Diode-like electron transfer across nanostructured films containing a redox ligand

被引:93
作者
Gittins, DI [1 ]
Bethell, D [1 ]
Nichols, RJ [1 ]
Schiffrin, DJ [1 ]
机构
[1] Univ Liverpool, Dept Chem, Liverpool L69 7ZD, Merseyside, England
关键词
D O I
10.1039/a902960e
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
Novel redox active dithiols containing the viologen (4,4'-bipyridinium group) have been synthesised. Monolayers and multilayers consisting of alternating layers of the dithiol and gold nanoparticles have been self-assembled on a gold substrate and visualised using SPM. Such materials have been investigated for their electroactivity and their ability to mediate electron transfer to an external redox couple, [Ru(NH3)(6)](3+/2+), in aqueous solution. Viologen moieties in these multilayers are addressable electrochemically provided they are within 6-8 layers of the external surface and it is shown that electron transfer through the deeper layers is very facile as a consequence of the presence of partially filled viologen pi-orbitals. When the viologen containing dithiol is present in the outer layer, a diode effect is observed; electron transfer from the multilayer to the external couple takes place, but the reverse electron transport is inhibited.
引用
收藏
页码:79 / 83
页数:5
相关论文
共 36 条
[1]   Semiconductor clusters, nanocrystals, and quantum dots [J].
Alivisatos, AP .
SCIENCE, 1996, 271 (5251) :933-937
[2]   Self-assembly of a two-dimensional superlattice of molecularly linked metal clusters [J].
Andres, RP ;
Bielefeld, JD ;
Henderson, JI ;
Janes, DB ;
Kolagunta, VR ;
Kubiak, CP ;
Mahoney, WJ ;
Osifchin, RG .
SCIENCE, 1996, 273 (5282) :1690-1693
[3]  
[Anonymous], VIOLOGENS
[4]   Surface plasmon enhanced non-linear optical response of gold nanoparticles at the air/toluene interface [J].
Antoine, R ;
Brevet, PF ;
Girault, HH ;
Bethell, D ;
Schiffrin, DJ .
CHEMICAL COMMUNICATIONS, 1997, (19) :1901-1902
[5]   Superstructures of functional colloids: Chemistry on the nanometer scale [J].
Antonietti, M ;
Goltner, C .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION IN ENGLISH, 1997, 36 (09) :910-928
[6]   Structure and dynamics in alkanethiolate monolayers self-assembled on gold nanoparticles: A DSC, FT-IR, and deuterium NMR study [J].
Badia, A ;
Cuccia, L ;
Demers, L ;
Morin, F ;
Lennox, RB .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (11) :2682-2692
[7]  
BARD AJ, 1980, ELECTROCHEMICAL METH
[8]   Electrochemical charge injection into immobilized nanosized gold particle ensembles: Potential modulated transmission and reflectance spectroscopy [J].
Baum, T ;
Bethell, D ;
Brust, M ;
Schiffrin, DJ .
LANGMUIR, 1999, 15 (03) :866-871
[9]   From monolayers to nanostructured materials: An organic chemist's view of self-assembly [J].
Bethell, D ;
Brust, M ;
Schiffrin, DJ ;
Kiely, C .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1996, 409 (1-2) :137-143
[10]   SYNTHESIS OF THIOL-DERIVATIZED GOLD NANOPARTICLES IN A 2-PHASE LIQUID-LIQUID SYSTEM [J].
BRUST, M ;
WALKER, M ;
BETHELL, D ;
SCHIFFRIN, DJ ;
WHYMAN, R .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1994, (07) :801-802