Journal
ANALYTICAL CHEMISTRY
Volume 83, Issue 2, Pages 542-548Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ac102113v
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Funding
- National Science Foundation [CHE-0911383]
- National Institutes of Health [GM 070544]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0911383] Funding Source: National Science Foundation
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We report on the design and performance of a thin-layer electrochemical cell optimized for use with optically transparent film electrodes in combination with UV/vis and IR transmission spectroscopic measurements. The cell allows for measurements under both aerobic and anaerobic conditions. The direct, unmediated electron transfer, as assessed by the current transient, and the corresponding optical response observed for the Fe(CN)(6)(3-/4-) couple were in good agreement with theoretical predictions for voltammetry and optical absorption by an analyte confined in a thin layer. Chronoamperometric and spectroscopic measurements of Fe(CN)(6)(3-/4-) on gold mesh electrode revealed fast kinetics strongly influenced by the electrolyte concentration. Maximal apparent rates exceeding 2 s(-1) in 1 M KCl were observed optically. The direct kinetic and thermodynamic behavior of cytochrome c was compared with several electrode materials using the cell. The results showed heme ligand-dependent changes in the protein-electrode interactions. Mid-UV/visible spectral changes upon redox transitions in native cytochrorne c and its cyanide derivative, as well as dissociation of the ferrous cytochrome c-CN complex, are reported.
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