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Capacitance Spectroscopy: A Versatile Approach To Resolving the Redox Density of States and Kinetics in Redox-Active Self-Assembled Monolayers
journal contribution
posted on 2012-08-02, 00:00 authored by Paulo R. Bueno, Giulia Mizzon, Jason J. DavisRedox active self-assembled monolayers inherently possess
both
electrochemically addressable and polarizable components. The latter
will contribute, with additional parasitic terms, to the iR drop effects within any form of electronic analysis, potentially
distorting results. A capacitive analysis of such interfaces (Electroactive
Monolayer Capacitance Spectroscopy), presented here, enables a clean
mapping of both the thermodynamic and kinetic faradaic characteristics
in a single experimental run, with parasitic nonfaradaic contributions
(polarization and resistance terms) both spectrally resolved and cleanly
removed. The methodology enables a rapid and undistorted quantification
of accessible redox site density of states (reported directly by redox
capacitance), molecular surface coverage, electron transfer kinetics,
and reorganization energies with comparatively little experimental
effort. Exemplified here with electroactive copper protein and ferrocene
films the approach is equally applicable to any redox active interface.
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electroactive copper proteinundistorted quantificationfaradaic characteristicsresistance termselectrochemically addressablenonfaradaic contributionsiR drop effectsferrocene filmsCapacitance Spectroscopyelectron transfer kineticsreorganization energiessurface coverageredox site densityinterfaceRedox Densitycapacitive analysisVersatile Approachpolarizable components
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