Electrochemical CYFRA21-1 DNA sensor with PCR-like sensitivity based on AgNPs and cascade polymerization
Electrochemical CYFRA21-1 DNA sensor with PCR-like sensitivity based on AgNPs and cascade polymerization
复制标题
DOI：
10.1007/s00216-020-02652-2
复制
发表时间：
2020-04
影响因子：
4.3
通讯作者：
Jinge Li;Liying Zhao;Dongxiao Wen;Xiaofei Li;Huaixia Yang;Dazhong Wang;J. Kong
中科院分区：
文献类型：
--
作者：
Jinge Li;Liying Zhao;Dongxiao Wen;Xiaofei Li;Huaixia Yang;Dazhong Wang;J. Kong
本文提出了一种基于电化学介导的原子转移自由基聚合（e-ATRP）和表面引发的可逆加成-破碎链转移聚合（SI-RAFT）级联聚合和AgNP沉积的CYFRA21-1 DNA （tDNA）检测新方法。首先，通过Au-S键将肽核酸（PNA）探针捕获在金电极上，用于特异性识别tDNA。杂交后，PNA/DNA链通过鉴定的羧酸- zr4 +-磷酸化学为后续的ATRP引发剂提供高密度磷酸基团。然后，通过e-ATRP反应成功地从DNA上接枝了大量单体。之后，SI-RAFT链转移剂与甲基丙烯酸（MAA）通过公认的羧酸- zr4 +-羧酸化学连接。随后，通过SI-RAFT，得到的聚合物引入了大量的醛基团，这些醛基团可以通过银镜像反应在tDNA上沉积许多AgNPs，引起电化学信号的显著放大。在最佳条件下，该方法的检出限较低，为0.487 aM。此外，该方法使我们能够在类似pcr的水平上检测DNA，并且在血清存在下显示出高选择性和强抗干扰能力。提示这种新的传感信号放大技术在非小细胞肺癌（NSCLC）的早期诊断中具有良好的应用潜力。基于e-ATRP和SI-RAFT信号放大技术的CYFRA21-1 DNA电化学检测原理。
In this work, a new method of CYFRA21-1 DNA (tDNA) detection based on electrochemically mediated atom transfer radical polymerization (e-ATRP) and surface-initiated reversible addition-fragmentation chain transfer polymerization (SI-RAFT) cascade polymerization and AgNP deposition is proposed. Firstly, the peptide nucleic acid (PNA) probe is captured on a gold electrode by Au-S bonds for specific recognition of tDNA. After hybridization, PNA/DNA strands provide high-density phosphate groups for the subsequent ATRP initiator by the identified carboxylate-Zr4+-phosphate chemistry. Then, a large number of monomers are successfully grafted from the DNA through the e-ATRP reaction. After that, the chain transfer agent of SI-RAFT and methacrylic acid (MAA) are connected by recognized carboxylate-Zr4+-carboxylate chemistry. Subsequently, through SI-RAFT, the resulting polymer introduces numerous aldehyde groups, which could deposit many AgNPs on tDNA through silver mirror reaction, causing significant amplification of the electrochemical signal. Under optimal conditions, this designed method exhibits a low detection limit of 0.487 aM. Moreover, the method enables us to detect DNA at the level of PCR-like and shows high selectivity and strong anti-interference ability in the presence of serum. It suggests that this new sensing signal amplification technology exhibits excellent potential of application in the early diagnosis of non-small cell lung cancer (NSCLC).Graphical abstractElectrochemical detection principle for CYFRA21-1 DNA based on e-ATRP and SI-RAFT signal amplification technology.