Self-Enhanced Electrochemiluminesence of Dye-Doped Polymer Dots for Coreactant-Free Visualized Detection of Iodide Ions

• Published in: Analytical chemistry (Washington) 2024-11, Vol.96 (44), p.17824-17830
• Main Authors: Cao, Xuewei, Wang, Ziyu, Liu, Ben, Li, Xinyu, Wu, Shanshan, Jiang, Jingshuo, Feng, Jiankai, Ju, Huangxian, Wang, Ningning
• Format: Article
• Language: English
• Subjects: analytical chemistry; Cancer; Chemical analysis; Coloring Agents - chemistry; detection limit; Electrochemical Techniques; Electrochemiluminescence; electrodes; Emitters; Energy transfer; Environmental monitoring; Environmental science; Free radicals; Hydrophobicity; Iodides; Iodides - analysis; Iodides - chemistry; Ions; Ions - analysis; Ions - chemistry; Limit of Detection; Luminescent Measurements; Marine environment; Nitrogen; Nitrogen radicals; Polymers; Polymers - chemistry; Quantum Dots - chemistry; Radiation therapy; Radiation tolerance; radiotherapy; Ruthenium; Ruthenium - chemistry; Seawater; Water analysis
• ISSN: 0003-2700; 1520-6882; 1520-6882
• DOI: 10.1021/acs.analchem.4c04301

The monitoring of radioactive iodide levels is of great significance in environmental science and cancer radiotherapy. In this work, a high-throughput, radiation-resistant, and visualized electrochemiluminescence (ECL) strategy was developed for detection of iodide ions. Herein, the hydrophobic ruthenium derivative (Ru­(bpy)3[B­(C6F5)4]2) (bpy = bipyridyl) was doped in tertiary amine-coupled polymer dots (N-PFO Pdots) to synthesize self-enhanced Pdots (Ru@Pdots), which showed extremely high ECL intensity in absence of coreactant. Due to the efficient ECL resonance energy transfer between Ru­(bpy)3[B­(C6F5)4]2 and N-PFO, the Ru@Pdots exhibited 18 times higher ECL intensity compared with bare N-PFO Pdots. Besides, Ru@Pdots also showed 220-times higher ECL intensity compared with Ru­(bpy)3[B­(C6F5)4]2 doped coreactant-dependent Pdots (Ru@PFO Pdots). Using Ru@Pdots as ECL emitters, an ECL imaging array was designed for iodide ion detection, which exhibited a detection range of 0.8 nM–4 μM and a limit of detection of 0.1 nM. In this strategy, iodide ions were oxidized as iodide free radicals on the surface of the electrode, which could further consume the nitrogen radical of Ru@Pdots and effectively quench the ECL signal. This method also showed good specificity, radiation-resistant performance, and accuracy in actual seawater sample testing, which indicated its value in marine environmental monitoring, nuclear security, and cancer radiotherapy.