期刊
ANALYTICAL CHEMISTRY
卷 93, 期 50, 页码 16906-16914出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.1c04006
关键词
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资金
- Natural Science Foundation of Shandong Province [ZR2019BB007, ZR2020QB097]
- National Key Scientific Instrument and Equipment Development Project of China [21627809]
- Special Foundation for Taishan Scholar Professorship of Shandong Province [ts20130937]
- Innovation Team Project of Colleges and Universities in Jinan [2019GXRC027]
- Science and Technology Program of University of Jinan [XBS2106]
The self-assembly of iridium complexes in water-soluble nanocontainers using PEGylated apoferritin is crucial for fabricating ECL bioprobes. The encapsulation of iridium cores in PEG-apoHSF cavities allows for enhanced ECL behavior and potential applications in biosensing systems. Additionally, the developed immunosensor based on Ti3C2Tx/TiO2 hybrids exhibited amplified ECL responses for neuron-specific enolase detection.
Dynamic self-assembly of iridium complexes in water-soluble nanocontainers is an important bottom-up process for fabricating electrochemiluminescence (ECL) bioprobes. PEGylated apoferritin (PEG-apoHSF) as the host offers a confined space to alter and modify the self-assembly of trans-bis(2-phenylpyridine)-(acetylacetonate)iridium(III) [Ir(ppy)(2)(acac)] based on a pH-depend-ent depolymerization/reassembly pathway, allowing the formation of ECL-active iridium cores in PEG-apoHSF cavities (Ir@PEG-apoHSF). With an improved encapsulation ratio in PEG-apoHSF, the coreactant ECL behavior of the fabricated Ir@PEG-apoHSF nanodots with tri-n-propylamine (TPrA) was further demonstrated, exhibiting maximum ECL emission at 530 nm that was theoretically dominated by the band gap transition. The application of Ir@PEG-apoHSF as a bioprobe in a signal-on ECL immunosensing system was developed based on electroactive Ti3C2Tx MXenes/TiO2 nanosheet (Ti3C2Tx/TiO2) hybrids. Combining with the efficiently catalyzed electro-oxidation of TPrA and Ir(ppy)(2)(acac) by Ti3C2Tx/TiO2 hybrids, the developed immunosensor showed dramatically amplified ECL responses toward the target analyte of neuron-specific enolase (NSE). Under experimental conditions, linear quantification of NSE from 100 fg/mL to 50 ng/mL was well established by this assay, achieving a limit of detection (LOD) of 35 fg/mL. The results showcased the capability of PEGylated apoHSF to host and stabilize water-insoluble iridium complexes as ECL emitters for aqueous biosensing and immunoassays.
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