Shuyun Meng, Yuye Li, Na Dong, Shuda Liu, Qingfa Gong, Yifan Liu, Li Zhang, Qijian Niu, Dong Liu, Tianyan You
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In the presence of the target Cry1Ab, the CRISPR/Cas12a system is activated to shear the ZIF-based heterojunction, resulting in the disintegration of the heterojunction and the disappearance of interfacial carrier migration. At this point, ZIF-Hemin is released from the CdSe/NH<sub>2</sub>-rGO interface, with the photocurrent switching from the anode to the cathode. Meanwhile, due to its rich accessible active sites, the released ZIF-Hemin nanosheet shows high peroxidase-like catalytic activity and generates colorimetric signals. The dual-modal biosensor demonstrates excellent performance in selectivity and sensitivity, with low detection limits of 0.05 pg mL<sup>–1</sup> (PEC) and 0.4 pg mL<sup>–1</sup> (colorimetric). 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引用次数: 0
摘要
调节异质结中界面载流子的迁移对于驱动高性能光学生物传感器的信号响应至关重要。本研究设计了一种极性可切换光电化学(PEC)和纳米酶比色双模态生物传感器,利用茎环 DNA 和 CRISPR/Cas12a 系统来调节基于沸石咪唑框架(ZIF)的异质结的界面载流子迁移。具体来说,ZIF-hemin(ZIF-Hemin)通过茎环 DNA 组装在 CdSe/NH2-rGO 界面上,形成基于 ZIF 的异质结。具有加强筋效应的茎环 DNA 可增强结合力,并加速异质结的界面载流子迁移。在目标 Cry1Ab 存在的情况下,CRISPR/Cas12a 系统被激活,对基于 ZIF 的异质结进行剪切,导致异质结解体,界面载体迁移消失。此时,ZIF-Hemin 从 CdSe/NH2-rGO 界面释放,光电流从阳极切换到阴极。同时,由于具有丰富的可访问活性位点,释放出的 ZIF-Hemin 纳米片显示出很高的过氧化物酶催化活性,并产生比色信号。该双模式生物传感器在选择性和灵敏度方面表现出色,检测限低至 0.05 pg mL-1(过氧化物酶法)和 0.4 pg mL-1(比色法)。这项研究为通过调节异质结中界面载流子的迁移来提高光学生物传感器的性能提供了一种通用策略。
CRISPR/Cas12a-Sheared ZIF-Based Heterojunction to Allow Polarity-Switchable Photoelectrochemical and Nanozyme-Enabled Colorimetric Dual-Modal Biosensing
Modulating the migration of interfacial carriers in heterojunctions is critical for driving the signal response of high-performance optical biosensors. In this study, a polarity-switchable photoelectrochemical (PEC) and nanozyme-enabled colorimetric dual-modal biosensor is designed to modulate the interfacial carrier migration of the zeolitic imidazolate framework (ZIF)-based heterojunction by exploiting stem-loop DNA and the CRISPR/Cas12a system. Specifically, ZIF-hemin (ZIF-Hemin) is assembled at the CdSe/NH2-rGO interface via stem-loop DNA to form a ZIF-based heterojunction. Stem-loop DNA with a reinforcing rib effect enhances binding and accelerates the interfacial carrier migration of the heterojunction. In the presence of the target Cry1Ab, the CRISPR/Cas12a system is activated to shear the ZIF-based heterojunction, resulting in the disintegration of the heterojunction and the disappearance of interfacial carrier migration. At this point, ZIF-Hemin is released from the CdSe/NH2-rGO interface, with the photocurrent switching from the anode to the cathode. Meanwhile, due to its rich accessible active sites, the released ZIF-Hemin nanosheet shows high peroxidase-like catalytic activity and generates colorimetric signals. The dual-modal biosensor demonstrates excellent performance in selectivity and sensitivity, with low detection limits of 0.05 pg mL–1 (PEC) and 0.4 pg mL–1 (colorimetric). This work provides a general strategy to improve the performance of optical biosensors by modulating the migration of interfacial carriers in heterojunctions.
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.