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Abstract:

The effect of surface charge on the electron transfer and charge propagation in layer by layer (LbL) electrostatically self-assembled redox poly-electrolyte multilayers (PEMs) has been studied. Thin films comprised of sequential layers of cationic poly(allylamine) covalently modified by osmium bipyridyl pyridine complexes (PAH-Os) and anionic poly(vinylsulfonate) (PVS) have been studied using electro-chemical impedance spectroscopy (EIS) and ellipsometry. For positively charged topmost layers a transition from low frequency redox pseudocapacitance to diffusion due to electron hopping between adjacent redox sites has been observed. This behavior could be modelled by a bound-diffusion modified Randles electrical equivalent circuit. Negatively charged surfaces terminated in PVS, on the other hand, presented a kinetic hindrance for the osmium redox switching process. This may be ascribed to a limitation in the flux of mobile anions compensating charge due to a skin Donnan potential at the film/electrolyte interface or effects on the local electrostatic environment of the osmium sites. Further adsorption of polycations or charge screening by increasing the electrolyte ionic strength restores the redox charge seen when the polycation was the topmost layer. © 2006 Elsevier B.V. All rights reserved.

Registro:

Documento: Artículo
Título:Surface charge effects on the redox switching of LbL self-assembled redox polyelectrolyte multilayers
Autor:Tagliazucchi, M.E.; Calvo, E.J.
Filiación:INQUIMAE, Departamento de Química Inorgánica, Analítica y Química Física, Facultad de Ciencias Exactas y Naturales, Argentina
Palabras clave:Donnan; EIS; Ellipsometry; Impedance; Layer by layer; Osmium bipyridyl; Redox polyelectrolyte; Self-assembled; Electron transitions; Ellipsometry; Layered manufacturing; Monolayers; Redox reactions; Spectroscopy; Osmium bipyridyl; Pseudocapacitance; Redox polyelectrolyte; Polyelectrolytes
Año:2007
Volumen:599
Número:2
Página de inicio:249
Página de fin:259
DOI: http://dx.doi.org/10.1016/j.jelechem.2006.03.014
Título revista:Journal of Electroanalytical Chemistry
Título revista abreviado:J Electroanal Chem
ISSN:15726657
CODEN:JECHE
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_15726657_v599_n2_p249_Tagliazucchi

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Citas:

---------- APA ----------
Tagliazucchi, M.E. & Calvo, E.J. (2007) . Surface charge effects on the redox switching of LbL self-assembled redox polyelectrolyte multilayers. Journal of Electroanalytical Chemistry, 599(2), 249-259.
http://dx.doi.org/10.1016/j.jelechem.2006.03.014
---------- CHICAGO ----------
Tagliazucchi, M.E., Calvo, E.J. "Surface charge effects on the redox switching of LbL self-assembled redox polyelectrolyte multilayers" . Journal of Electroanalytical Chemistry 599, no. 2 (2007) : 249-259.
http://dx.doi.org/10.1016/j.jelechem.2006.03.014
---------- MLA ----------
Tagliazucchi, M.E., Calvo, E.J. "Surface charge effects on the redox switching of LbL self-assembled redox polyelectrolyte multilayers" . Journal of Electroanalytical Chemistry, vol. 599, no. 2, 2007, pp. 249-259.
http://dx.doi.org/10.1016/j.jelechem.2006.03.014
---------- VANCOUVER ----------
Tagliazucchi, M.E., Calvo, E.J. Surface charge effects on the redox switching of LbL self-assembled redox polyelectrolyte multilayers. J Electroanal Chem. 2007;599(2):249-259.
http://dx.doi.org/10.1016/j.jelechem.2006.03.014