基于聚集诱导发光分子的免标记癌胚抗原生物传感新方法研究  

Aggregation Induced Emission Fluorogen-based Label-free Biosensor for Highly Sensitive Detection of Carcinoembryonic Antigen

作　　者：李海银[1] 常加富 吕文欣 李峰[1] LI Hai-Yin;CHANG Jia-Fu;LYU Wen-Xin;LI Feng(College of Chemistry and Pharmaceutical Sciences,Qingdao Agricultural University,Qingdao 266109,China)

机构地区：[1]青岛农业大学化学与药学院,青岛266109

出　　处：《分析化学》2020年第10期1325-1333,共9页Chinese Journal of Analytical Chemistry

基　　金：国家自然科学基金项目(Nos.21605093,21775082)资助。

摘　　要：基于目标物诱导酶循环放大反应,借助Hemin/G-四链体对L-半胱氨酸(L-Cys)的催化氧化作用,构建了聚集诱导发光(AIE)分子介导的荧光生物传感器,实现了癌胚抗原(CEA)的免标记、高灵敏检测。以弱发光的马来酰亚胺功能化四苯乙烯(TPE-M)作为信号源,其可与L-Cys反应,使荧光增强。当目标物存在时,CEA引发聚合酶/内切酶辅助的循环放大反应,原位生成大量Hemin/G-四链体,其催化氧化L-Cys变成胱氨酸(Cys-cys),阻止L-Cys与TPE-M反应,致使传感体系的荧光强度降低;当CEA不存在时,L-Cys可继续与TPE-M反应,体系荧光信号增强。基于体系中荧光信号的变化,即可实现CEA的免标记、高灵敏检测,检出限为0.033 fmol/L。本传感器具有优异的选择性、稳定性与抗干扰能力,为生物样品中CEA的灵敏与准确检测提供了新方法。A highly sensitive and label-free fluorescence carcinoembryonic antigen(CEA)biosensor was developed via target-triggered enzymatic recycling amplification reaction.In this strategy,aggregation induced emission fluorogen(AIEgen)TPE-M was chosen as a signal reporter to enhance the detection efficiency,as well as L-cysteine(L-cys)was utilized as a reactant to control over the fluorescence intensity due to its distinct capability of reacting with TPE-M and hemin/G-quadruplex.CEA triggered the in-situ generation of abundant hemin/G-quadruplex through polymerase/nicking enzyme-assisted recycling amplification,and the in-situ generated hemin/G-quadruplex catalyzed the destruction of L-cys.With L-cys consuming,a significantly decreased fluorescence was observed,demonstrating that the fluorescence intensity was relied on CEA amount.As a consequence,a facile,precise and sensitive strategy for CEA assay was readily realized.Furthermore,the detection limit was 0.033 fmol/L(S/N=3).The developed AIEgen-based biosensor provided a new method for sensitive and reliable detection of CEA in biological liquids,displaying a significant promise for CEA-related disease diagnosis.

关 键 词：聚集诱导发光 免标记 癌胚抗原 荧光 生物传感器 

分 类 号：O657.3[理学—分析化学] R730.43[理学—化学]