.

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    1. [1]

      1 Min, B. K.; Friend, C. M. Chem. Rev. 2007, 107, 2709, and references therein.

    2. [2]

      2 Zhang, X.; Xu, B. Q. Acta Chim. Sin. 2005, 63, 86.

    3. [3]

      [张 鑫, 徐柏庆. 化学学报, 2005, 63, 86.]

    4. [4]

      3 Shao, J. J.; Zhang, P.; Song, W.; Huang, X. M.; Xu, Y. D.; Shen, W. J. Acta Chim. Sin. 2007, 65, 2007.

    5. [5]

      [邵建军, 张 平, 宋 巍, 黄秀敏, 徐奕德, 申文杰. 化学学报, 2007, 65, 2007.]

    6. [6]

      4 Chen, M.; odman, D. W. Acc. Chem. Res. 2006, 39, 739.

    7. [7]

      5 Bowker, M. Chem. Soc. Rev. 2008, 37, 2204.

    8. [8]

      6 Campbell, C. T. Science 2004, 306, 234.

    9. [9]

      7 Reveles, J. U.; Johnson,G. E.; Khanna, S. N.; Castleman, A. W., Jr. J. Phys. Chem. C 2010, 114, 5438.

    10. [10]

      8 Xue, W.; Wang, Z. C.; He, S. G.; Xie, Y.; Bernstein, E. R. J. Am. Chem. Soc. 2008, 130, 15879.

    11. [11]

      9 Wang, A. Q.; Liu, J. H.; Lin, S. D.; Lin, T. S.; Mou, C. Y. J. Catal. 2005, 233, 186.

    12. [12]

      10 Wang, A. Q.; Chang, C. M.; Mou, C. Y. J. Phys. Chem. B 2005, 109, 18860.

    13. [13]

      11 Liu, X.; Wang, A. Q.; Wang, X.; Mou, C. Y.; Zhang, T. Chem. Commun. 2008, No. 27, 3187.

    14. [14]

      12 Yen, C. W.; Lin, M. L.; Wang, A.; Chen, S. A.; Chen, J. M.; Mou, C. Y. J. Phys. Chem. C 2009, 113, 17831.

    15. [15]

      13 Wang, A. Q.; Hsieh, Y. P.; Chen, Y. F.; Mou, C. Y. J. Catal. 2006, 237, 197.

    16. [16]

      14 Liu, J. H.; Wang, A. Q.; Chi, Y. S.; Lin, H. P.; Mou, C. Y. J. Phys. Chem. B 2005, 109, 40.

    17. [17]

      15 Liu, X.; Wang, A. Q.; Yang, X. F.; Zhang, T.; Mou, C. Y.; Su, D. S.; Li, J. J. Chem. Mater. 2009, 21, 410.

    18. [18]

      16 Wittstock, A.; Neumann, B.; Schaefer, A.; Dumbuya, K.; Kübel, C.; Biener, M. M.; Zielasek, V.; Steinrück, H. P.; ttfried, J. M.; Biener, J.; Hamza, A.; B?umer, M. J. Phys. Chem. C 2009, 113, 5593.

    19. [19]

      17 Bernhardt, T. M.; Socaciu-Siebert, L. D.; Hagen, J.; Wöste, L. Appl. Catal. A-Gen. 2005, 291, 170.

    20. [20]

      18 Mitri?, R.; Burda, J.; Bona?i?-Koutecký, V.; Fantucci, P. Euro. Phys. J. D 2003, 24, 41.

    21. [21]

      19 Chang, C. M.; Cheng, C.; Wei, C. M. J. Chem. Phys. 2008, 128, 124710.

    22. [22]

      20 Gao, Y.; Shao, N.; Pei, Y.; Zeng, X. C. Nano Lett. 2010, 10, 1055.

    23. [23]

      21 Kimble, M. L.; Moore, N. A.; Johnson, G. E.; Castleman, A. W. J. Chem. Phys. 2006, 125, 204311.

    24. [24]

      22 Tang, D. Y.; Zhang, Y. Q.; Hu, C. W. Acta Chim. Sin. 2008, 66, 1501.

    25. [25]

      [唐典勇, 张元勤, 胡常伟. 化学学报, 2008, 66, 1501.]

    26. [26]

      23 Tang, D. Y.; Hu, J. P., Zhang, Y. Q., Hu, C. W. Acta Chim. Sin. 2009, 67, 1859.

    27. [27]

      [唐典勇, 胡建平, 张元勤, 胡常伟. 化学学报, 2009, 67, 1859.]

    28. [28]

      24 Dholabhai, P. P.; Wu, X.; Ray, A. K. J. Mol. Struct.-Theochem 2005, 723, 139.

    29. [29]

      25 Tang, D. Y.; Hu, J. P.; Zhang, Y. Q.; Hu, C. W. Acta Chim. Sin. 2010, 68, 1379.

    30. [30]

      [唐典勇, 胡建平, 张元勤, 胡常伟. 化学学报, 2010, 68, 1379.]

    31. [31]

      26 Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al. Gaussian 03, Revision E.01; Gaussian Inc.: Pittsburgh, PA, 2004.

    32. [32]

      27 Couty, M.; Hall, M. B. J. Comput. Chem. 1996, 17, 1359.

    33. [33]

      28 Ehlers, A. W.; Dapprich, B. S.; bbi, A.; Hollwarth, A.; Jonas, V.; Kohler, K. F.; Stegmann, R.; Veldkamp, A.; Frenking, G. Chem. Phys. Lett. 1993, 208, 111.

    34. [34]

      29 Ojifinni, R. A.; ng, J.; Froemming, N. S.; Flaherty, D. W.; Pan, M.; Henkelman, G.; Mullins, C. B. J. Am. Chem. Soc. 2008, 130, 11250.

    35. [35]

      30 Wang, F.; Zhang, D.; Xu, X.; Ding, Y. J. Phys. Chem. C 2009, 113, 18032.


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