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通过固定化 MoS 量子点和酶的智能电催化界面构建组合和时序逻辑器件。

Constructing combinational and sequential logic devices through an intelligent electrocatalytic interface with immobilized MoS quantum dots and enzymes.

机构信息

Key Laboratory of Radiopharmaceuticals, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing, 100875, People's Republic of China.

School of Basic Medicine, Ningxia Medical University, Yinchuan, 750004, People's Republic of China.

出版信息

Talanta. 2022 Oct 1;248:123615. doi: 10.1016/j.talanta.2022.123615. Epub 2022 May 29.

DOI:10.1016/j.talanta.2022.123615
PMID:35687950
Abstract

Stable molybdenum disulfide quantum dots (MoS QDs) were synthesized using a simple method and embedded into chitosan (Chit) films with glucose oxidase (GOD) on the surface of a polyaniline (PANI) pre-electrodeposited ITO electrode, designated as Chit-MoS-GOD/PANI. At the prepared film electrode, the fluorescence property of MoS QDs as well as the catalytic properties of MoS QDs and GOD were well maintained and could be reversibly regulated by external stimuli, such as pH, potential, and the concentrations of glucose and ascorbic acid (AA) in the solution. By controlling the redox state of PANI with an externally applied voltage, the color of the film electrode switched between violet blue and nearly transparent, simultaneously quenching/dequenching the fluorescence signals from MoS QDs through Fӧster resonance energy transfer (FRET). The electrocatalytic signals toward hydrogen peroxide (HO), a product formed by biocatalysis between glucose and GOD, could be tuned through the catalytic capacity of MoS QDs in the films. Thus, an intelligent platform was built based on the film electrode with pH, potential, glucose and AA as inputs and UV-vis extinction (E), photoluminescent intensity (PL), and amperometric current (I) as outputs. Combinational logic operations such as a 4-input/5-output logic network and sequential logic operations such as a keypad lock and a reprogrammable delay/data (D) flip flop was first simulated in a biocomputing system with the film-modified electrode. This work demonstrated the construction of a multiple stimulus-responsive system with dual-functional nanomaterials and provided a new approach for sequential logic operations for further applications in the information storage.

摘要

稳定的二硫化钼量子点(MoS QDs)通过一种简单的方法合成,并嵌入壳聚糖(Chit)薄膜中,在聚苯胺(PANI)预先电沉积的 ITO 电极表面上具有葡萄糖氧化酶(GOD),标记为 Chit-MoS-GOD/PANI。在制备的薄膜电极中,MoS QDs 的荧光性质以及 MoS QDs 和 GOD 的催化性质得以很好地保持,并且可以通过外部刺激(例如 pH 值、电位以及溶液中葡萄糖和抗坏血酸(AA)的浓度)进行可逆调节。通过用外部施加的电压控制 PANI 的氧化还原状态,薄膜电极的颜色在紫蓝色和几乎透明之间切换,同时通过Förster 共振能量转移(FRET)猝灭/去猝灭来自 MoS QDs 的荧光信号。通过薄膜中 MoS QDs 的催化能力,可以调节作为葡萄糖和 GOD 之间生物催化产物的过氧化氢(HO)的电催化信号。因此,构建了一个基于薄膜电极的智能平台,以 pH 值、电位、葡萄糖和 AA 作为输入,以紫外可见消光(E)、光致发光强度(PL)和安培电流(I)作为输出。通过薄膜修饰电极在生物计算系统中首次模拟了组合逻辑运算,如 4 输入/5 输出逻辑网络和顺序逻辑运算,如键盘锁和可重编程延迟/数据(D)触发器。这项工作展示了具有双重功能纳米材料的多重刺激响应系统的构建,并为顺序逻辑运算提供了一种新方法,可进一步应用于信息存储。

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