Ge Zhi-Li, Song Tian-Mei, Chen Zhe, Guo Wu-Run, Xie Hong-Ping, Xie Lian
College of Pharmaceutical Science, Soochow University, Suzhou 215123, PR China.
College of Pharmaceutical Science, Soochow University, Suzhou 215123, PR China; College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637002, PR China.
Anal Chim Acta. 2015 Mar 3;862:24-32. doi: 10.1016/j.aca.2015.01.013. Epub 2015 Jan 12.
In this paper the strong electrochemiluminescence (ECL) nanoparticles have been prepared based on the anionic polyelectrolyte sodium polyacrylate (PAA)-ECL enhancement for Ru(bpy)3(2+), which were loaded by the carrier of SiO2 nanoparticle. There were two kinds of Ru(bpy)3(2+) for the as-prepared nanoparticles, the doped one and the exchanged one. The former was loaded inside the ECL nanoparticles by doping, in a form of ion-pair macromolecules PAA-Ru(bpy)3(2+). The corresponding ECL was enhanced about 2 times owing to the doping increase of Ru(bpy)3(2+). The latter was loaded on the PAA-doped Nafion membrane by ion exchange. The corresponding ECL was enhanced about 3 times owing to the ion-exchanging increase of Ru(bpy)3(2+). At the same time, ECL intensity of the doped-inside Ru(bpy)3(2+) was further enhanced 13 times because polyelectrolyte PAA in the doped membrane could obviously enhance electron transfer between the doped Ru(bpy)3(2+) and the working electrode. Furthermore, based on hydrophobic regions of the doped membrane antibody labeling could be easily realized by the as-prepared nanoparticles and then a high sensitive ECL immunoassay for HBsAg was developed. The linear range was between 1.0 and 100 pg mL(-1) (R(2)=0.9912). The detection limit could be as low as 0.11 pg mL(-1) (signal-to-noise ratio=3).
本文基于阴离子聚电解质聚丙烯酸钠（PAA）对Ru(bpy)₃²⁺的电化学发光（ECL）增强作用，制备了强ECL纳米粒子，其载体为SiO₂纳米粒子。所制备的纳米粒子中有两种Ru(bpy)₃²⁺，一种是掺杂的，另一种是交换的。前者通过掺杂以离子对大分子PAA-Ru(bpy)₃²⁺的形式负载在ECL纳米粒子内部。由于Ru(bpy)₃²⁺掺杂量增加，相应的ECL增强了约2倍。后者通过离子交换负载在PAA掺杂的Nafion膜上。由于Ru(bpy)₃²⁺离子交换量增加，相应的ECL增强了约3倍。同时，掺杂在内部的Ru(bpy)₃²⁺的ECL强度进一步增强了13倍，因为掺杂膜中的聚电解质PAA可以明显增强掺杂的Ru(bpy)₃²⁺与工作电极之间的电子转移。此外，基于掺杂膜的疏水区域，所制备的纳米粒子可以轻松实现抗体标记，进而开发了一种用于检测HBsAg的高灵敏度ECL免疫分析法。线性范围为1.0至100 pg mL⁻¹（R² = 0.9912）。检测限可低至0.11 pg mL⁻¹（信噪比 = 3）。
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