Modular "Click" Chemistry for Electrochemically and Photoelectrochemically Active Molecular Interfaces to Tin Oxide Surfaces

被引:39
作者
Benson, Michelle C. [1 ]
Ruther, Rose E. [1 ]
Gerken, James B. [1 ]
Rigsby, Matthew L. [1 ]
Bishop, Lee M. [1 ]
Tan, Yizheng [1 ]
Stahl, Shannon S. [1 ]
Hamers, Robert J. [1 ]
机构
[1] Univ Wisconsin, Dept Chem, Madison, WI 53706 USA
基金
美国国家科学基金会;
关键词
click chemistry; tin oxide; surface; electron transfer; metal oxide; surface functionalization; SENSITIZED SOLAR-CELLS; ELECTRON-TRANSFER; COVALENT ATTACHMENT; TIO2; SNO2; TRANSPORT; EFFICIENCY; RUTHENIUM(II); SPECTROSCOPY; DYNAMICS;
D O I
10.1021/am200615r
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
We demonstrate the use of "click" chemistry to form electrochemically and photoelectrochemically active molecular interfaces to SnO2 nanoparticle thin films. By using photochemical grafting to link a short-chain alcohol to the surface followed by conversion to a surface azide group, we enable use of the Cu(I)-catalyzed azide-alkyne [3 + 2] cycloaddition (CuAAC) reaction, a form of "click" chemistry, on metal oxide surfaces. Results are shown with three model compounds to test the surface chemistry and subsequent ability to achieve electrochemical and photoelectrochemical charge transfer. Surface-tethered ferrocene groups exhibit good electron-transfer characteristics with thermal rates estimated at >1000 s(-1). Time-resolved surface photovoltage measurements using a ruthenium terpyridyl coordination compound demonstrate photoelectron charge transfer on time scales of nanoseconds or less, limited by the laser pulse width. The results demonstrate that the CuAAC "click" reaction can be used to form electrochemically and photoelectrochemically active molecular interfaces to SnO2 and other metal oxide semiconductors.
引用
收藏
页码:3110 / 3119
页数:10
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