Dual-Label Sequentially Released DNA Probe for Self-Powered PEC-RGB Sensing of Coexisting Mycotoxins

IF 7.3 1区化学 Q1 CHEMISTRY, ANALYTICAL

Analytical Chemistry Pub Date : 2026-10-16 DOI:10.1021/acs.analchem.6c05916

Yanru Zhang,Yutong Fu,Xue Fan,Hongye Liu,Jingyao Peng,Ying Sun,Xuechen Zhang,Wenbo Song,Daqian Song

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引用次数: 0

Abstract

Abstract On-site assay of multiple coexisting mycotoxins is critical for securing food safety and safeguarding public health. Photoelectrochemical (PEC) sensing meets the demand of on-site analysis owing to the advantages of easy miniaturization, rapid response, and low cost. However, existing signal discrimination strategies for multiplexed PEC detection typically rely on complex electrode modification and external instrumentation, limiting their on-site applicability. To address this issue, we developed a dual-label sequentially released DNA probe (DSRDP) and constructed an ion exchange-mediated modification-free self-powered sensing platform, which enables on-site PEC red-green-blue (RGB) sensing of dual targets. The DSRDP was formed by assembling Ag NPs-terminated double-stranded DNA and PC-Linker-modified hairpin DNA bearing CuO NPs on the magnetic beads’ surface. Upon the simultaneous recognition of two targets, the first signal label (Ag NPs) was obtained in the supernatant through magnetic separation, and the other signal label (CuO NPs) was released via UV-induced photocleavage of the photocleavable linker (PC-Linker). Subsequently, acidification of each signal label triggered the ion exchange (Ag+ or Cu2+) with the MgIn2S4 photoanode, which quenched the photocurrent resulting from the heterostructure formation. Meanwhile, Ag+ or Cu2+ also induced a color change of Na2S solution, which provided the visual RGB signal for the dual-target assay using a smartphone. The PEC-RGB sensor exhibited linear ranges of 1 fg/mL−100 ng/mL of aflatoxin B1 (AFB1) and ochratoxin A (OTA) with LODs of 0.24 fg/mL and 0.33 fg/mL in PEC mode, respectively, and linear ranges of 1 pg/mL−100 ng/mL of AFB1 and OTA with LODs of 10.96 fg/mL and 3.63 fg/mL in RGB mode, respectively. Featuring convenient target separation, rapid signal transduction, and self-powered detection, this work may pave the way for portable on-site detection of coexisting mycotoxins for food safety assessment and environmental monitoring.

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双标签顺序释放DNA探针用于自供电PEC-RGB感应共存真菌毒素

摘要多种共存真菌毒素的现场检测对保障食品安全和公众健康至关重要。光电化学（PEC）传感具有易于小型化、响应速度快、成本低等优点，满足了现场分析的需要。然而，现有的多路PEC检测信号识别策略通常依赖于复杂的电极修饰和外部仪器，限制了其现场适用性。为了解决这一问题，我们开发了一种双标签顺序释放DNA探针（DSRDP），并构建了一个离子交换介导的无修饰自供电传感平台，实现了双靶标的现场PEC红绿蓝（RGB）传感。DSRDP是通过在磁珠表面组装Ag NPs终止的双链DNA和pc - linker修饰的带有CuO NPs的发夹DNA而形成的。同时识别两个靶标后，通过磁分离在上清液中获得第一个信号标记（Ag NPs），另一个信号标记（CuO NPs）通过光切割连接子（PC-Linker）的紫外诱导光裂解释放。随后，每个信号标签的酸化触发离子交换（Ag+或Cu2+）与MgIn2S4光阳极，这淬灭了由异质结构形成的光电流。同时，Ag+或Cu2+也能引起Na2S溶液的颜色变化，为智能手机双靶检测提供了视觉RGB信号。PEC-RGB传感器对黄曲霉毒素B1 （AFB1）和赭曲霉毒素A （OTA）的检测线性范围为1 fg/mL ~ 100 ng/mL，在PEC模式下的lod分别为0.24 fg/mL和0.33 fg/mL；对AFB1和OTA的检测线性范围为1 pg/mL ~ 100 ng/mL，在RGB模式下的lod分别为10.96 fg/mL和3.63 fg/mL。该方法具有目标分离方便、信号转导快速、检测自供电等特点，可为食品安全评价和环境监测中共存真菌毒素的便携式现场检测奠定基础。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Analytical Chemistry 化学-分析化学

CiteScore

12.10

自引率

12.20%

发文量

1949

审稿时长

1.4 months

期刊介绍： Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.