Conversion of anionic [Au25(SCH2CH2Ph)18]- cluster to charge neutral cluster via air oxidation

被引:392
作者
Zhu, Manzhou [1 ]
Eckenhoff, William T. [2 ]
Pintauer, Tomislav [2 ]
Jin, Rongchao [1 ]
机构
[1] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA
[2] Duquesne Univ, Dept Chem & Biochem, Pittsburgh, PA 15282 USA
关键词
D O I
10.1021/jp805786p
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We report a solution-phase conversion process of the [Au-25(SCH2CH2Ph)(18)](-) anionic cluster into a charge neutral cluster [Au-25(SCH2CH2Ph)(18)](0) via air oxidation. The one-electron loss of the Au-25(-) cluster and conversion to Au-25(0) is a surprise in light of the chemical inertness of gold nanoparticles. In contrast with the crystal structure of the anion Cluster Au-25(-), which exhibits apparent structural distortions in the Au25S18 framework, such distortions are not observed in the neutral cluster. The cluster charge effect is also manifested in the optical absorption spectra of the clusters. Given the only recently reported structure of the parent Au-25(-) cluster, it is of substantial interest whether its one-electron oxidized product is similar to that of Au-25(-). This work unambiguously determined the structure of the one-electron oxidized product and correlates the structure with the optical properties.
引用
收藏
页码:14221 / 14224
页数:4
相关论文
共 51 条
[1]   On the structure of thiolate-protected Au25 [J].
Akola, Jaakko ;
Walter, Michael ;
Whetten, Robert L. ;
Haekkinen, Hannu ;
Groenbeck, Henrik .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (12) :3756-+
[2]   Molecular electron-transfer properties of Au38 clusters [J].
Antonello, Sabrina ;
Holm, Allan H. ;
Instuli, Emanuele ;
Maran, Flavio .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (32) :9836-+
[3]   Structure and bonding of gold metal clusters, colloids, and nanowires studied by EXAFS, XANES, and WAXS [J].
Benfield, RE ;
Grandjean, D ;
Kröll, M ;
Pugin, R ;
Sawitowski, T ;
Schmid, G .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (10) :1961-1970
[4]   MIXED-METAL GOLD CLUSTERS - SYNTHESIS AND X-RAY STRUCTURAL CHARACTERIZATION OF [AU5RE(H)4(PPH3)7](PF6)2 AND [AU3RH(H)(CO)(PPH3)5](PF6) [J].
BOYLE, PD ;
JOHNSON, BJ ;
BUEHLER, A ;
PIGNOLET, LH .
INORGANIC CHEMISTRY, 1986, 25 (01) :5-7
[5]  
Cerrada E, 2000, ANGEW CHEM INT EDIT, V39, P2353, DOI 10.1002/1521-3773(20000703)39:13<2353::AID-ANIE2353>3.0.CO
[6]  
2-R
[7]   Self-assembling of monolayer-protected gold nanoparticles [J].
Chen, SW .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (04) :663-667
[8]  
CRESPO O, 2003, ANGEW CHEM INT EDIT, V36, P993
[9]   Synthesis and structural analysis of the first nanosized platinum-gold carbonyl/phosphine cluster, Pt13[Au2(PPh3)2]2(CO)10(PPh3)4, containing a Pt-centered [Ph3PAu-AuPPh3]-capped icosahedral Pt12 cage [J].
de Silva, N ;
Dahl, LF .
INORGANIC CHEMISTRY, 2005, 44 (26) :9604-9606
[10]   The four-step, double-autocatalytic mechanism for transition-metal nanocluster nucleation, growth, and then agglomeration: Metal, ligand, concentration, temperature, and solvent dependency studies [J].
Finney, Eric E. ;
Finke, Richard G. .
CHEMISTRY OF MATERIALS, 2008, 20 (05) :1956-1970