电化学发光
化学
铱
生物结合
检出限
生物传感器
组合化学
单体
分子内力
计时安培法
光化学
电化学
聚合物
色谱法
有机化学
物理化学
循环伏安法
催化作用
生物化学
电极
作者
Lei Yang,Xu Sun,Dong Wei,Huangxian Ju,Yu Du,Hongmin Ma,Qin Wei
标识
DOI:10.1021/acs.analchem.0c03877
摘要
An intriguing aggregation-induced electrochemiluminescence (AIECL) bioconjugate was fabricated by encapsulating fac-tris(2-phenylpyridine)iridium(III) complexes [Ir(ppy)3] in the apoferritin (apoFt) cavity for biosensing application. Based on the unique pH-dependent disassembly/reassembly characteristic of apoFt, approximately 44.3 molecules of Ir(ppy)3 aggregated in the single cavity through both intermolecular π–π-stacking interactions and hydrogen bonds that efficiently restricted the intramolecular motions to trigger the AIECL effect. Compared to monomers, Ir(ppy)3 aggregates performed 5.3-fold-enhanced ECL emission using tri-n-propylamine (TPrA) as a coreactant. The fabricated Ir(ppy)3@apoFt bioconjugate was flexibly labeled with a detection antibody to act as a transducer for the immunosensor construction. To further catalyze the ECL reaction between the reductive TPrA• and the oxidative Ir(ppy)3+• radicals, a conductive and electroactive substrate of Fe2N and gold nanoparticle-codecorated reduced graphene oxide (Fe2N/rGO/Au) was established to incubate the capture antibody. Therefore, a “signal on” immunosensor was developed for sensitive assay of cytokeratin 19 fragment 21–1 (CYFRA 21–1), in which good linearity ranging from 1 pg/mL to 50 ng/mL with a low detection limit of 0.43 pg/mL (S/N = 3) was obtained. This study shares with an inspiration of using apoFt to design iridium(III)-based AIECL emitters, which will expand more possibilities of organic iridium(III) complexes in establishing innovative ECL immunoassays.
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