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功能化氧化石墨烯原位引发开环聚合用于高灵敏度检测细胞角蛋白 19 片段。

Functionalized graphene oxide in situ initiated ring-opening polymerization for highly sensitive sensing of cytokeratin-19 fragment.

机构信息

Pharmacy College, Henan University of Chinese Medicine, Zhengzhou, 450046, People's Republic of China.

Henan Key Laboratory of TCM Syndrome and Prescription in Signaling, Henan International Joint Laboratory of TCM Syndrome and Prescription in Signaling, Academy of Chinese Medical Sciences, Henan University of Chinese Medicine, Zhengzhou, 450046, People's Republic of China.

出版信息

Mikrochim Acta. 2021 Mar 12;188(4):123. doi: 10.1007/s00604-021-04780-7.

DOI:10.1007/s00604-021-04780-7
PMID:33712913
Abstract

Improving the sensitivity of detection is crucial to monitor biomarker, assess toxicity, and track therapeutic agent. Herein, a sensitivity-improved immunosensor is reported for the first time via functionalized graphene oxide (GO) and a "grafting-to" ring-opening polymerization (ROP) dual signal amplification strategy. Through the ROP reaction using 2-[(4-ferrocenylbutoxy)methyl] oxirane (FcEpo) as the monomer, lots of electroactive tags are linked in situ from multiple initiation sites on the GO surface modified with ethanol amine (GO-ETA), thereby achieving high sensitivity even in the case of trace amounts of tumor markers. The utmost important factor for achieving this high sensitivity is to select functionalized GO as the initiator that contains a large number of repeated hydroxyl functional groups so as to trigger additional ROP reaction. Under the optimal conditions, the high sensitivity and applicability is demonstrated by the use of GO-ETA-mediated ROP-based immunosensor to detect non-small cell lung cancer (NSCLC)-specific biomarker down to 72.58 ag/mL (equivalent to ~6 molecules in a 5 μL sample). Furthermore, the satisfactory results for the determination of biomarkers in clinical serum samples highlighted that this immunosensor holds a huge potential in practical clinical application. This work described an electrochemical immunosensor for ultrasensitive detection of CYFRA 21-1 via the functionalized graphene oxide (GO) and a "grafting-to" ring-opening polymerization (ROP) dual signal amplification strategy, which hold the merits of high sensitivity, applicability, selectivity, efficiency, easy operation and environmental friendliness.

摘要

提高检测灵敏度对于监测生物标志物、评估毒性和跟踪治疗剂至关重要。本文首次报道了一种通过功能化氧化石墨烯(GO)和“接枝到”开环聚合(ROP)双重信号放大策略提高灵敏度的免疫传感器。通过使用 2-[(4- 二茂铁基丁氧基)甲基]环氧乙烷(FcEpo)作为单体的 ROP 反应,大量的电活性标记物从 GO 表面上的多个引发点原位连接,GO 表面经乙醇胺(GO-ETA)修饰,从而实现了即使在痕量肿瘤标志物的情况下也具有高灵敏度。实现这种高灵敏度的最重要因素是选择功能化 GO 作为引发剂,其中包含大量重复的羟基官能团,从而引发额外的 ROP 反应。在最佳条件下,通过使用 GO-ETA 介导的基于 ROP 的免疫传感器检测非小细胞肺癌(NSCLC)特异性生物标志物,灵敏度高达 72.58 ag/mL(相当于 5 μL 样品中约 6 个分子)。此外,该免疫传感器在临床血清样本中对生物标志物的测定结果令人满意,这表明它在实际临床应用中具有巨大的潜力。本工作描述了一种基于功能化氧化石墨烯(GO)和“接枝到”开环聚合(ROP)双重信号放大策略的电化学免疫传感器,用于超灵敏检测 CYFRA 21-1,具有灵敏度高、适用性强、选择性好、效率高、操作简单、环保等优点。

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