High-Frequency Electrochemiluminescent Investigation of the Reaction Pathway between Tris(2,2‘-bipyridyl)ruthenium(II) and Tripropylamine Using Carbon Fiber Microelectrodes

Gross, Erin M.; Pastore, Paolo; Wightman, R. Mark

doi:10.1021/jp011434z

Cited by 78 publications

(91 citation statements)

References 44 publications

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“…. Particularly, the observed redox potential is far more positive than À [5,14] It also contradicts Wightman's explanation [4] of the ECL quenching by p-nitroacetophenone (E 1/2 À 1.03 V vs. Ag/AgCl) and 4-nitrotoluene (E 1/2 À 1.25 V vs. Ag/AgCl) via intercepting the reducing free radical. However, it should be noted that the ECL experiments compared here are carried out in aqueous solutions.…”

Section: N]mentioning

confidence: 92%

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Direct Voltammetric Evidence for a Reducing Agent Generated from the Electrochemical Oxidation of Tripropylamine for Electrochemiluminescence of Ruthenium Tris(bipyridine) Complexes?

et al. 2003

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After the initial suggestion [1] involving the simultaneous electrochemical formation of [Ru(bpy) 3 ] 3 (bpy 2,2'-bipyridine) and tripropylamine (TPA) cation radical [(C 3 H 7 ) 3 N]. , referred to here as TPA . , several mechanisms for [Ru(bpy) 3 ] 2 /TPA electrochemiluminescence (ECL) system have been proposed and examined.[2±5] In all these proposals, a strong reducing agent, which is believed to be a free radical produced from the deprotonation of the cation radical TPA. , serves as a key coreactant in the course . , which, contrary to the previous conception, is considered to be reasonably long-lived and evidenced by its electron spin resonance (ESR) signal.[5]Although the search for voltammetric evidence of TPA . failed, this mechanism provides an explanation for the luminescence observed at potentials where the electrochemical oxidation of [Ru(bpy) 3 ] 2 does not occur. It was also used to explain the ECL that is thought to be generated from the microbead surface out of the electrode diffusion layer in the commercial immunoassay systems.[6±7] As a fundamental factor in this mechanism, the redox potential of the reducing radical must be more negative than À 1.48 V (vs. Ag/AgCl), a value for the [Ru(bpy) . is formed. Therefore, instead of searching for TPA . , the study reported here was focused on tracing voltammetric evidence for the reducing agent and its oxidized product Pr. Although the ECL studies [1±5] mentioned above were carried out in aqueous solutions, a nonaqueous system is suitable for the electrochemical study of TPA. Cyclic voltammograms (CVs) of TPA were first recorded using a platinum-disk working electrode (0.785 mm 2 ) in acetonitrile solutions with tetrabutylammonium hexafluorophosphate (TBAPF 6 , 0.1 M) as a supporting electrolyte and silver wire as a quasi-reference electrode, which was calibrated with the ferrocene/ferrocenium (Fc/Fc ) redox couple by taking E8 Fc/Fc 0.35 V vs. Ag/AgCl. The details of the procedure and the specially designed cell connected with a vacuum line for removing water and oxygen were described previously.[10±11] To rule out the possibility of any redox active impurity existing in the system, we scanned the potential, firstly, downwards from À 0.28 to À 2.28 V and then upwards to 1.02 V. After sufficient amount of TPA was oxidized (oxidation peak appeared), the scan was reversed to move downwards until a cathodic wave was found. Once a cathodic wave was detected, multiple cyclic scans around the wave were followed. Figure 1 demonstrates a typical experimental result. During the initial scan from À 0.28 to À 2.28 V, no redox wave was detected. It indicates that no electrochemically active impurity existed in the system and that TPA itself cannot be reduced. As expected, after TPA undergoes an electrochemical oxidation and the potential scanning is switched back, a cathodic wave with a peak potential (E pc ) equal to À 1.02 V can be found. The follow-up multiple scans between À 1.48 and À 0.58 V indicate a fair reversibility and stability of the redox coupl...

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Section: N]mentioning

confidence: 92%

“…This change in lifetime was explained in terms of energy transfer between the dye and the metal coating of the probe. [4] Transient linear reflectivity, [5,6] transient transmissivity, [7] and transient absorption NSOM techniques have also been demonstrated.…”

Section: Time-resolved Second Harmonic Generation Near-field Scanningmentioning

confidence: 99%

Direct Voltammetric Evidence for a Reducing Agent Generated from the Electrochemical Oxidation of Tripropylamine for Electrochemiluminescence of Ruthenium Tris(bipyridine) Complexes?

et al. 2003

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“…[1][2][3] Several tandem systems involving more complex kinetic frameworks have also been reported. [4,5] Electron transfer can be initiated by adding a strong reductant, called co-reactant, to a solution of RuA C H T U N G T R E N N U N G (bpy) 3 2 + which is electrochemically oxidized. [5][6][7][8][9][10][11][12] The tandem generation of both reduced and oxidized reactants can be achieved experimentally in various ways.…”

Section: Introductionmentioning

confidence: 99%

“…They generate light after diffusing towards each other and exchanging their subsequent electron. [4,[13][14][15] Another way became available with the development of microelectrode assemblies. It consists of using two microelectrodes in close proximity (i.e.…”

Section: Introductionmentioning

confidence: 99%

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Mapping Electrochemiluminescence as Generated at Double‐Band Microelectrodes by Confocal Microscopy under Steady State

et al. 2006

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A confocal microspectrometer was used to collect spatially resolved electrochemiluminescence (ECL) spectra from the annihilation reaction between Ru(bpy)3+ and Ru(bpy)3(3+), each species being generated at a platinum band microelectrode and separated by a micrometric insulating gap. The use of a confocal microspectrometer allows in situ photon detection of the ECL reaction with micrometric spatial resolution and observes the concentration distribution of the photon source in the vicinity of the interelectrode gap.

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Light‐Emitting Devices Based on Electrochemiluminescence Gels

Cho

Lee

et al. 2020

Adv Funct Materials

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Electrochemiluminescence (ECL) is a self‐emission of light from electrochemically excited luminophores via a series of redox reactions. Over the past decade, light‐emitting devices based on gel‐phase ECL active materials, i.e., gel electrolyte composites (referred to as ECL gels) containing an ECL luminophore, electrolyte, and network matrix, have attracted considerable attention as a complementary device platform to conventional electroluminescent devices for low‐cost printable displays and solid‐state light sources. Although the ECL phenomenon is extensively exploited in analytical diagnostics and sensing, the development of printable and fast‐response gel‐type luminescent materials may further expand the potential application of ECL in solid‐state flexible, bendable, and stretchable light‐emitting devices. This review summarizes the operation mechanisms of ECL‐based light‐emitting devices, ECL emitters and electrolytes, engineering strategies for obtaining printable high‐strength/high‐conductivity ECL gels, and emerging applications of gel‐type ECL devices.

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High-Frequency Electrochemiluminescent Investigation of the Reaction Pathway between Tris(2,2‘-bipyridyl)ruthenium(II) and Tripropylamine Using Carbon Fiber Microelectrodes

Cited by 78 publications

References 44 publications

Direct Voltammetric Evidence for a Reducing Agent Generated from the Electrochemical Oxidation of Tripropylamine for Electrochemiluminescence of Ruthenium Tris(bipyridine) Complexes?

Direct Voltammetric Evidence for a Reducing Agent Generated from the Electrochemical Oxidation of Tripropylamine for Electrochemiluminescence of Ruthenium Tris(bipyridine) Complexes?

Mapping Electrochemiluminescence as Generated at Double‐Band Microelectrodes by Confocal Microscopy under Steady State

Light‐Emitting Devices Based on Electrochemiluminescence Gels

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