高量子产率电致化学发光金纳米团簇探针的设计及其在生命分析中的应用

As a novel electrochemiluminescence (ECL) emitter, quantum dots (QDs) own several distinctive merits like high luminescence efficiency, good stability, size/surface-trap controlled luminescence and facile surface functionalization modification. In recent years, QD ECL systems have been attracted increasing attentions. However, most of the QD luminophor species, such as the cadimium-containing QDs, are environmental toxicity and poor biocompatibility, which limit their practical applications, especially in biosystems. Thus, developing environment-friendly ECL species is imperative. Gold nanocluster (AuNC) has become a promising material due to its fantastic characteristics, such as good biocompatibility, outstanding catalytic performance, and unusual photophysical properties. However, due to the restrictions of weak ECL intensity, low quantum yield and unclear mechanism, the ECL study based on AuNCs, especially in aqueous solution systems has been reported rarely. Aiming at these problems above, this project proposes to accurately prepare a series of functionalized AuNCs by nanotechnology, and then systematically study on the affecting factors of the ECL properties of the AuNCs and reveal the luminescence mechanism. Based on the revealing influence factors and ECL mechanism, a series of AuNCs, ECL probes with high performance can be screened, and apply to develop novel ECL methods for life analysis. This project combines nanotechnology, molecular biology technique, clinical detection technology and sensing technology, and shows outstanding academic innovation value and great significance in its clinical application.

在电致化学发光（ECL）生物分析中，量子点作为一种新型ECL纳米发光体，具有发光效率高、光稳定性好、多波段发光可控及表面修饰功能化等优点。但目前大部分的量子点发光体本身的毒性极大地限制了其在生物分析中的应用。因此，发展环境友好型ECL发光体用于生命分析具有重要意义。金纳米团簇作为一种新型无毒的荧光纳米材料由于其优良的光电性能得到了人们的广泛关注。然而由于其ECL强度小、量子产率低、发光机制不清楚等问题的限制，使其在ECL领域的研究，尤其是在水相中的ECL研究鲜有报道。针对以上问题，本项目拟通过可控纳米制备技术精准制备一系列功能化的金纳米团簇，深入探讨其ECL性能影响因素并揭示其发光机制，筛选一系列高性能金纳米团簇ECL探针，并将其应用于发展生命分析新体系、新方法。本项目有机结合了纳米技术、分子生物学技术、生物传感技术和临床检测技术，具有突出的学术创新性和临床医学应用价值。

电化学发光具有背景信号低、灵敏度高、可控、设备简单及适用性广等优点，在生命分析领域具有广泛的应用前景。然而，该领域尚存在量子产率低、发光机理研究尚不成熟等基础科学问题，深入探究电化学发光探针发光机制以及本质机理问题具有重要意义。本课题紧密围绕上述核心问题，从探究水相中AuNC ECL探针发光机制以及ECL本质机理问题入手，提出了纳米尺度价态调控、电催化和聚集诱导双增强等ECL调控的特殊机制，制备了高性能AuNC ECL纳米探针；针对传感器的应用需求，在传感材料、界面设计、共反应体系等方面提出创新策略，建立了基于其调控机制介导的ECL分析平台、免疫金簇“二合一”ECL传感器、分离式ECL检测平台及共反应剂介导的低电位ECL分析平台等检测方法，为合理设计ECL纳米探针及生物传感提供了新机制和新方法。