电位分辨的多色电化学发光纳米发光体及其分析应用研究

Recently, multi-color electrochemiluminescence (ECL) has attracted considerable interests, with the enticing prospect of simultaneously detecting multi-analytes, built-in self-calibration for a precise and quantitative analysis and constructing multi-color emitting devices, and so on. However, up to date, multi-color ECL has been limited to molecular system in organic solvents and could not satisfy the requirements of analytical applications. Thus, this project is to develop new strategies for the synthesis of novel potential-resolved multi-color ECL nanoluminophores. The surface properties, potential-resolved multi-color ECL properties, interactions between ECL reagents and nanoluminophores and related ECL mechanisms are to be studied. Furthermore, based on the design and assembly of the analytical nano-interfaces and nano-probes with multi ECL signals, novel ECL analytical methods are to be developed for simultaneously detecting multi-analytes or for a precise and quantitative analysis with built-in self-calibration. Meanwhile, based on the studies of interactions between nanoliminophores and analytes, sensing arrays are to be developed for multi-analytes analysis. This work opens a new research area of potential-resolved multi-color ECL nanoluminophores. It will further enrich our knowledge on the unique properties of multi-color ECL nanoluminophores. The new methods and strategies for precision analysis and multivariate analysis will be established, which is of great application potential in multivariate analysis at ultra-trace level in complex systems.

近年来，多色电化学发光由于具有多目标物的多元分析、内部校正的精准定量分析和构建多色光发射器件等潜在应用前景受到了重要的关注。然而，现有的相关研究仅限于有机溶剂中的分子体系，且基本处于基础研究阶段。本项目拟探索新的合成方法，制备新型在水相中具有电位分辨的多色电化学发光性质的纳米发光体；对其表面性质、电位分辨的多色电化学发光特性、电化学发光试剂和纳米发光体的相互作用以及电化学发光机理进行研究；构建新型具有多个电化学发光信号的纳米分析探针和界面，发展内部校正的精准分析方法和多目标物的多元分析方法；基于电位分辨的多色纳米发光体与分析物的直接相互作用，发展传感阵列用于多目标物的分析。此项工作开拓了电位分辨的多色电化学发光纳米发光体新的研究方向，将进一步丰富人们对多色纳米发光体特殊性质的认识，建立新型的精准分析和多元分析方法和策略，在复杂体系中多种低含量物质的分析中具有重要的应用潜力。

近年来，多色电化学发光（ECL）由于具有多目标物的多元分析、内部校正的精准定量分析和构建多色光发射器件等潜在应用前景受到了重要的关注。然而，现有的相关研究仅限于有机溶剂中的分子体系，且基本处于基础研究阶段。本项目提出选择高效的ECL试剂和高效、稳定的ECL纳米发光体，设计基于多种组装原理的电位分辨、多色ECL纳米发光体。基于此，本项目利用水热法、π-π堆积、水/油微乳法、酰胺化反应、原位生长等方法，设计与合成了一系列新型电位分辨的多色ECL纳米发光体，如纳米氧化石墨烯包裹的TiO2纳米颗粒、N-(4-氨基丁基)-N-乙基异鲁米诺（ABEI）修饰的g-C3N4纳米片、MOF-5包裹的CdS量子点、ABEI功能化石墨烯量子点、四(4-羧苯基)卟吩修饰的壳聚糖/Ru(bpy)32+/SiO2纳米颗粒、掺杂Ru(bpy)32+的SiO2纳米粒子修饰的g-C3N4纳米片等，研究了其大小、形貌、组成、表面状态、组装机理、ECL特性、发光体之间的相互作用以及催化特性等。基于上述纳米发光体独特的电位分辨和多色的ECL特性，针对急性心肌梗死标志物心肌肌钙蛋白I（cTnI）和miR-133a，发展了多种快速、简单、高灵敏度、高特异性和准确性的无标记比率型ECL分析方法。所提出的“差分型”和“三电位比率型”分析新原理，可以有效的消除系统误差，提高检测灵敏度、选择性和准确度。此项目开拓了电位分辨的多色电化学发光纳米发光体新的研究方向，进一步丰富了人们对多色纳米发光体特殊性质的认识，提出了分析新原理，建立了多种新型的精准分析方法和策略，在体外诊断中具有重要的应用潜力。