Journal
LANGMUIR
Volume 26, Issue 2, Pages 1340-1346Publisher
AMER CHEMICAL SOC
DOI: 10.1021/la902418v
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Funding
- St. John's College, Oxford
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We demonstrate proof-of-concept that generator-collector experiments can be pet-formed at a single macroelectrode and used to determine mechanistic information. The practical advantages of such a system over conventional generator-collector techniques are also outlined. The single-electrode genera tor-col lector technique is applied to study the known mechanism of oxygen reduction in aqueous conditions as a model system. We seek to demonstrate that the single-electrode genera tor-col lector approach is capable of detecting local pH changes, immediately adjacent to the electrode surface during a redox reaction. Experiments are pet-formed using a molecular pH probe attached to the electrode surface. Comparison of experimental data with numerical simulations verifies that the reduction of oxygen at pH 6.8 proceeds via a two-electron, two-proton mechanism. Experiments were also performed with a molecular pH probe dissolved in the electrolyte Solution in order to explore the feasibility of this approach, which is potentially applicable to a much wider range of electrochemical systems.
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