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Boron Carbon Nitride Nanosheets-Ru Nanocomposite Self-Enhancement Electrochemiluminescence Emitter with a Three-Dimensional DNA Network Structure as a Signal Amplifier for Ultrasensitive Detection of TK1 mRNA
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-08-02 , DOI: 10.1021/acs.analchem.2c02110
Jicui Hu 1 , Yue Zhang 1 , Yaqin Chai 1 , Ruo Yuan 1
Affiliation  

In this study, a neoteric self-enhanced nanocomposite boron carbon nitride nanosheets (BCN NSs)-Ru obtained by chemical crosslinking between boron carbon nitride nanosheets (BCN NSs) and tris (4,4′-dicarboxylicacid-2,2′-bipyridyl) ruthenium(II) dichloride (Ru(dcbpy)3Cl2) was used as an emitter to build an electrochemiluminescence (ECL) biosensor for ultrasensitive detection of the cancer marker human thymidine kinase 1 (TK1) mRNA. Importantly, the self-enhanced BCN NSs-Ru could exhibit strong ECL emission because boron radicals and amine groups derived from BCN NSs could significantly enhance the ECL response of Ru(dcbpy)3Cl2, which avoided the defects of the long electron transfer path and large energy loss between the emitter and coreactant in the traditional coreaction ECL system. Impressively, in the presence of target TK1 mRNA, three-dimensional DNA network structure-labeled numerous ferrocene probes could be assembled to quickly quench the ECL signal of BCN NSs-Ru, resulting in improved biosensor sensitivity. The obtained “on–off” biosensor showed excellent stability and high sensitivity with a detection limit of 32.3 aM. In general, the developed strategy provided a new biosensing way for ultrasensitive detection of biomolecules in early disease diagnosis.

中文翻译:

具有三维DNA网络结构的氮化硼纳米片-钌纳米复合自增强电化学发光体作为信号放大器用于超灵敏检测TK1 mRNA

在这项研究中,通过氮化碳纳米片(BCN NSs)和三(4,4'-二羧酸-2,2'-联吡啶)之间的化学交联获得了一种新的自增强纳米复合氮化碳纳米片(BCN NSs)-Ru使用二氯化钌 (II) (Ru(dcbpy) 3 Cl 2 ) 作为发射器构建电化学发光 (ECL) 生物传感器,用于超灵敏检测癌症标志物人胸苷激酶 1 (TK1) mRNA。重要的是,自增强 BCN NSs-Ru 可以表现出强烈的 ECL 发射,因为源自 BCN NSs 的硼自由基和胺基可以显着增强 Ru(dcbpy) 3 Cl 2的 ECL 响应,避免了传统共反应ECL系统中发射极与共反应物之间电子传输路径长、能量损失大的缺陷。令人印象深刻的是,在存在目标 TK1 mRNA 的情况下,可以组装三维 DNA 网络结构标记的大量二茂铁探针,以快速淬灭 BCN NSs-Ru 的 ECL 信号,从而提高生物传感器的灵敏度。获得的“开-关”生物传感器表现出优异的稳定性和高灵敏度,检测限为 32.3 aM。总体而言,所开发的策略为早期疾病诊断中生物分子的超灵敏检测提供了一种新的生物传感方式。
更新日期:2022-08-02
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