Jiang Kai, Xie Hong, Zhan Wei
Department of Chemistry and Biochemistry, Auburn University, Auburn, Alabama 36849, USA.
Langmuir. 2009 Sep 15;25(18):11129-36. doi: 10.1021/la901548b.
A new photocurrent-generation system based on Ru(bpy)3(2+) (bpy=2,2'-bipyridine) tethered on phospholipid/alkanethiol hybrid bilayers in aqueous media is reported. The construction of such a system is straightforward. First, a self-assembled monolayer (SAM) of alkanethiol is formed on gold, and separately, liposomes containing Ru(bpy)3(2+)-conjugated dioleoylphosphoethanolamine (DOPE) are prepared by extrusion. Subsequent exposure of the Ru(bpy)3(2+)-containing liposome solution to the preformed SAM induces the addition of a monolayer of phospholipids on top of the SAM and thereby the immobilization of a Ru(bpy)3(2+) layer on the gold electrode. Either anodic or cathodic photocurrent generation can be obtained, when ascorbate (anodic) or methyl violgen/oxygen (cathodic) is used as a sacrificial electron donor/acceptor, respectively. Light conversion quantum efficiencies of 0.84% (anodic) and 0.21% (cathodic) were obtained under blue light (lambda=470+/-20 nm) irradiation. The photocurrent-generation and electron-transfer mechanisms of this new system as well as its potential usefulness in fundamental photoconversion studies are discussed.
报道了一种基于钌(联吡啶)3(2 +)(联吡啶= 2,2'-联吡啶)固定在水介质中的磷脂/烷硫醇混合双层上的新型光电流产生系统。这种系统的构建很简单。首先,在金上形成烷硫醇的自组装单层(SAM),然后通过挤压制备含有钌(联吡啶)3(2 +)共轭二油酰基磷脂酰乙醇胺(DOPE)的脂质体。随后将含钌(联吡啶)3(2 +)的脂质体溶液暴露于预先形成的SAM中,会在SAM顶部诱导添加单层磷脂,从而将钌(联吡啶)3(2 +)层固定在金电极上。当分别使用抗坏血酸盐(阳极)或甲基紫精/氧气(阴极)作为牺牲电子供体/受体时,可以获得阳极或阴极光电流产生。在蓝光(λ= 470±20 nm)照射下,光转换量子效率分别为0.84%(阳极)和0.21%(阴极)。讨论了这种新系统的光电流产生和电子转移机制及其在基础光转换研究中的潜在用途。