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Visualising electrochemical reaction layers: mediated vs. direct oxidation

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Abstract

Electrochemical treatments are widely used for ‘clean up’ in which toxic metals and organic compounds are removed using direct or mediated electrolysis. Herein we report novel studies offering proof of concept that spectrofluorometric electrochemistry can provide important mechanistic detail into these processes. A thin layer opto-electrochemical cell, with a carbon fibre (radius 3.5 μm) working electrode, is used to visualise the optical responses of the oxidative destruction of a fluorophore either directly, on an electrode, or via the indirect reaction of the analyte with an electrochemically formed species which ‘mediates’ the destruction. The optical responses of these two reaction mechanisms are first predicted by numerical simulation followed by experimental validation of each using two fluorescent probes, a redox inactive (in the electrochemical window) 1,3,6,8-pyrenetetrasulfonic acid and the redox-active derivative 8-hydroxypyrene-1,3,6-trisulfonic acid. In the vicinity of a carbon electrode held at different oxidative potentials, the contrast between indirect electro-destruction, chlorination, and direct oxidation is very obvious. Excellent agreement is seen between the numerically predicted fluorescence intensity profiles and experiment.

Graphical abstract: Visualising electrochemical reaction layers: mediated vs. direct oxidation

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Supplementary files

Article information


Submitted
08 Apr 2020
Accepted
22 May 2020
First published
22 May 2020

This article is Open Access

Phys. Chem. Chem. Phys., 2020, Advance Article
Article type
Paper

Visualising electrochemical reaction layers: mediated vs. direct oxidation

J. Ma, M. Yang, C. Batchelor-McAuley and R. G. Compton, Phys. Chem. Chem. Phys., 2020, Advance Article , DOI: 10.1039/D0CP01904F

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