钯掺杂的25-原子和38-原子金纳米团簇

doi:10.3866/PKU.WHXB20110304

物理化学学报 >> 2011, Vol. 27 >> Issue (03): 513-519.doi: 10.3866/PKU.WHXB20110304

钯掺杂的25-原子和38-原子金纳米团簇

QIAN Huifeng¹, BARRY Ellen², ZHU Yan¹, JIN Rongchao¹

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

收稿日期:2010-11-04 修回日期:2011-01-10 发布日期:2011-03-03
通讯作者: JIN Rongchao E-mail:rongchao@andrew.cmu.edu
基金资助:
The project was supported by Carnegie Mellon University (CMU), the Air Force Office of Scientific Research (AFOSR) and the National Institute for ccupational Safety and Health (NIOSH), USA. BARRY Ellen was supported by the National Science Foundation-Research Experiences for Undergraduates, USA (NSF grant DMR #1005076).

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

QIAN Huifeng¹, BARRY Ellen², ZHU Yan¹, JIN Rongchao¹

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

Received:2010-11-04 Revised:2011-01-10 Published:2011-03-03
Contact: JIN Rongchao E-mail:rongchao@andrew.cmu.edu
Supported by:
The project was supported by Carnegie Mellon University (CMU), the Air Force Office of Scientific Research (AFOSR) and the National Institute for ccupational Safety and Health (NIOSH), USA. BARRY Ellen was supported by the National Science Foundation-Research Experiences for Undergraduates, USA (NSF grant DMR #1005076).

摘要/Abstract

摘要：

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 homogold 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.

关键词: Gold, Nanocluster, Doping, Palladium

Abstract:

Key words: Gold, Nanocluster, Doping, Palladium

QIAN Huifeng, BARRY Ellen, ZHU Yan, JIN Rongchao. 钯掺杂的25-原子和38-原子金纳米团簇[J]. 物理化学学报, 2011, 27(03): 513-519.

QIAN Huifeng, BARRY Ellen, ZHU Yan, JIN Rongchao. Doping 25-Atom and 38-Atom Gold Nanoclusters with Palladium[J]. Acta Phys. -Chim. Sin., 2011, 27(03): 513-519.

参考文献

(1) Jin, R. Nanoscale 2010, 2, 343.
(2) Schaaff, T. G.; Knight, G.; Shafigullin, M. N.; Borkman, R. F.; Whetten, R. L. J. Phys. Chem. B 1998, 102, 10643.
(3) Parker, J. F.; Fields-Zinna, C. A.; Murray, R. W. Acc. Chem. Res. 2010, 43, 1289.
(4) Tsunoyama, H.; Tsukuda, T. J. Am. Chem. Soc. 2009, 131, 18216.
(5) Zhu, Y.; Wu, Z.; Gayathri, G. C.; Qian, H.; Gil, R. R.; Jin, R. J. Catal. 2010, 271, 155.
(6) Li, J.; Wang, S. G. J. Mol. Model. 2010, 16, 505.
(7) Shichibu, Y.; Negishi, Y.; Watanabe, T.; Chaki, N. K.; Kawaguchi, H.; Tsukuda, T. J. Phys. Chem. C 2007, 111, 7845.
(8) Jiang, D. E. Acta Phys. -Chim. Sin. 2010, 26, 999.
(9) Zhou, R. J.; Shi, M. M.; Chen, X. Q.; Wang, M.; Chen, H. Z. Chem. -Eur. J. 2009, 15, 4944.
(10) Zhu, M.; Aikens, C. M.; Hollander, F. J.; Schatz, G. C.; Jin, R. J. Am. Chem. Soc. 2008, 130, 5883.
(11) Zhu, M.; Eckenhoff, W. T.; Pintauer, T.; Jin, R. J. Phys. Chem. C 2008, 112, 14221.
(12) Qian, H.; Eckenhoff, W. T.; Zhu, Y.; Pintauer, T.; Jin, R. J. Am. Chem. Soc. 2010, 132, 8280.
(13) Schaaff, T. G.; Whetten, R. L. J. Phys. Chem. B 2000, 104, 2630.
(14) Negishi, Y.; Nobusada, K.; Tsukuda, T. J. Am. Chem. Soc. 2005, 127, 5261.
(15) Wu, Z.; Jin, R. Nano Lett. 2010, 10, 2568.
(16) Rao, T. U. B.; Pradeep, T. Angew. Chem. Int. Edit. 2010, 49, 3925.
(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) 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) Iwasa, T.; Nobusada, K. Chem. Phys. Lett. 2007, 441, 268.
(20) Tsunoyama, H.; Ichikuni, N.; Sakurai, H.; Tsukuda, T. J. Am. Chem. Soc. 2009, 131, 7086.
(21) Zhu, Y.; Qian, H.; Zhu, M.; Jin, R. Adv. Mater. 2010, 22, 1915.
(22) Zhu, Y.; Qian, H.; Jin, R. Chem. -Eur. J. 2010, 16, 11455.
(23) Zhu, Y.; Qian, H.; Drake, B. A.; Jin, R. Angew. Chem. Int. Edit. 2010, 49, 1295.
(24) Jin, R.; Qian, H.; Wu, Z.; Zhu, Y.; Zhu, M.; Mohanty, A.; Garg, N. J. Phys. Chem. Lett. 2010, 1, 2903.
(25) Zhu, M.; Lanni, E.; Garg, N.; Bier, M. E.; Jin, R. J. Am. Chem. Soc. 2008, 130, 1138.
(26) Wu, Z.; Suhan, J.; Jin, R. J. Mater. Chem. 2009, 19, 622.
(27) Parker, J. F.; Weaver, J. E. F.; McCallum, F.; Fields-Zinna, C. A.; Murray, R. W. Langmuir 2010, 26, 13650.
(28) Negishi, Y.; Kurashige, W.; Niihori, Y.; Iwasa, T.; Nobusada, K. Phys. Chem. Chem. Phys. 2010, 12, 6219.
(29) Jiang, D.; Dai, S. Inorg. Chem. 2009, 48, 2720.
(30) Kacprzak, K. A.; Lehtovaara, L.; Akola, J.; Lopez-Acevedoa, O.; Hakkinen, H. Phys. Chem. Chem. Phys. 2009, 11, 7123.
(31) Walter, M.; Moseler, M. J. Phys. Chem. C 2009, 113, 15834.
(32) Jiang, D. E; Whetten, R. L. Phys. Rev. B 2009, 80, 115402.
(33) Akola, J.; Kacprzak, K. A.; Lopez-Acevedo, O.; Walter, M.; Gronbeck, H.; Hakkinen, H. J. Phys. Chem. C 2010, 114, 15986.
(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) 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) 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) Chaki, N. K.; Negishi, Y.; Tsunoyama, H.; Shichibu, Y.; Tsukuda, T. J. Am. Chem. Soc. 2008, 130, 8608.
(38) Qian, H.; Zhu, M.; Andersen, U. N.; Jin, R. J. Phys. Chem. A 2009, 113, 4281.
(39) Qian, H.; Zhu, Y.; Jin, R. J. Am. Chem. Soc. 2010, 132, 4583.
(40) Fields-Zinna, C. A.; Crowe, M. C.; Dass, A.; Weaver, J. E. F.; Murray, R. W. Langmuir 2009, 25, 7704.
(41) Qian, H.; Jin, R. Nano Lett. 2009, 9, 4083.
(42) Dharmaratne, A. C.; Krick, T.; Dass, A. J. Am. Chem. Soc. 2009, 131, 13604.
(43) Zhu, M.; Qian, H.; Jin, R. J. Phys. Chem. Lett. 2010, 1, 1003.
(44) Wu, Z.; Lanni, E.; Chen, W.; Bier, M. E.; Ly, D.; Jin, R. J. Am. Chem. Soc. 2009, 131, 16672.
(45) Dass, A.; Stevenson, A.; Dubay, G. R.; Tracy, J. B.; Murray, R. W. J. Am. Chem. Soc. 2008, 130, 5940.
(46) Xiang, H. J.; Wei, S. H.; Gong, X. G. J. Am. Chem. Soc. 2010, 132, 7355.
(47) MacDonald, M. A.; Zhang, P.; Qian, H.; Jin, R. J. Phys. Chem. Lett. 2010, 1, 1821.
(48) Angel, L. A.; Majors, L. T.; Dharmaratne, A. C.; Dass, A. ACS Nano 2010, 4, 4691.
(49) Wu, Z.; Gayathri, C.; Gil, R.; Jin, R. J. Am. Chem. Soc. 2009, 131, 6535.
(50) Kogo, A.; Sakai, N.; Tatsuma, T. Electrochem. Commun. 2010, 12, 996.
(51) Zheng, N.; Johnson, J. P.; Williams, C. C.; Wang, G. Nanotechnology 2010, 21, 295708.
(52) Wang, Z.; Cai, W.; Sui, J. ChemPhysChem 2009, 10, 2012.
(53) Jiang, D. E.; Walter, M.; Dai, S. Chem. -Eur. J. 2010, 16, 4999.

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钯掺杂的25-原子和38-原子金纳米团簇

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

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