基于核酸-光/电传导界面的均相电致化学发光生物传感及细胞成像研究

In this project, ultrasensitive homogeneous electrochemiluminescence biosensing and cell imaging will be developed based on DNA-photic/electric transduce interface. According to various principle of electrochemiluminescent reaction, inorganic and organic single-strand DNA-sensitive membranes are fabricated, respectively, using Layered 2D nanomaterials and conductive block copolymers to construct affinity-mediated homogeneous electrochemiluminescence biosensing electrodes, which enhanced the discrimination ability of electrode over single-stranded DNA and double-stranded DNA. Then electrochemiluminescent single-strand DNA-sensitive organic membrane with low excitation potential and fast electrochemiluminescent response is constructed through the internal in-situ fabrication of nanoclusters or conjugated small molecules as electrochemiluminescent luminophors. Then, ultrasensitive and single-molecular homogeneous biosensing method will be developed with the aid of novel homogeneous signal amplification strategies. According to the photovoltaic principle of metalloid semiconductors, an enhancing mechanism of photic-activated electric-photic signal feedback oscillation will be developed to construct dual-electrode homogeneous electrochemiluminescence sandwich cell imaging strategy, resulting high resolution, ultrasensitive, and single-cell homogeneous electrochemiluminescence imaging array. This project is of great scientific importance, and innovative research results are expected.

本项目拟开展基于核酸-光/电传导界面的超灵敏均相电致化学发光生物传感及细胞成像研究。根据不同的电致化学发光原理，利用层状二维纳米材料与导电嵌段共聚物，开发单链DNA无机/有机敏感膜，构建亲和力介导均相电致化学发光生物传感电极，提升电极对单/双链DNA的特异性区分能力。探索电致化学发光纳米簇与共轭小分子发光体的原位制备技术，构筑响应速度快、激发电位低的共反应式电致化学发光单链DNA有机敏感膜。设计均相电致化学发光信号放大新策略，实现超灵敏、单分子均相电致化学发光生物传感。根据非金属半导体光伏原理，研究探索光信号-激活电信号-光信号反馈振荡增强新机制，发展双电极夹心式均相电致化学发光细胞成像新策略，为实现超灵敏、单细胞、阵列化、高空间分辨的均相电致化学发光成像分析奠定理论与技术基础，具有重要的科学意义和研究价值，有望获得一系列具有特色的创新性研究成果。

发展高灵敏、特异性均相电致化学发光生物传感技术，对于重大疾病的临床早期诊断、治疗具有十分重要的研究意义。本项目开展了高灵敏均相电致化学发光生物传感新方法及其在重大疾病生物标志物分析中的应用研究。提出了自催化原位生成共反应试剂，增强电致化学发光(ECL)信号新策略(Anal. Chem. 2021, 93, 36, 12441–12446)；首次实现了生物燃料电池（BFC）驱动电致化学发光，构建了BFC-ECL系统(Anal. Chem. 2021, 93, 34, 11745–11750)；基于聚集诱导发光材料作为ECL发光试剂，建立了博来霉素的ECL传感新方法(Anal. Chem. 2020, 92, 17, 11747–11754)；建立了有机磷农药的均相ECL检测新方法(J. Agric. Food Chem. 2021, 69, 6087−6095)；制备了固态ECL电极LI-CdS-G@GC，实现了碘离子的ECL灵敏检测(Sens. Actuators B Chem. 2021, 337, 129766)；基于均相电化学、光致电化学、生物燃料电池传感策略，建立了单核苷酸多态性、甲基转移酶、外泌体、microRNA等高灵敏、高选择性传感平台。“基于核酸信号放大的疾病标志物均相传感新方法研究”（ZR2019-2-6-R01）获山东省自然科学二等奖。 . 在国家自然科学基金的资助下，发表 SCI 收录论文50篇。培养了9名硕士专业人才。