Self-induced redox cycling coupled luminescence on nanopore recessed disk-multiscale bipolar electrodes

Ma, Chaoxiong; Zaino, Lawrence P.; Bohn, Paul W.

doi:10.1039/c5sc00433k

Cited by 39 publications

(38 citation statements)

References 43 publications

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“…For example, they can utilize optical readout by coupling the analytical redox reaction at one pole to a fluorogenic (e.g. dark‐to‐emissive transition) redox process at the other pole, thereby combining the low background of photon emission measurements with the attractive features of BPEs for supporting redox reactions . Furthermore, by exploiting closed BPE systems it is possible to arrange for the light emission measurement to be carried out remotely from the analytical redox process, greatly simplifying experimental design.…”

Section: Introductionmentioning

confidence: 99%

“…dark-to-emissive transition) redoxp rocess at the other pole, therebyc ombining the low background of photon emission measurements with the attractive features of BPEs for supporting redox reactions. [16] Furthermore,b ye xploiting closed BPE systems it is possible to arrangef or the light emission measurement to be carriedo ut remotely from the analytical redox process, greatly simplifying experimental design.R ealizing this principle, Crooks and coworkers demonstrated coupling between an on-fluorescent electrochemical reactions uch as benzylv iologen reduction ande lectrogenerated chemiluminescence (ECL) in Ru(bpy) 3 2/3 + /tri-n-propylamine. [17] Measuring the ECL light intensity neatly solves the problem associatedw ith direct measurement of current flowing throught he BPE.…”

Section: Introductionmentioning

confidence: 99%

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Coupling of Independent Electrochemical Reactions and Fluorescence at Closed Bipolar Interdigitated Electrode Arrays

Bohn

2015

ChemElectroChem

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Electrochemical reactions occurring at the opposite ends of bipolar electrodes (BPEs) are necessarily coupled, enabling electron transfer events at one end to be read out optically, for example, by coupling to fluorogenic reactions at the other end. To explore the potential of this technique for studying multiple redox events, arrays of parallel BPE interdigitated electrode arrays (IDEAs) were fabricated and integrated with separate analytical and reporter microfluidic channels, respectively, in a closed BPE configuration. The apparatus was initially evaluated employing Fe(CN)63/4− in the analytical channel coupled to weakly emissive resazurin and strongly emissive resorufin as the fluorogenic redox reporter pair. The device was then used to investigate a proton‐coupled electron transfer reaction, hydroquinone (QH2) oxidation, in structures with an integrated pH modulation electrode (PME). A pH‐sensitive dye, fluorescein, was co‐introduced into the analytical channel to monitor PME modulation of solution pH, and its coupling to QH2 oxidation, thereby permitting changes in solution pH, and consequently QH2 oxidation rate, to be monitored directly in the analytical channel and compared to the fluorescence in the reporter channel. In addition, diffusion of OH− generated at the PME produced a spatial pH profile that was visualized via fluorescein emission, and, because the oxidation of QH2 at each BPE is strongly dependent on the local pH, via the coupled fluorogenic reaction at the opposite pole of the corresponding BPE digit in the reporter channel. Thus, BPE IDEAs support the coupling of independent redox reactions and the use of fluorescence imaging to explore a diverse set of spatially varying electrochemical phenomena realized in a variety of electrochemical geometries.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Coupling of Independent Electrochemical Reactions and Fluorescence at Closed Bipolar Interdigitated Electrode Arrays

Bohn

2015

ChemElectroChem

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“…Redox cycling signals were obtained in dual mode (DM) with the generator and collector electrodes connected appropriately to the bipotentiostat. Single mode (SM) data was collected by running the same test but with the collector electrode open circuited (bipotentiostat lead was disconnected from the bottom LME electrode) as is common in the literature .…”

Section: Methodsmentioning

confidence: 99%

An Improved Design and Versatile New Lamination Fabrication Method for Twin Electrode Thin Layer Cells Utilizing Track‐etch Membranes

Hauke

Ehrlich²,

Levine³

et al. 2018

Electroanalysis

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Reported here are laminated membrane electrodes, an improved design and more advantageous method of fabrication for previously reported thin layer cell electrode systems developed on track‐etch membranes. The laminated membrane approach potentially further improves flow resistance by dramatically reducing the surface area to volume ratio, but also produces a cohesive device that can be more readily applied to a broad range of applications. In addition, this new fabrication method was implemented in a scalable, commercial process and resulting product demonstrations indicate that volume manufacturing is feasible. Characterization of laminated membrane electrodes reveal redox cycling amplification factors as high as 30 with linear responses to variable concentrations of redox couple. These performance characteristics are shown to be comparable to similar generator‐collector systems fabricated through much more laborious laboratory methods. This combination of added versatility, cost‐reduced fabrication and exceptional performance clearly reveals unrealized potential of track‐etch membrane approaches and boosts their candidacy as powerful new options for generator‐collector electrode systems.

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“…It is still challenging to detect both ion flux and accompanying “bipolar” redox reactions in conjunction. Related and very interesting attempts to introduce bipolar detection processes in nanopores have been reported, for example, by Albrecht and co‐workers, and by Bohn and co‐workers . The electrochemical detection with metal‐based nanopores, with graphene‐based nanopores, and with bipotentiostatically controlled probe electrodes at nanopores has been proposed ,…”

Section: Figurementioning

confidence: 99%

Confining Nanopore Bipolar Electrochemical Processes to Give Pattern in Space and Time

Marken

2017

ChemElectroChem

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“Wireless” metal‐coated nanopore electrode processes have been developed by Long and co‐workers (R. Gao, Y. Lin, Y.‐L. Ying, X.‐Y. Liu, X. Shi, Y.‐X. Hu, Y.‐T. Long, Small, 2017 DOI: 10.1002/smll.201700234), confining bipolar electrochemical processes into a nanopore. The reported concept of this new methodology may lead to intriguing new analytical and micro‐structuring applications based on a temporal pattern in ionic current responses and based on a spatial pattern leading to micro‐ring nanoassembly.

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Self-induced redox cycling coupled luminescence on nanopore recessed disk-multiscale bipolar electrodes

Abstract: Self-induced redox cycling at nanopore ring-disk electrodes is coupled, through a bipolar electrode, to a remote fluorigenic reporter reaction.

Cited by 39 publications

References 43 publications

Coupling of Independent Electrochemical Reactions and Fluorescence at Closed Bipolar Interdigitated Electrode Arrays

Coupling of Independent Electrochemical Reactions and Fluorescence at Closed Bipolar Interdigitated Electrode Arrays

An Improved Design and Versatile New Lamination Fabrication Method for Twin Electrode Thin Layer Cells Utilizing Track‐etch Membranes

Confining Nanopore Bipolar Electrochemical Processes to Give Pattern in Space and Time

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