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Abstract:

The redox switching kinetics, that is, charge transfer and transport in layer-by-layer-deposited electroactive polyelectrolyte multilayers is systematically studied with variable-scan-rate cyclic voltammetry. The experiments are performed with films finished in the redox polycation (an osmium pyridine-bipyridine derivatized polyallylamine, PAH-Os) and the polyanion (polyvinyl sulfonate, PVS), in solutions of different electrolyte concentrations. A modified diffusion model is developed to account for the experimentally observed dependence of the average peak potential with the scan rate. This model is able to describe both the redox peak potential and the current, providing information on the electron-transfer rate constants and the diffusion coefficient for the electron-hopping mechanism. While the former does not vary with the ionic strength or the nature of the outmost layer, polyanion-capped films present an electron-hopping diffusion coefficient at low ionic strength that is three orders of magnitude smaller than that for PAH-Os-capped films. The effect is offset at high ionic strength. We discuss the possible causes of the effect and the important consequences for electrochemical devices built by layer-by-layer self-assembly, such as amperometric biosensors or electrochromic devices. © 2010 Wiley-VCH Verlag GmbH& Co. KGaA, Weinheim.

Registro:

Documento: Artículo
Título:Charge transport in redox polyelectrolyte multilayer films: The dramatic effects of outmost layer and solution ionic strength
Autor:Tagliazucchi, M.; Calvo, E.J.
Filiación:INQUIMAE-Departamento de Química Inorgánica, Analítica y Química Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires-CONICET, Pabellón 2, Ciudad Universitaria, 1428 Buenos Aires, Argentina
Palabras clave:Electron hopping; Electron transport; Polyelectrolyte multilayers; Polymers; Redox chemistry
Año:2010
Volumen:11
Número:13
Página de inicio:2957
Página de fin:2968
DOI: http://dx.doi.org/10.1002/cphc.201000172
Título revista:ChemPhysChem
Título revista abreviado:ChemPhysChem
ISSN:14394235
CODEN:CPCHF
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_14394235_v11_n13_p2957_Tagliazucchi

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Citas:

---------- APA ----------
Tagliazucchi, M. & Calvo, E.J. (2010) . Charge transport in redox polyelectrolyte multilayer films: The dramatic effects of outmost layer and solution ionic strength. ChemPhysChem, 11(13), 2957-2968.
http://dx.doi.org/10.1002/cphc.201000172
---------- CHICAGO ----------
Tagliazucchi, M., Calvo, E.J. "Charge transport in redox polyelectrolyte multilayer films: The dramatic effects of outmost layer and solution ionic strength" . ChemPhysChem 11, no. 13 (2010) : 2957-2968.
http://dx.doi.org/10.1002/cphc.201000172
---------- MLA ----------
Tagliazucchi, M., Calvo, E.J. "Charge transport in redox polyelectrolyte multilayer films: The dramatic effects of outmost layer and solution ionic strength" . ChemPhysChem, vol. 11, no. 13, 2010, pp. 2957-2968.
http://dx.doi.org/10.1002/cphc.201000172
---------- VANCOUVER ----------
Tagliazucchi, M., Calvo, E.J. Charge transport in redox polyelectrolyte multilayer films: The dramatic effects of outmost layer and solution ionic strength. ChemPhysChem. 2010;11(13):2957-2968.
http://dx.doi.org/10.1002/cphc.201000172