Gou Xiaodan, Zhang Yiwen, Xing Zejing, Ma Cheng, Mao Changjie, Zhu Jun-Jie
State Key Laboratory of Analytical Chemistry for Life Science School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 P. R. China
School of Chemistry and Chemical Engineering, Anhui University Hefei 230601 P. R. China
Chem Sci. 2023 Aug 2;14(34):9074-9085. doi: 10.1039/d3sc02298f. eCollection 2023 Aug 30.
visualization of local electrochemical reactions provides mechanical insights into the dynamic transport of interfacial charge and reactant/product. Electrochemiluminescence is a crossover technique that quantitatively determines Faraday current and mass transport in a straightforward manner. However, the sensitivity is hindered by the low collision efficiency of radicals and side reactions at high voltage. Here, we report a site-selective heat boosting electrochemiluminescence microscopy. By generating a micron-scale heat point at the electrode-solution interface, we achieved an enhancement of luminescence intensity up to 63 times, along with an advance of 0.2 V in applied voltage. Experimental results and finite element simulation demonstrate that the fundamental reasons are accelerated reaction rate and thermal convection a photothermal effect. The concentrated electrochemiluminescence not only boosts the contrast of single cells by 20.54 times but also enables the site-selective cell-by-cell analysis of the heterogeneous membrane protein abundance. This electrochemical visualization method has great potential in the highly sensitive and selective analysis of local electron transfer events.
局部电化学反应的可视化提供了对界面电荷和反应物/产物动态传输的力学见解。电化学发光是一种交叉技术,能够以直接的方式定量测定法拉第电流和质量传输。然而,自由基的低碰撞效率和高压下的副反应阻碍了其灵敏度。在此,我们报告了一种位点选择性热增强电化学发光显微镜。通过在电极-溶液界面产生微米级热点,我们实现了发光强度增强高达63倍,同时施加电压提前了0.2 V。实验结果和有限元模拟表明,其根本原因是反应速率加快和热对流——一种光热效应。集中的电化学发光不仅将单细胞的对比度提高了20.54倍,还能够对异质膜蛋白丰度进行逐个细胞的位点选择性分析。这种电化学可视化方法在局部电子转移事件的高灵敏度和选择性分析方面具有巨大潜力。