Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, Institute for Advanced Interdisciplinary Research, University of Jinan, Jinan 250022, P.R. China.
Collaborative Innovation Center for Green Chemical Manufacturing and Accurate Detection, School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P.R. China.
Anal Chem. 2020 Jun 2;92(11):7604-7611. doi: 10.1021/acs.analchem.0c00231. Epub 2020 May 11.
Herein an ultrasensitive photoelectrochemical (PEC)/visual biosensor coupled with a multiple signal amplification strategy was proposed for the detection of nucleic acids. The initial signal amplification was achieved via ternary AgInSe quantum dot (QD)-sensitized ZnO nanoflowers (ZnO NFs) to form an excellent photoelectric layer. A gold-modified nanorod-anchored CeO (Au@NR-CeO) octahedron was introduced as a multifunctional signal regulator via the formation of triple helix molecules. The Au@NR-CeO octahedron could not only quench the photocurrent signal due to the competitive capture of photon energy and electron donors with the photoelectric layer but could also act like a peroxidase to catalyze the formation of mimetic enzymatic catalytic precipitation (MECP) on the surface of the photoelectric layer. Furthermore, the steric hindrance effect from the Au@NR-CeO octahedron further reduced the output of the photocurrent signal. After incubation with t-DNA, the triple helix conformation was disassembled and the Au@NR-CeO octahedron was released from the electrode surface, leading to the significant increase of photocurrent signal. Meanwhile, the released Au@NR-CeO octahedron could flow into the colorimetric area of the lab-on-paper device to catalyze the occurrence of the color reaction, achieving a visual detection for t-DNA. On the basis of the multiple signal amplification strategy, t-DNA was detected specifically with a lower limit of detection of 0.28 fM and a wider linear range from 0.5 fM to 50 nM. The proposed method has the potential utility to detect a variety of nucleic acids and biomarkers.
本文提出了一种基于光电化学(PEC)/可视化生物传感器的超灵敏检测核酸的方法,该方法结合了多重信号放大策略。首先,通过三元 AgInSe 量子点(QD)敏化 ZnO 纳米花(ZnO NFs)形成了优异的光电层,实现了初始信号的放大。然后,通过形成三螺旋分子,引入了金修饰的纳米棒锚定的 CeO(Au@NR-CeO)八面体作为多功能信号调节剂。由于光电层与光电子层竞争捕获光子能量和电子供体,Au@NR-CeO 八面体不仅可以猝灭光电流信号,还可以像过氧化物酶一样在光电层表面催化模拟酶催化沉淀(MECP)的形成。此外,Au@NR-CeO 八面体的空间位阻效应进一步降低了光电流信号的输出。与 t-DNA 孵育后,三螺旋构象被拆开,Au@NR-CeO 八面体从电极表面释放出来,导致光电流信号显著增加。同时,释放的 Au@NR-CeO 八面体可以流入纸芯片装置的比色区,以催化显色反应的发生,实现对 t-DNA 的可视化检测。基于多重信号放大策略,t-DNA 的检测具有较低的检测限为 0.28 fM 和较宽的线性范围从 0.5 fM 到 50 nM。该方法具有检测多种核酸和生物标志物的潜力。