增强型量子点固态电致化学发光研究及其生物分析新方法

Quantum dots (QDs) as a new kind of electrogenerated chemiluminescence (ECL) emitters, in comparison with conventional molecular emitters, own several distinctive merits like wide resources, versatile types, facile preparation, easy surface functionalization, convenience to bind with biological macromolecules, controllable multi-wavelength emitting and etc. However, the proposed ECL mechanisms of QDs are not perfect, and there still exist some questions and new phenomena unresolved during the ECL experiments. In aqueous solution, the QDs diffusion rate is very low, and the electrolytes used could lead to the aggregation of QDs, which limits the investigation and application of QDs ECL. Meanwhile, the ECL intensity of QDs is weak, while the initiated potential is quite high. This proposal plans to carry out the following tasks:(1) Synthesize some new QDs; (2) Immobilize those QDs onto the electrode surfaces to investigate their ECL in aqueous solution to further demonstrate the ECL mechanism and establish QDs’ ECL database for selecting QDs with high ECL efficiency and low electrochemical initial potential; (3) Assembly the QDs with multidimensional micro-nano structures to improve the film’s conductivity and the diffusion of the co-reactant in the film, and the synergetic effect to develop enhanced solid-state ECL platforms; (4) Modify the QDs with orientated biomolecules to develop new biosensing systems and approaches for analytical applications in clinical diagnostics and life analysis.

量子点 （QDs）作为一种新兴的电致化学发光体，具有来源广泛，种类繁多，制备方便，易于表面官能化，便于结合生物大分子，多波段发光可控等传统发光试剂无法媲美的优点。但QDs电致化学发光（ECL）机制尚不成熟，ECL过程中仍存在大量的实验新现象，新问题亟待解决；其 ECL强度相对较弱，发光激发电位偏高等不足亟待改善。而液相ECL中，QDs扩散迁移速度慢，受支持电解质影响易团聚等，不利于ECL实验的开展。为此，本项目拟通过制备多种类型QDs，并固定于电极表面，在水相中研究其固态ECL行为，进一步揭示QDs的ECL机理， 建立QDs ECL数据库，筛选ECL强度大的发光体；通过构建QDs的多维纳、微复合结构，提高QDs薄膜的导电性，改善共反应试剂在薄膜内的扩散传输，发挥协同效应发展增强型ECL传感界面；进而组装取向性生物大分子，发展生物分析新体系、新方法。

电化学发光分析法具有灵敏度高、电化学电位可控、动态范围宽、设备简易以及抗干扰能量强等特点，广泛应用于免疫分析、环境检测、食品分析以及生物试剂的检测。本项目中，我们构建了多种新型电化学发光生物传感器。同时，我们还合成了如荧光碳点、贵金属纳米簇、量子点等发光材料，建立了高灵敏度、高选择性的荧光传感体系。根据研究计划，我们已经顺利完成了全部相关的研究工作，并取得了较好的研究成果。研究成果分别发表在 Anal. Chem., Biosens. Bioelectron., Analyst, RSC Adv.等国际知名期刊上。在 SCI刊物上发表或被接受发表的研究论文12篇，其中影响因子大于 3.0的论文7篇。培养硕士毕业生1名。