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将CuO/g-CN p-n异质结光阴极与MoS QDs@Cu NWs多功能信号放大器集成用于超灵敏检测AβO。

Integrating CuO/g-CN p-n heterojunctioned photocathode with MoS QDs@Cu NWs multifunctional signal amplifier for ultrasensitive detection of AβO.

作者信息

Zhang Jinling, Zhang Xuechen, Gao Yao, Yan Jianyue, Song Wenbo

机构信息

College of Chemistry, Jilin University, Changchun, 130012, PR China.

College of Chemistry, Jilin University, Changchun, 130012, PR China.

出版信息

Biosens Bioelectron. 2021 Mar 15;176:112945. doi: 10.1016/j.bios.2020.112945. Epub 2020 Dec 30.

Abstract

Superior to anodic photoelectrochemical (PEC) method, cathodic bioanalysis integrates merits of excellent anti-interference and high stability, representing a promising and competitive methodology in precise monitoring targets in complex matrices. However, serious consideration of photocathode is far behind the anodic one, developing high-performance photocathode for PEC biosensing is thus urgently desired. Herein, a high-performance cathodic PEC aptasensing platform for detection of amyloid-beta oligomers (AβO) was constructed by integrating CuO/g-CN p-n heterojunction with MoS QDs@Cu NWs multifunction signal amplifier. The CuO/g-CN, exhibiting intense visible light-harvesting and high photoelectric conversion efficiency, was synthesized by in-situ pyrolysis of Cu-MOF and dicyandiamide. The MoS QDs@Cu NWs was obtained by electrostatical self-assembly, which acted not only as a sensitizer to boost PEC response, but also as a nanozyme for biocatalytic precipitation. The aptasensor was fabricated by DNA hybridization between the cDNA on photocathode and MoS QDs@Cu NWs-labeled aptamer. Based on "on-off-on" photocurrent response generated by multifunction signal amplification, ultrasensitive aptasensing of AβO was realized in a wider linear range from 10 fM to 0.5 μM with an ultralow detection limit of 5.79 fM. The feasibility of the sensor for AβO determination in human blood serum was demonstrated.

摘要

与阳极光电化学(PEC)方法相比,阴极生物分析具有抗干扰性强和稳定性高的优点,是在复杂基质中精确监测目标的一种有前景且具竞争力的方法。然而,对光阴极的深入研究远远落后于阳极光阴极,因此迫切需要开发用于PEC生物传感的高性能光阴极。在此,通过将CuO/g-CN p-n异质结与MoS QDs@Cu NWs多功能信号放大器相结合,构建了一种用于检测淀粉样β寡聚体(AβO)的高性能阴极PEC适体传感平台。通过Cu-MOF和双氰胺的原位热解合成了具有强烈可见光捕获能力和高光电转换效率的CuO/g-CN。通过静电自组装获得了MoS QDs@Cu NWs,它不仅作为敏化剂增强PEC响应,还作为纳米酶用于生物催化沉淀。通过光阴极上的cDNA与MoS QDs@Cu NWs标记的适体之间的DNA杂交制备了适体传感器。基于多功能信号放大产生的“开-关-开”光电流响应,在10 fM至0.5 μM的更宽线性范围内实现了对AβO的超灵敏适体传感,检测限低至5.79 fM。证明了该传感器用于测定人血清中AβO的可行性。

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