State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences , Changchun, Jilin 130022, China.
University of Science and Technology of China , Hefei, Anhui 230029, P. R. China.
Anal Chem. 2017 Apr 4;89(7):3867-3872. doi: 10.1021/acs.analchem.7b00246. Epub 2017 Mar 22.
A highly efficient fluorescence switch system based on a closed bipolar electrode (C-BPE) system was proposed for the first time. Here, Au nanoclusters (Au NCs) were premodified on one pole of the BPE and acted as the fluorescent donor. On the basis of the spectral overlap between the absorbance of electrochromic material-Prussian blue (PB) and the fluorescence spectrum of Au NCs, fluorescence quenching ("off" state) induced by the inner filter effect was observed. Due to the electrochemical reversible redox reaction between PB and Prussian white, switching the polarity of driving voltage could easily achieve the fluorescence recovery of the Au NCs, corresponding to the "on" state. Through the reasonable design of C-BPE and optimization of driving voltage, the on-off ratio of the integrated fluorescence switch was up to 2.7 and a good fatigue resistance while performing 10 on-off cycles was obtained owing to the good stability of Au NCs and the reversible redox feature of PB. The introduction of BPE made the fluorescence switch more simple and controllable compared with the traditional three-electrode system, which will provide a new route for the design of the electrical-stimuli responsive fluorescence switch, especially for the integration of the miniaturized device.
首次提出了一种基于闭双极电极（C-BPE）系统的高效荧光开关系统。在这里，Au 纳米团簇（Au NCs）预先修饰在 BPE 的一个极上，充当荧光供体。基于电致变色材料普鲁士蓝（PB）的吸收光谱与 Au NCs 的荧光光谱之间的光谱重叠，观察到内滤效应引起的荧光猝灭（“关”态）。由于 PB 和普鲁士白之间的电化学可逆氧化还原反应，通过改变驱动电压的极性，可以轻松实现 Au NCs 的荧光恢复，对应于“开”态。通过合理设计 C-BPE 和优化驱动电压，集成荧光开关的开-关比高达 2.7，并且在进行 10 次开-关循环时表现出良好的疲劳抗性，这归因于 Au NCs 的良好稳定性和 PB 的可逆氧化还原特性。与传统的三电极系统相比，BPE 的引入使荧光开关更加简单和可控，这将为电刺激响应荧光开关的设计提供新途径，特别是对于小型化设备的集成。
