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

IF 6.7 1区化学 Q1 CHEMISTRY, ANALYTICAL Analytical Chemistry Pub Date : 2024-11-05 Epub Date: 2024-10-22 DOI:10.1021/acs.analchem.4c04301

Xuewei Cao, Ziyu Wang, Ben Liu, Xinyu Li, Shanshan Wu, Jingshuo Jiang, Jiankai Feng, Huangxian Ju, Ningning Wang

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Abstract

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.

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用于碘离子无核心活性可视化检测的掺染染料聚合物点的自增强电化学发光。

放射性碘水平的监测在环境科学和癌症放射治疗中具有重要意义。本研究开发了一种高通量、抗辐射和可视化的电化学发光（ECL）策略，用于检测碘离子。在这项研究中，疏水性钌衍生物（Ru(bpy)3[B(C6F5)4]2）（bpy = 联吡啶）被掺杂到叔胺耦合聚合物点（N-PFO Pdots）中，合成了自增强 Pdots（Ru@Pdots），在没有核心反应物的情况下，该衍生物显示出极高的 ECL 强度。由于 Ru(bpy)3[B(C6F5)4]2 和 N-PFO 之间高效的 ECL 共振能量转移，Ru@Pdots 的 ECL 强度是裸 N-PFO Pdots 的 18 倍。此外，Ru@Pdots 的 ECL 强度比 Ru(bpy)3[B(C6F5)4]2 掺杂核心反应物的 Pdots（Ru@PFO Pdots）高 220 倍。利用 Ru@Pdots 作为 ECL 发射器，设计了一种用于碘离子检测的 ECL 成像阵列，其检测范围为 0.8 nM-4 μM，检测限为 0.1 nM。在该方法中，碘离子在电极表面被氧化成碘自由基，从而进一步消耗 Ru@Pdots 的氮自由基，有效淬灭 ECL 信号。该方法在实际海水样品测试中也表现出良好的特异性、抗辐射性能和准确性，表明其在海洋环境监测、核安全和癌症放射治疗中的价值。

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来源期刊

Analytical Chemistry 化学-分析化学

CiteScore

12.10

自引率

12.20%

发文量

1949

审稿时长

1.4 months

期刊介绍： Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.