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将 TiC/MgInS 异质结与控制释放策略集成,用于 miRNA-21 的分体式光电化学传感。

Integrating TiC/MgInS heterojunction with a controlled release strategy for split-type photoelectrochemical sensing of miRNA-21.

机构信息

School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, PR China.

Institute for Advanced Interdisciplinary Research, University of Jinan, Jinan, 250022, PR China.

出版信息

Anal Chim Acta. 2022 Jul 4;1215:339990. doi: 10.1016/j.aca.2022.339990. Epub 2022 May 25.

Abstract

The harsh operating conditions and time-consuming fabrication process of the photoelectrode modification process have limited the potential applications of photoelectrochemical (PEC) sensors. To overcome these drawbacks, this study introduced a unique split-type PEC biosensor for microRNA-21 (miRNA-21) detection. Specifically, a TiC/MgInS heterojunction was adopted as the photosensitive material, and a target-controlled glucose release system, comprising a multifunctional porphyrin-based metal-organic framework (PCN-224), was used for signal amplification. The TiC/MgInS heterojunction effectively separated the photogenerated electrons and holes, and improved the photoelectric conversion efficiency, offering a strong initial photocurrent signal during PEC biosensing. Meanwhile, the porous PCN-224 acted as a nimble nanocontainer that encapsulated glucose using a capture probe (CP). In the presence of miRNA-21, the CP formed a CP-miRNA-21 complex and then detached from PCN-224, controllably releasing the trapped glucose. The oxidization of glucose by glucose oxidase resulted in hydrogen peroxide generation, which acted as a scavenger for the holes generated on the surface of TiC/MgInS, and significantly enhanced the photocurrent response under visible light irradiation. Finally, the sensor exhibited good performance for miRNA-21 detection with a low detection limit (0.17 fM) and wide linearity range (0.5 fM-1.0 nM). Thus, the proposed TiC/MgInS-based split-type PEC sensor is a promising tool for sensitive and accurate detection of miRNA-21 and provides an innovative basis for the preparation of other high-performance sensors.

摘要

光电化学(PEC)传感器的光电电极修饰过程苛刻的操作条件和耗时的制造工艺限制了其潜在应用。为了克服这些缺点,本研究引入了一种独特的分体式 PEC 生物传感器用于检测 microRNA-21(miRNA-21)。具体来说,采用 TiC/MgInS 异质结作为光敏材料,采用目标控制的葡萄糖释放系统,包括多功能卟啉基金属有机骨架(PCN-224),用于信号放大。TiC/MgInS 异质结有效地分离了光生电子和空穴,提高了光电转换效率,在 PEC 生物传感过程中提供了强大的初始光电流信号。同时,多孔 PCN-224 充当灵活的纳米容器,使用捕获探针 (CP) 封装葡萄糖。在 miRNA-21 存在的情况下,CP 形成 CP-miRNA-21 复合物,然后从 PCN-224 上脱离,可控地释放被捕获的葡萄糖。葡萄糖氧化酶氧化葡萄糖产生过氧化氢,作为 TiC/MgInS 表面生成的空穴的清除剂,在可见光照射下显著增强了光电流响应。最后,该传感器对 miRNA-21 的检测表现出良好的性能,具有低检测限(0.17 fM)和宽线性范围(0.5 fM-1.0 nM)。因此,所提出的基于 TiC/MgInS 的分体式 PEC 传感器是一种用于灵敏和准确检测 miRNA-21 的有前途的工具,并为制备其他高性能传感器提供了创新基础。

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