College of Chemistry, Beijing Normal University, Beijing 100875, P. R. China.
Nanoscale. 2018 Apr 26;10(16):7484-7493. doi: 10.1039/c8nr01258j.
In this work, a resettable 4-input/2-output keypad lock system based on red-emission carbon dots (rCDs) and Prussian blue (PB) modified electrodes was developed. Electrochromic PB layers were first electrochemically deposited on the indium tin oxide (ITO) electrode surface. An admixture of rCDs and chitosan (Chi) was then cast on the surface of PB layers, forming rCDs-Chi/PB film electrodes. UV-vis absorption of the films was sensitive to the applied potential since the blue PB constituent of the films would be transformed to nearly colorless Prussian white (PW) at the reduction potential of -0.2 V and then from PW back to PB at the oxidation potential of 0.4 V, and the transformation between PB and PW would also influence the fluorescence emission of the rCD constituent in the films. The addition of cysteine (Cys) in the testing solution could reduce the PB in the films into PW and generate an amperometric electrocatalytic current at 0.4 V. Meanwhile, the addition of Fe3+ in solution could greatly quench the fluorescence from the rCD component in the films. Thus, the responses of UV-vis absorbance, fluorescence emission and amperometric current of the rCDs-Chi/PB film electrode system exhibited potential-, Cys- and Fe3+-responsive switching properties. Based on the aforementioned work, a combinational logic gate circuit with 3 inputs and 3 outputs was established. In particular, on the same platform, a novel chemical/molecular 4-input/2-output keypad lock with easy resettability was elaborately designed with amperometric current and fluorescence peak intensity as two different types of outputs, so that a higher security level could be achieved.
在这项工作中,开发了一种基于红色发光碳点(rCDs)和普鲁士蓝(PB)修饰电极的可重置 4 输入/2 输出键盘锁系统。首先,将电化学沉积的 PB 层沉积在氧化铟锡(ITO)电极表面。然后,将 rCDs 和壳聚糖(Chi)的混合物浇铸在 PB 层的表面上,形成 rCDs-Chi/PB 薄膜电极。由于薄膜中的蓝色 PB 成分在还原电位为-0.2 V 时会转化为几乎无色的普鲁士白(PW),然后在氧化电位为 0.4 V 时从 PW 再转化为 PB,因此薄膜的 UV-vis 吸收对施加的电位敏感,并且 PB 和 PW 之间的转变也会影响薄膜中 rCD 成分的荧光发射。在测试溶液中添加半胱氨酸(Cys)可以将薄膜中的 PB 还原为 PW,并在 0.4 V 时产生安培电流。同时,溶液中添加 Fe3+可以大大猝灭薄膜中 rCD 成分的荧光。因此,rCDs-Chi/PB 薄膜电极系统的 UV-vis 吸光度、荧光发射和安培电流响应表现出电位、Cys 和 Fe3+响应的开关特性。基于上述工作,建立了一个具有 3 个输入和 3 个输出的组合逻辑门电路。特别是,在同一个平台上,设计了一种新颖的化学/分子 4 输入/2 输出键盘锁,具有易重置性,以安培电流和荧光峰强度作为两种不同类型的输出,从而可以实现更高的安全级别。