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ELECTROCHEMISTRY COMMUNICATIONS · 2011 · IF 4.287

Thiol-ene click chemistry for the fabrication of Ru(bpy)32+-based solid-state electrochemiluminescence sensor

Kai Zeng,Manli Guo,Yingjun Zhang,Meng Qing,Afang Liu,Zhou Nie,Yan Huang,Yuliang Pan,Shouzhuo Yao

A novel method based on click chemistry for the immobilization of Ru(bpy) 3 2+ derivative on electrode to fabricate a solid state electrochemiluminescence (ECL) sensor was reported. Pentenyl functionalized Ru(bpy′) 3 Cl 2 was synthesized and immobilized on a (3-mercaptopropyl) trimethoxysilane (MPTMS) pretreated indium tin oxide (ITO) substrate via thiol-ene click chemistry reaction between its alkenyl group and the sulfhydryl group of MPTMS. The immobilization method is simple, fast, and efficient. More importantly, the resulting Ru(bpy′) 3 2+ monolayer film exhibited excellent stability in organic solvent, which is superior to many previously reported methods. Using tri- n -propylamine (TPrA) as a model analyte, the ECL sensor gave a wide linear range over 5   ×   10 −   6 to 5   ×   10 −   3   M, with a satisfactory detection limit of 1   ×   10 −   6   M ( S / N   =   3).

研究领域: 分析化学 · 材料科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2024 · IF 3.9

Dual-Coreactants Enhanced Electrochemiluminescence

Jialian Ding,Bin Su

Graphical One plus one is greater than two: A remarkable electrochemiluminescence (ECL) enhancement of Ru(bpy) 3 2+ /TPrA is observed by introducing another coreactant, TEOA, with a 10.8-fold increase of ECL intensity and 1.7-fold extension of ECL layer. The enhancement was interpreted by a chemical oxidation route, in which TEOA + ⋅ acts as an enhancer to produce more TPrA + ⋅ and meanwhile allow the remote formation of TPrA + ⋅. This dual-coreactants strategy works not only in solution with freely diffusive Ru(bpy) 3 2+ but also on Ru(bpy) 3 2+ -functionalized microbeads, showing promise in ECL-based bioassay and microscopy. The electrochemiluminescence (ECL) of ruthenium(II) tris(2,2′-bipyridyl) (Ru(bpy) 3 2+ ) 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) 3 2+ /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) 3 2+ , but also on Ru(bpy) 3 2+ -functionalized microbeads, suggesting that ethanolamines could act as cheap, easily available and low-background enhancers for ECL-based bioanalysis and microscopy.

研究领域: 分析化学 · 生物分析 · 显微技术
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ELECTROCHEMISTRY COMMUNICATIONS · 2024 · IF 4.7

Local electrochemiluminescence imaging using scanning electrochemical cell microscopy

Yufei Deng,Xiaofan He,Rong Jin,Dechen Jiang,Danjun Fang

In this communication, local electrochemiluminescence (ECL) imaging is achieved using scanning electrochemical cell microscopy (SECCM) to create a localized region for the occurrence of ECL reaction. The system is demonstrated using a droplet at the micropipette that is contact with the prepared Ru-Silica@Au particles at indium tin oxide (ITO) slide. Tri- n -propylamine (TPrA) in the droplet reacts with ruthenium complex in a 10 μm-diameter-region to produce ECL emission, which is recorded by photo multiplier tube (PMT) underneath the ITO slide. By contacting each local region consecutively, the distribution of steady-state current and the related ECL emission at the ITO surface is imaged. The local ECL intensity show an approximately linear dependence with the current, but obvious deviation from the linear curve is observed at some regions. This result suggests that the ECL emission is not only determined by the transferred electron number in the electrochemical reaction, and also affected by local environments at ITO surface. As compared with the traditionally used ECL imaging in the bulk solution, this strategy avoids the cross-talking of ECL emission from nearby regions, and could offer a new way to unveil more molecular mechanism in the ECL reaction.

研究领域: 分析化学 · 电化学 · 成像技术
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ChemElectroChem · 2017 ·Vol. 4 ·期 7 ·1763-1767 · IF 4.136

Electrochemiluminescence of a Vinyl-Functionalized Ruthenium Complex and Its Monolayer Formed through the Photoinduced Thiol-Ene Click Reaction

Weiliang Guo,Zhiyuan Cao,Yanhuan Liu,Bin Su

Graphical Ready to react : Electrochemiluminescence (ECL) generated from vinyl-functionalized bipyridine ruthenium complex, [Ru(bpy) 2 (dvbpy)] 2+ , is studied by using an ECL spooling technique. Its monolayer immobilized on an ITO electrode is also prepared through the thiol-ene click reaction. This solid-state ECL sensor exhibits good ECL stability and a large linear range for the model analysis of common amine species, such as TPrA. Vinyl-functionalized bipyridine ruthenium complex, bis(2,2′-bipyridine)(4,4′-di(4-vinylphenyl)-2,2′-bipyridine)ruthenium(II) hexaflurophosphate [Ru(bpy) 2 (dvbpy)](PF 6 ) 2 , was synthesized and the electrochemiluminescence (ECL) generated in the presence of co-reactant, namely tri- n -propylamine (TPrA), was investigated by using an ECL spooling technique. This complex was then covalently attached to the indium tin oxide electrode surface through photoinduced thiol-ene click chemistry to prepare a solid-state ECL sensor. The covalently immobilized [Ru(bpy) 2 (dvbpy)] 2+ monolayer film exhibited excellent stability toward ECL generation. The analytical sensitivity of the solid-state ECL sensor was evaluated through the detection of TPrA in the aqueous solution. A low limit of detection (LOD) of 0.25 μM and a wide linear range (ca. 10 −7 –10 −4 M) were obtained, indicating its potential usefulness in chemical and biochemical analysis.

研究领域: 分析化学 · 电化学 · 材料科学
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RSC Advances · 2022 ·Vol. 12 ·期 5 ·3157-3164 · IF 4.036

Electrogenerated chemiluminescence of a Ru(bpy)32+/arginine system: a specific and sensitive detection of acetaminophen

Yi Xiao,Guofang Wang,Haomin Yi,Suhua Chen,Qinyu Wu,Siyi Zhang,Kexin Deng,Simeng Zhang,Zi-Qi Shi,Xiaoping Yang

Ru(bpy)3Cl2/TPrA is a prominent and widely used ECL system in analytical science. However, the co-reactant TPrA restricts the variety of applications because of its toxicity, volatility, and high cost. Here, we use arginine (Arg) as an alternative co-reactant for Ru(bpy)32+ by taking advantage of its low cost, non-toxicity, and biocompatibility. The mechanism of the Ru(bpy)32+/Arg system is that the deprotonated Arg can react with Ru(bpy)32+ to release emission. The similarity between the Ru(bpy)32+/Arg, Ru(bpy)32+/TPrA, and Ru(bpy)32+/DBAE systems demonstrates that Arg can be used as an alternative co-reactant for Ru(bpy)32+ ECL. As a proof of concept, we achieve an excellent performance for acetaminophen (Ace) detection based on the specificity of Arg and Ace, with excellent linearity, low detection limits, and good recoveries. This work is promising to expand the scope of the Ru(bpy)32+/Arg system and move forward their applications in bioassays.

研究领域: 分析化学 · 生物分析 · 电化学
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