​Dual-Coreactants Enhanced Electrochemiluminescence.

IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Chemistry - A European Journal Pub Date : 2024-11-19 DOI:10.1002/chem.202403804
Jialian Ding, Bin Su
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Abstract

The electrochemiluminescence (ECL) of ruthenium(II) tris(2,2'-bipyridyl) (Ru(bpy)32+) with tri-n-propylamine (TPrA) as the good coreactant can be unexpectedly enhanced by a weak coreactant, such as triethanolamine (TEOA). First, the intensity of ECL emitted by Ru(bpy)32+/TPrA can be remarkably amplified by 10.8-fold after adding some amount of TEOA. Moreover, the ECL layer thickness, measured by self-interference spectroscopy, is also doubled. The enhancement far exceeding the superposition of respective contribution of TPrA and TEOA was elucidated by a "chemical oxidation mechanism", in which TEOA+• acts as a chemical enhancer to oxidize TPrA in solution and to accelerate significantly the ECL reaction kinetics. This mechanism was proved by single-photon counting experiment and finite element simulations. In addition, the dual-coreactants strategy works well not only in solution with freely diffusive Ru(bpy)32+, but also on Ru(bpy)32+-functionalized microbeads, suggesting that ethanolamines could act as cheap, easily available and low-background enhancers for ECL-based bioanalysis and microscopy.

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双核反应物增强电化学发光。
以三正丙胺(TPrA)为良好核心反应剂的三(2,2'-联吡啶)钌(II)(Ru(bpy)32+)的电化学发光(ECL)可以意外地通过三乙醇胺(TEOA)等弱核心反应剂得到增强。首先,加入一定量的 TEOA 后,Ru(铋)32+/TPRA 发出的 ECL 强度可显著放大 10.8 倍。此外,用自干涉光谱法测量的 ECL 层厚度也增加了一倍。这种远远超过 TPrA 和 TEOA 各自贡献的叠加效应的增强是通过 "化学氧化机制 "来阐明的,在该机制中,TEOA+- 作为一种化学增强剂,氧化溶液中的 TPrA,并显著加速 ECL 反应动力学。单光子计数实验和有限元模拟证明了这一机制。此外,双核活性剂策略不仅在具有自由扩散的 Ru(bpy)32+ 的溶液中效果良好,而且在 Ru(bpy)32+ 功能化的微珠上效果也很好,这表明乙醇胺可以作为廉价、易得和低背景的增强剂用于基于 ECL 的生物分析和显微镜检查。
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来源期刊
Chemistry - A European Journal
Chemistry - A European Journal 化学-化学综合
CiteScore
7.90
自引率
4.70%
发文量
1808
审稿时长
1.8 months
期刊介绍: Chemistry—A European Journal is a truly international journal with top quality contributions (2018 ISI Impact Factor: 5.16). It publishes a wide range of outstanding Reviews, Minireviews, Concepts, Full Papers, and Communications from all areas of chemistry and related fields. Based in Europe Chemistry—A European Journal provides an excellent platform for increasing the visibility of European chemistry as well as for featuring the best research from authors from around the world. All manuscripts are peer-reviewed, and electronic processing ensures accurate reproduction of text and data, plus short publication times. The Concepts section provides nonspecialist readers with a useful conceptual guide to unfamiliar areas and experts with new angles on familiar problems. Chemistry—A European Journal is published on behalf of ChemPubSoc Europe, a group of 16 national chemical societies from within Europe, and supported by the Asian Chemical Editorial Societies. The ChemPubSoc Europe family comprises: Angewandte Chemie, Chemistry—A European Journal, European Journal of Organic Chemistry, European Journal of Inorganic Chemistry, ChemPhysChem, ChemBioChem, ChemMedChem, ChemCatChem, ChemSusChem, ChemPlusChem, ChemElectroChem, and ChemistryOpen.
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