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含氟引发剂通过原子转移自由基聚合实现肺癌 DNA 的超灵敏荧光检测。

F-containing initiatior for ultrasensitive fluorescent detection of lung cancer DNA via atom transfer radical polymerization.

机构信息

Pharmacy College, Henan University of Chinese Medicine, Zhengzhou, 450008, PR China.

School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094, PR China.

出版信息

Anal Chim Acta. 2020 Jan 15;1094:99-105. doi: 10.1016/j.aca.2019.09.080. Epub 2019 Oct 4.

DOI:10.1016/j.aca.2019.09.080
PMID:31761052
Abstract

An ultrasensitive fluorescence method for early diagnosis of lung cancer via Nafion-initiated atom transfer radical polymerization (ATRP) is reported, in this paper. In the proposed method, thiolated peptide nucleic acid (PNA) is modified to amino magnetic beads (MBs) via a cross-linking agent to specifically capture target DNA (tDNA), and the initiator (Nafion) of ATRP is attached to PNA/DNA heteroduplexes based on the phosphate groups of the tDNA and sulfonate groups of Nafion via phosphate-Zr-sulfonate chemistry. Nafion as a macroinitiator of ATRP possesses multiple C-F active sites to initiate polymerization, and numerous polymeric chains that significantly amplify the fluorescent signal are formed. Under optimal conditions, a good linear relationship is obtained in the range of 0.1 nM-0.1 fM with correlation coefficients of 0.9975, and the detection limit is as low as 35.5 aM (∼214 molecules). The proposed strategy has several advantages of simplicity, cost-effectiveness, selectivity and sensitivity. More importantly, the anti-interference results demonstrate that the proposed Nafion-initiated ATRP strategy has great potential in bioanalytical applications.

摘要

本文报道了一种通过 Nafion 引发原子转移自由基聚合(ATRP)用于肺癌早期诊断的超灵敏荧光方法。在该方法中,巯基化肽核酸(PNA)通过交联剂修饰到氨基磁性珠(MBs)上,以特异性捕获靶 DNA(tDNA),并且 ATRP 的引发剂(Nafion)基于 tDNA 的磷酸基团和 Nafion 的磺酸盐基团通过磷酸锆-磺酸盐化学连接到 PNA/DNA 杂合体上。Nafion 作为 ATRP 的大分子引发剂具有多个 C-F 活性位点来引发聚合,并且形成了大量显著放大荧光信号的聚合链。在最佳条件下,在 0.1 nM-0.1 fM 的范围内获得了良好的线性关系,相关系数为 0.9975,检测限低至 35.5 aM(约 214 个分子)。该策略具有简单、经济高效、选择性和灵敏度高的优点。更重要的是,抗干扰结果表明,所提出的 Nafion 引发的 ATRP 策略在生物分析应用中具有很大的潜力。

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