基于共振能量转移的电致化学发光新体系及其生物传感机理

Electrogenerated chemiluminescence (ECL) is one of highly sensitive analytical technique. However, the development of ECL is severely restricted due to the lack of ECL systems. Therefore, it is urgently needed to explore new ECL systems and develop new ECL theory to meet the request of analytical chemistry for life science. The present project will investigate ECL resonance energy transfer between some traditional luminescent reagents, such as luminol, and some nanomaterials, such as quantum dots. With the deep investigation of the energy transfer phenomena, new ECL systems will be constructed and the biosensing mechanisms of new ECL systems will be studied. The nature of resonance energy transfer between quantum dots and ECL reagents will be revealed to construct energy donor/acceptor pairs. The electrochemical and the luminescent behaviors of nanomaterials and ECL reagents as well as the way of their interaction will be studied. The effect law of these parameters on energy transfer efficiency will be revealed, which can improve the energy transfer efficiency. The novel ECL systems will be established based on resonance energy transfer process. The mechanisms of new ECL systems will be studied, which can be used to elucidate the avenue and the mechanism of resonance energy transfer during the luminescent process. The basic theory of ECL will also be developed to guide the establishment of various energy transfer donor/acceptor pairs. The biosensing mechanism of new ECL systems will be studied, which can provide theoretical and technical supports for the construction of highly sensitive and highly selective ECL biosensors

电致化学发光是一种高灵敏的现代分析技术，但发光体系少的缺陷严重制约了该技术的发展，急需探索新的电致化学发光体系，发展新的发光理论，以适应快速发展的生命分析化学的需求。本项目拟研究鲁米诺等传统电致化学发光试剂与半导体量子点等纳米材料间的电致化学发光共振能量转移现象，在对该现象进行深层次探讨的基础上，建立新的电致化学发光体系并研究其生物传感机理。揭示量子点与发光试剂产生共振能量转移过程的本质，构建共振能量转移给体/受体对；研究纳米材料与发光试剂的光电性质及相互作用方式对共振能量转移过程的影响规律，提高共振能量转移效率；构建基于共振能量转移的电致化学发光新体系，对其发光机理进行研究，阐明发光过程的能量转移途径及形成机制，发展电致化学发光基础理论，指导建立多种类型的能量转移给体/受体对；研究电致化学发光新体系的生物传感机理，为构建高灵敏度、高选择性的电致化学发光生物传感器提供理论与技术支持。

电致化学发光是一种高灵敏的现代分析技术，但发光体系少的缺陷严重制约了该技术的发展，急需探索新的电致化学发光体系，发展新的发光理论，以构建具有高灵敏度和高选择性的电致化学发光生物传感器。本项目探讨了半导体量子点等新型纳米材料与鲁米诺等传统发光试剂间的相互作用规律，发展了电致化学发光共振能量转移理论，构建了多种基于共振能量转移的电致化学发光新体系；系统研究了纳米材料参与的电致化学发光过程和机理，丰富了电致化学发光基础理论和研究内容，建立了新的电致化学发光体系，扩展了电致化学发光的应用范围。主要研究成果有：（1）揭示了鲁米诺、联吡啶钌和光泽精等传统发光试剂与半导体量子点和石墨烯等纳米材料间存在共振能量转移现象，据此建立了多种电致化学发光共振能量转移体系，构建了可用于灵敏检测三磷酸腺苷、溶菌酶、细胞色素c等物质的生物传感器，并提出了基于共振能量转移的生物传感机理；（2）揭示了半导体量子点和黑磷量子点等新型纳米材料催化联吡啶钌等传统发光试剂的发光反应的机理，获得了增强的发光信号，提高了电致化学发光技术的检测灵敏度，据此构建了检测caspase-3、溶菌酶、多巴胺、细胞色素c等物质的生物传感器，并提出了相应的传感机理；（3）发现了硅量子点、碳点、Ag2Te量子点、黑磷纳米片、氧化锌纳米棒，以及一些纳米复合材料在共反应剂存在的条件下，可以产生强的电致化学发光信号，构建了多种新型的电致化学发光体系，提出了电致化学发光机理，在此基础上构建了可检测半胱氨酸、细胞色素c、DNA、邻苯二酚和过氧化氢等物质的基于纳米材料的电致化学发光传感器。本项目的研究结果揭示了纳米材料与发光试剂间的作用本质，为构建高灵敏度、高选择性的电致化学发光生物传感器提供了必要的理论与技术支持，具有较好的应用前景。