基于纳米多孔膜界面的电化学发光测量与成像

Electrochemiluminescence (also called as electrogenerated chemiluminescence, ECL) refers to chemical luminescence generated by electrochemistry, which has apparent advantages in terms of low background interference, high signal-to-noise ratio, good spatiotemporal resolution, high sensitivity and so on. One of key scientific and technical issues is to design the microstructure of electrode surface to control the electron transfer and/or mass transport of electroluminophore, co-reactant and target molecule, thus increasing the selectivity, sensitivity, anti-fouling/anti-interference capacity and spatiotemporal resolution. This project aims at preparing silica nanochannel membrane (SNM) consisting of highly ordered and vertically oriented channels in both electrode-supported and free-standing formats, with which various microstructured electrode surfaces will be fabricated. The main objective is to develop precise ECL analysis and imaging method and technique with high selectivity, sensitivity, anti-fouling/anti-interference capacity and high spatiotemporal resolution. Thanks to uniform nanochannels with precise selectivity at the molecular level, the electrodes are expected to accomplish the analysis of dopamine in complex samples. Based on the one-dimensional confinement effect on the mass transport of electroluminophore, co-reactant and target molecule inside vertical nanochannels, the anti-fouling/anti-interference ability, sensitivity and spatiotemporal resolution at the micro-scale are expected to be highly improved. The ultimate goal is to measure and image dopamine released by PC-12 cell, thus understanding the spatial distribution of release sites on the cell.

电化学发光(或电致化学发光，简称ECL)是电化学和化学发光相结合的一种分析方法，具有背景低、信噪比高、优良的时空可控性和高灵敏度等优势。构建电极表面微观结构，调控ECL探针、共反应剂及待测分子在微观界面的传荷和传质过程，从而提高电极表界面的选择性、抗污染/抗干扰能力和ECL分析的灵敏度和时空分辨性能是ECL研究领域的重要科学问题之一。本项目拟以孔道高度有序分布且垂直于表面的二氧化硅薄膜(SNM)为基础，构建不同电极微观结构，发展高选择性、抗污染/抗干扰、高灵敏和高时空分辨的精准ECL测量和成像方法、技术；利用SNM纳米孔道的分子选择性，实现复杂样品中多巴胺的ECL测量；基于SNM纳米孔道对ECL探针、共反应剂和待测分子的空间限域效应，提高微体系中ECL测量和成像的抗污染能力、灵敏度和空间分辨能力；开展大鼠肾上腺嗜铬细胞瘤细胞胞吐释出多巴胺的ECL测量与成像。

电化学发光(简称ECL)是电化学反应触发的发光现象，具有背景低、灵敏度高等优势。提高电极界面的选择性、抗污染/抗干扰能力、分析灵敏度和时空分辨率是ECL分析研究领域的重要科学问题之一。本项目以有序多孔膜修饰电极表面，调控探针、共反应剂及待测分子在微观界面的传荷和传质过程，实现了复杂体系中的电化学和ECL分析、细胞及细胞外泄物的ECL成像分析，主要成果包括：（1）发展了ECL显微成像以及ECL自干涉光谱技术，突破了ECL纵向空间分辨测量的技术局限，实现了发光分子定位识别，解析了ECL的表面限域和空间延展机制；（2）以高度有序的二氧化硅纳米孔薄膜修饰电极表面，发展了高选择性、抗污染/抗干扰的电化学分析方法，建立了高灵敏和高时空分辨ECL测量和成像方法，并解析了界面传质和传荷反应机制；（3）通过电极表面ECL信号的空间选择性调控，实现了细胞-基质黏着蛋白和细胞-细胞间链接蛋白的顺次成像分析，揭示了化学微环境在调控细胞黏附行为中的重要作用以及细胞集体迁移的动态机制，实现了大鼠肾上腺嗜铬细胞瘤细胞胞吐释出多巴胺的固态ECL测量与成像。项目执行期内共发表论文31篇，包括4篇Angew. Chem., 2篇JACS和5篇Anal. Chem., 获得授权中国发明专利2项。