Electrochemically Mediated Surface-Initiated de Novo Growth of Polymers for Amplified Electrochemical Detection of DNA
Electrochemically Mediated Surface-Initiated de Novo Growth of Polymers for Amplified Electrochemical Detection of DNA
复制标题
电化学介导的表面引发聚合物从头生长，用于放大 DNA 电化学检测
DOI：
10.1021/acs.analchem.7b02039
复制
发表时间：
2017-09-05
影响因子：
7.4
通讯作者：
Zhang, Xueji
中科院分区：
文献类型：
--
作者：
Hu, Qiong;Wang, Qiangwei;Zhang, Xueji
在生物分析应用中，开发不涉及任何复杂纳米材料或酶的方便有效的信号放大策略是非常重要的。在这项工作中，我们报道了使用电化学介导的表面引发原子转移自由基聚合（si - erap）作为一种基于聚合物从头生长（dnGOPs）的电化学检测DNA的新型扩增策略。具体来说，固定化肽核酸（PNA）探针捕获目标DNA （tDNA）提供了高密度的磷酸基团，随后通过磷酸- zr4 +-羧酸盐化学将ATRP引发剂附着在电极表面，然后通过si - eattp重新生长电活性聚合物。长聚合链的从头生长使许多电活性探针的标记成为可能，这反过来又大大提高了电化学响应。此外，它还克服了纳米材料或预成型聚合物的缓慢动力学和耦合效率差的问题，并且在控制信号放大程度方面具有足够的灵活性和简单性。在最佳条件下，它可以在0.1 fM ~ 0.1 nM的宽线性范围内（R-2 = 0.996）对tDNA进行高灵敏度和选择性检测，检测限低至0.072 fM。与未扩增的方法相比，DNA检测灵敏度提高了1.2 × 10(6)倍以上。基于dngps的信号放大策略具有简单、高效、低成本的优点，在生物分析领域具有很大的应用潜力，可用于生物分子的灵敏检测。
The development of convenient and efficient strategies without involving any complex nanomaterials or enzymes for signal amplification is of great importance in bioanalytical applications. In this work, we report the use of electrochemically mediated surface-initiated atom transfer radical polymerization (SI-eATRP) as a novel amplification strategy based on the de novo growth of polymers (dnGOPs) for the electrochemical detection of DNA. Specifically, the capture of target DNA (tDNA) by the immobilized peptide nucleic acid (PNA) probes provides a high density of phosphate groups for the subsequent attachment of ATRP initiators onto the electrode surface by means of the phosphate-Zr4+-carboxylate chemistry, followed by the de novo growth of electroactive polymer via the SI-eATRP. De novo growth of long polymeric chains enables the labeling of numerous electroactive probes, which in turn greatly improves the electrochemical response. Moreover, it circumvents the slow kinetics and poor coupling efficiency encountered when nanomaterials or preformed polymers are used and features sufficient flexibility and simplicity in controlling the degree of signal amplification. Under optimal conditions, it, allows a highly sensitive and selective detection of tDNA within a broad linear range from 0.1 fM to 0.1 nM (R-2 = 0.996), with the detection limit down to 0.072 fM. Compared with the unamplified method, more than 1.2 X 10(6)-fold sensitivity improvement in DNA detection can be achieved. By virtue of its simplicity, high efficiency, and cost-effectiveness, the proposed dnGOPs-based signal amplification strategy holds great potential in bioanalytical applications for the sensitive detection of biological molecules.