Citation: QIAN Huifeng, BARRY Ellen, ZHU Yan, JIN Rongchao. Doping 25-Atom and 38-Atom ld Nanoclusters with Palladium[J]. Acta Physico-Chimica Sinica, ;2011, 27(03): 513-519. doi: 10.3866/PKU.WHXB20110304 shu

Doping 25-Atom and 38-Atom ld Nanoclusters with Palladium

1.
1. Department of Chemistry, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, USA;
2. Department of Chemistry, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, USA

Received Date: 4 November 2010
Available Online: 21 January 2011
Fund Project: The project was supported by Carnegie Mellon University (CMU) (CMU) the Air Force Office of Scientific Research (AFOSR) (AFOSR)the National Institute for ccupational Safety and Health (NIOSH) (NIOSH) USA. BARRY Ellen was supported by the National Science Foundation-Research Experiences for Undergraduates, USA (NSF grant DMR #1005076). (NSF grant DMR #1005076)

In this work, we describe two synthetic procedures for preparing palladium doped 25-atom nanoclusters (referred to as Pd₁Au₂₄(SR)₁₈, where ―SR represents thiolate, R=C₂H₄Ph). Pure Pd₁Au₂₄(SC₂H₄Ph)₁₈ nanoclusters are isolated by solvent extraction and size exclusion chromatography. Mass spectrometry and optical spectroscopy analyses demonstrate that the Pd₁Au₂₄(SC₂H₄Ph)₁₈ nanocluster adopts the same core-shell structure as that of the homo ld Au₂₅(SC₂H₄Ph)₁₈ nanocluster, that is, a Pd- or Au-centered icosahedron surrounded by six Au₂(SR)₃ “staple”-like motifs. Similar doping behavior has also been observed in 38-atom M₃₈(SR)₂₄ (M: metal) nanoclusters, indicating the unique behavior of Pd dopant being preferentially located in the icosahedral center. The catalytic activity of Pd₁Au₂₄(SC₂H₄Ph)₁₈ has also been evaluated for the selective hydrogenation of α,β-unsaturated ketone (e.g., benzalacetone) to α,β- unsaturated alcohol, and a 42% conversion of benzalacetone is attained.
- ld,
- Nanocluster,
- Doping,
- Palladium
1. [1]
  
  (1) Jin, R. Nanoscale 2010, 2, 343.
2. [2]
  (2) Schaaff, T. G.; Knight, G.; Shafigullin, M. N.; Borkman, R. F.; Whetten, R. L. J. Phys. Chem. B 1998, 102, 10643.
3. [3]
  (3) Parker, J. F.; Fields-Zinna, C. A.; Murray, R. W. Acc. Chem. Res. 2010, 43, 1289.
4. [4]
  (4) Tsunoyama, H.; Tsukuda, T. J. Am. Chem. Soc. 2009, 131, 18216.
5. [5]
  (5) Zhu, Y.; Wu, Z.; Gayathri, G. C.; Qian, H.; Gil, R. R.; Jin, R. J. Catal. 2010, 271, 155.
6. [6]
  (6) Li, J.; Wang, S. G. J. Mol. Model. 2010, 16, 505.
7. [7]
  (7) Shichibu, Y.; Negishi, Y.; Watanabe, T.; Chaki, N. K.; Kawaguchi, H.; Tsukuda, T. J. Phys. Chem. C 2007, 111, 7845.
8. [8]
  (8) Jiang, D. E. Acta Phys. -Chim. Sin. 2010, 26, 999.
9. [9]
  (9) Zhou, R. J.; Shi, M. M.; Chen, X. Q.; Wang, M.; Chen, H. Z. Chem. -Eur. J. 2009, 15, 4944.
10. [10]
  (10) Zhu, M.; Aikens, C. M.; Hollander, F. J.; Schatz, G. C.; Jin, R. J. Am. Chem. Soc. 2008, 130, 5883.
11. [11]
  (11) Zhu, M.; Eckenhoff, W. T.; Pintauer, T.; Jin, R. J. Phys. Chem. C 2008, 112, 14221.
12. [12]
  (12) Qian, H.; Eckenhoff, W. T.; Zhu, Y.; Pintauer, T.; Jin, R. J. Am. Chem. Soc. 2010, 132, 8280.
13. [13]
  (13) Schaaff, T. G.; Whetten, R. L. J. Phys. Chem. B 2000, 104, 2630.
14. [14]
  (14) Negishi, Y.; Nobusada, K.; Tsukuda, T. J. Am. Chem. Soc. 2005, 127, 5261.
15. [15]
  (15) Wu, Z.; Jin, R. Nano Lett. 2010, 10, 2568.
16. [16]
  (16) Rao, T. U. B.; Pradeep, T. Angew. Chem. Int. Edit. 2010, 49, 3925.
17. [17]
  (17) Zhu, M.; Aikens, C. M.; Hendrich, M. P.; Gupta, R.; Qian, H.; Schatz, G. C.; Jin, R. J. Am. Chem. Soc. 2009, 131, 2490.
18. [18]
  (18) Negishi, Y.; Tsunoyama, H.; Suzuki, M.; Kawamura, N.; Matsushita, M. M.; Maruyama, K.; Sugawara, K.; Yokoyama, T.; Tsukuda. T. J. Am. Chem. Soc. 2006, 128, 12034.
19. [19]
  (19) Iwasa, T.; Nobusada, K. Chem. Phys. Lett. 2007, 441, 268.
20. [20]
  (20) Tsunoyama, H.; Ichikuni, N.; Sakurai, H.; Tsukuda, T. J. Am. Chem. Soc. 2009, 131, 7086.
21. [21]
  (21) Zhu, Y.; Qian, H.; Zhu, M.; Jin, R. Adv. Mater. 2010, 22, 1915.
22. [22]
  (22) Zhu, Y.; Qian, H.; Jin, R. Chem. -Eur. J. 2010, 16, 11455.
23. [23]
  (23) Zhu, Y.; Qian, H.; Drake, B. A.; Jin, R. Angew. Chem. Int. Edit. 2010, 49, 1295.
24. [24]
  (24) Jin, R.; Qian, H.; Wu, Z.; Zhu, Y.; Zhu, M.; Mohanty, A.; Garg, N. J. Phys. Chem. Lett. 2010, 1, 2903.
25. [25]
  (25) Zhu, M.; Lanni, E.; Garg, N.; Bier, M. E.; Jin, R. J. Am. Chem. Soc. 2008, 130, 1138.
26. [26]
  (26) Wu, Z.; Suhan, J.; Jin, R. J. Mater. Chem. 2009, 19, 622.
27. [27]
  (27) Parker, J. F.; Weaver, J. E. F.; McCallum, F.; Fields-Zinna, C. A.; Murray, R. W. Langmuir 2010, 26, 13650.
28. [28]
  (28) Negishi, Y.; Kurashige, W.; Niihori, Y.; Iwasa, T.; Nobusada, K. Phys. Chem. Chem. Phys. 2010, 12, 6219.
29. [29]
  (29) Jiang, D.; Dai, S. Inorg. Chem. 2009, 48, 2720.
30. [30]
  (30) Kacprzak, K. A.; Lehtovaara, L.; Akola, J.; Lopez-Acevedoa, O.; Hakkinen, H. Phys. Chem. Chem. Phys. 2009, 11, 7123.
31. [31]
  (31) Walter, M.; Moseler, M. J. Phys. Chem. C 2009, 113, 15834.
32. [32]
  (32) Jiang, D. E; Whetten, R. L. Phys. Rev. B 2009, 80, 115402.
33. [33]
  (33) Akola, J.; Kacprzak, K. A.; Lopez-Acevedo, O.; Walter, M.; Gronbeck, H.; Hakkinen, H. J. Phys. Chem. C 2010, 114, 15986.
34. [34]
  (34) Reveles, J. U.; Clayborne, P. A.; Reber, A. C.; Khanna, S. N.; Pradhan, K.; Sen, P.; Pederson, M. R. Nat. Chem. 2009, 1, 310.
35. [35]
  (35) Wyrwas, R. B.; Alvarez, M. M.; Khoury, J. T.; Price, R. C.; Schaaff, T. G. Whetten, R. L. Eur. Phys. J. D 2007, 43, 91.
36. [36]
  (36) Schaaff, T. G.; Shafigullin, M. N.; Khoury, J. T.; Vezmar, I.; Whetten, R. L.; Cullen, W. G.; First, P. N.; Gutierrez-Wing, C.; Ascensio, J.; Jose-Yacaman, M. J. J. Phys. Chem. B 1997, 101, 7885.
37. [37]
  (37) Chaki, N. K.; Negishi, Y.; Tsunoyama, H.; Shichibu, Y.; Tsukuda, T. J. Am. Chem. Soc. 2008, 130, 8608.
38. [38]
  (38) Qian, H.; Zhu, M.; Andersen, U. N.; Jin, R. J. Phys. Chem. A 2009, 113, 4281.
39. [39]
  (39) Qian, H.; Zhu, Y.; Jin, R. J. Am. Chem. Soc. 2010, 132, 4583.
40. [40]
  (40) Fields-Zinna, C. A.; Crowe, M. C.; Dass, A.; Weaver, J. E. F.; Murray, R. W. Langmuir 2009, 25, 7704.
41. [41]
  (41) Qian, H.; Jin, R. Nano Lett. 2009, 9, 4083.
42. [42]
  (42) Dharmaratne, A. C.; Krick, T.; Dass, A. J. Am. Chem. Soc. 2009, 131, 13604.
43. [43]
  (43) Zhu, M.; Qian, H.; Jin, R. J. Phys. Chem. Lett. 2010, 1, 1003.
44. [44]
  (44) Wu, Z.; Lanni, E.; Chen, W.; Bier, M. E.; Ly, D.; Jin, R. J. Am. Chem. Soc. 2009, 131, 16672.
45. [45]
  (45) Dass, A.; Stevenson, A.; Dubay, G. R.; Tracy, J. B.; Murray, R. W. J. Am. Chem. Soc. 2008, 130, 5940.
46. [46]
  (46) Xiang, H. J.; Wei, S. H.; ng, X. G. J. Am. Chem. Soc. 2010, 132, 7355.
47. [47]
  (47) MacDonald, M. A.; Zhang, P.; Qian, H.; Jin, R. J. Phys. Chem. Lett. 2010, 1, 1821.
48. [48]
  (48) Angel, L. A.; Majors, L. T.; Dharmaratne, A. C.; Dass, A. ACS Nano 2010, 4, 4691.
49. [49]
  (49) Wu, Z.; Gayathri, C.; Gil, R.; Jin, R. J. Am. Chem. Soc. 2009, 131, 6535.
50. [50]
  (50) Ko , A.; Sakai, N.; Tatsuma, T. Electrochem. Commun. 2010, 12, 996.
51. [51]
  (51) Zheng, N.; Johnson, J. P.; Williams, C. C.; Wang, G. Nanotechnology 2010, 21, 295708.
52. [52]
  (52) Wang, Z.; Cai, W.; Sui, J. ChemPhysChem 2009, 10, 2012.
53. [53]
  (53) Jiang, D. E.; Walter, M.; Dai, S. Chem. -Eur. J. 2010, 16, 4999.
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