Long Yan-Min, Bao Lei, Zhao Jing-Ya, Zhang Zhi-Ling, Pang Dai-Wen
Key Laboratory of Analytical Chemistry for Biology and Medicine (Ministry of Education), College of Chemistry and Molecular Sciences, State Key Laboratory of Virology, and Wuhan Institute of Biotechnology, Wuhan University , Wuhan, 430072, P. R. China.
Anal Chem. 2014 Aug 5;86(15):7224-8. doi: 10.1021/ac502405p. Epub 2014 Jul 24.
Recently, research on carbon nanodots (C-dots), a new type of luminescent nanoparticles with superior optical properties, biocompatibility, and low cost, has been focused on exploring novel properties and structure-related mechanisms to extend their scope. Herein, electrochemiluminescence, a surface-sensitive tool, is used to probe the unrevealed property of carbon nanodots which is characterized by surface oxygen-containing groups. Together with chemiluminescence, carbon nanodots as the coreactants for the anodic electrochemiluminescence of Ru(bpy)3(2+) are demonstrated for the first time. During the anodic scan, the benzylic alcohol units on the C-dots surface are oxidized "homogeneously" by electrogenerated-Ru(bpy)3(3+) to form reductive radical intermediate, which further reduce Ru(bpy)3(3+) into Ru(bpy)3(2+)* that produces a strong ECL emission. This work has provided an insight into the ECL mechanism of the C-dots-involved system, which will be beneficial for in-depth understanding of some peculiar phenomena of C-dots, such as photocatalytic activity and redox properties. Moreover, because of the features of C-dots, the ECL system of Ru(bpy)3(2+)/C-dots is more promising in the bioanalysis.
最近,对碳纳米点(C点)的研究聚焦于探索其新特性及与结构相关的机制以拓展其应用范围,碳纳米点是一类具有优异光学性质、生物相容性且成本低廉的新型发光纳米颗粒。在此,电化学发光作为一种表面敏感工具,被用于探究碳纳米点以表面含氧基团为特征的未被揭示的性质。首次证明了碳纳米点作为Ru(bpy)3(2+)阳极电化学发光的共反应剂,与化学发光一起发挥作用。在阳极扫描过程中,C点表面的苄醇单元被电生成的Ru(bpy)3(3+)“均匀地”氧化,形成还原自由基中间体,该中间体进一步将Ru(bpy)3(3+)还原为产生强电化学发光发射的Ru(bpy)3(2+)*。这项工作为涉及C点的体系的电化学发光机制提供了深入见解,这将有助于深入理解C点的一些特殊现象,如光催化活性和氧化还原性质。此外,由于C点的特性,Ru(bpy)3(2+)/C点的电化学发光体系在生物分析中更具前景。