This tutorial review gives a brief introduction to impedance spectroscopy and discusses how it has been used to provide insight into charge transport through conducting polymers, particularly when the polymers are used as electrodes for solution studies or the design of electrodes for biomedical applications. As such it provides both an introduction to the topic and references to both classic and contemporary work for the more advanced reader.

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The impedance behavior of semiconducting polymer film electrodes based on poly(3,4-ethylenedioxythiophene) (PEDOT) in combination with a series of anionic dopants has been investigated using electrochemical impedance spectroscopy (EIS) over the frequency range from 0.1 Hz to 100 kHz. Films were electrodeposited on gold-coated Pt wire electrodes from a nonaqueous solution containing 3,4-ethylenedioxythiophene (EDOT). EIS results reveal that, under the optimal synthesis conditions, PEDOT electrodes consistently exhibit low, frequency-independent impedance over a wide frequency range (from ∼10 Hz to 100 kHz). These results suggest that the behavior originates from the two-layer homogeneous morphology of the film. A model for conduction in the films that is supported by experimental evidence is proposed, and EIS data for electrodes produced under a variety of electropolymerization conditions are presented.

We have examined the interaction of methyl isocyanide with the purified component proteins of Azotobacter vinelandii nitrogenase (Av1 and Av2). CH3NC was shown to be a potent reversible inhibitor (Ki = 158 microM) of total electron flow, apparently uncoupling magnesium adenosine 5'-triphosphate hydrolysis from electron transfer to substrate. CH3NC is a substrate (Km = 0.688 mM at Av2/Av1 = 8), and extrapolation of the data indicates that at high enough CH3NC concentration, H2 evolution can be eliminated. The products are methane plus methylamine (six electrons) and dimethylamine (four electrons). There is an excess (relative to methane) of methylamine formed, which may arise by hydrolysis of a two-electron intermediate. A rapid high-performance liquid chromatography/fluorescence method was developed for methylamine determination. The products C2H4 and C2H6 appear to be formed via a reduction followed by an insertion mechanism. CH3NC appears to be reduced at an enzyme state more oxidized than the one responsible for H2 evolution or N2 reduction. Other substrates (C2H2 greater than N2 congruent to azide greater than N2O) all both relieve CH3NC inhibition and inhibit CH3NC reduction. Both effects occur in the same relative order, implying productive (substrate) and nonproductive (inhibitor) modes of binding of CH3NC to the same site.

Microelectrode arrays have been extensively utilized to record extracellular neuronal activity for brain-machine interface applications. Poly(3,4-ethylenedioxythiophene) (PEDOT) has gained interest because of its unique electrochemical characteristics and its excellent intrinsic electrical conductivity. However, the long-term stability of the PEDOT film, especially for chronic neural applications, is unclear. In this manuscript, we report for the first time the use of highly stable PEDOT doped with tetrafluoroborate (TFB) for long-term neural recordings. We show that PEDOT-TFB coated microelectrodes on average register more units compared to control gold microelectrodes for at least first four weeks post implantation. We collected the in vivo impedance data over a wide frequency spectrum and developed an equivalent circuit model which helped us determine certain parameters to distinguish between PEDOT-TFB microelectrodes with and without long-term activity. Our findings suggest that PEDOT-TFB is a chronically stable coating for neural recording microelectrodes. As such, PEDOT-TFB could facilitate chronic recordings with ultra-small and high-density neural arrays.

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