基于表面钝化效应的增强型均相阴极光电化学分析

引用本文: 闫梦华, 杨高霞, 王光丽. 基于表面钝化效应的增强型均相阴极光电化学分析[J]. 分析化学, 2023, 51(2): 276-286. doi: 10.19756/j.issn.0253-3820.221494 shu

Citation: YAN Meng-Hua, YANG Gao-Xia, WANG Guang-Li. Enhanced and Homogeneous Cathodic Photoelectrochemical Analysis Based on Surface Passivation Effect[J]. Chinese Journal of Analytical Chemistry, 2023, 51(2): 276-286. doi: 10.19756/j.issn.0253-3820.221494 shu

基于表面钝化效应的增强型均相阴极光电化学分析

江南大学化学与材料工程学院, 合成与生物胶体教育部重点实验室, 无锡 214122

通讯作者: 王光丽,E-mail:glwang@jiangnan.edu.cn

基金项目:
国家自然科学基金项目(No.22174054)资助。

摘要: 基于Cd²⁺对硒化铅量子点（PbSe QDs）光电流的增强作用，构建了新型的分离式均相光电化学（PEC）传感器，分别用于miRNA-21和癌胚抗原（CEA）的灵敏检测。此传感器利用含有T-Hg²⁺-T碱基错配的发夹结构DNA，其环部分别与miRNA-21或CEA适配体的互补链结合形成双链，借助DNA链置换反应进行信号放大，释放发夹结构中的Hg²⁺。Hg²⁺与CdS QDs进行阳离子交换释放Cd²⁺，Cd²⁺与固定在电极上的PbSe QDs发生阳离子交换反应，在PbSe QDs表面形成硒化镉（CdSe），消除了PbSe表面的电子-空穴复合中心，提高了电荷的分离效率，增强了光电流响应。本方法检测miRNA-21的线性范围为5.0×10^-16~5.0×10^-10 mol/L，检出限为6.8×10^-17 mol/L（S/N=3）；对CEA检测的线性范围为5.0×10^-2~5.0×10⁴ pg/mL，检出限为0.007 pg/mL（S/N=3）。此传感器具有良好的抗干扰性和选择性，可用于实际样品的检测。

关键词:

English

Enhanced and Homogeneous Cathodic Photoelectrochemical Analysis Based on Surface Passivation Effect

Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China

Corresponding author: WANG Guang-Li, glwang@jiangnan.edu.cn

Received Date: 06 October 2022
Revised Date: 01 December 2022
Fund Project:
Supported by the National Natural Science Foundation of China (No.22174054).

Abstract: Homogeneous and split-type photoelectrochemical (PEC) sensors based on the enhancement effect of Cd²⁺ on the photocurrent of lead selenide quantum dots (PbSe QDs) were constructed for sensitive detection of miRNA-21 and carcinoembryonic antigen (CEA). The detection method used the hairpin DNA assembly by T-Hg²⁺-T base mismatch, whose loops were combined with miRNA-21 or the complementary strand of CEA aptamer to form double strands. Signal amplification was carried out by non-enzymatic DNA strand displacement reaction to release Hg²⁺ in the hairpin structure, and then the released Hg²⁺ exchanged ions with cadmium sulfide quantum dots (CdS QDs) to release Cd²⁺. Then, Cd²⁺ reacted with PbSe QDs modified electrode to form cadmium selenide (CdSe) layer on its surface, which eliminated the electron-hole recombination center on the surface and improved the charge separation efficiency, realizing enhanced photocurrent output. The experimental results showed that the linear range for detection of miRNA-21 was 5.0×10^-16-5.0×10^-10 mol/L, and the detection limit was 6.8×10^-17 mol/L (S/N = 3). The logarithm of the concentration of CEA was linear with the photocurrent in the range of 5.0×10^-2-5.0×10⁴ pg/mL, and the detection limit was 0.007 pg/mL (S/N = 3). The developed PEC biosensors showed good selectivity and could be used for detection of real samples with satisfactory results.

Key words:

Cathodic photoelectrochemistry
/ Lead selenide quantum dots
/ Non-enzymatic strand displacement amplification reaction
/ Surface passivation

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

基于表面钝化效应的增强型均相阴极光电化学分析

通讯作者: 王光丽,E-mail:glwang@jiangnan.edu.cn

English

Enhanced and Homogeneous Cathodic Photoelectrochemical Analysis Based on Surface Passivation Effect

Corresponding author: WANG Guang-Li, glwang@jiangnan.edu.cn

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

基于表面钝化效应的增强型均相阴极光电化学分析

通讯作者: 王光丽,E-mail:glwang@jiangnan.edu.cn

English

Enhanced and Homogeneous Cathodic Photoelectrochemical Analysis Based on Surface Passivation Effect

Corresponding author: WANG Guang-Li, glwang@jiangnan.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs