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Abstract:

This work reports the fabrication of redox-active films of oligomeric and molecular viologens and mesoporous silica via the infiltration method. Pore-ellipsometry and UV-vis confirm that low-molecular-weight poly(viologens) in solution are able to enter the mesoporous structure, in contrast to high-molecular weight polymers that adsorb only on top of the film. Cyclic voltammetry shows that viologens are able to reach the bottom of the pores and access the electrode/film interface. However, the number of viologen sites that can be accessed by cyclic voltammetry at 50 mV s-1 is only a tenth of the total viologen population determined by UV-vis and pore-ellipsometry. The effect is ascribed to the very small apparent diffusion coefficient for charge transport within the film (Dapp < 10-12 cm2 s-1). A theoretical model is put forward to describe charge transport via the electron-hopping mechanism for redox sites randomly adsorbed on the inner walls of the pores. Our model predicts that the threshold of charge percolation occurs for viologen surface coverages close to those observed in our experiments; therefore, the low fraction of electrochemically addressable viologens is ascribed to inefficient charge percolation via the electron-hopping mechanism. © 2019 the Owner Societies.

Registro:

Documento: Artículo
Título:Charge percolation in redox-active thin membrane hybrids of mesoporous silica and poly(viologens)
Autor:Saint-André, S.; Albanese, F.; Soler-Illia, G.J.A.A.; Tagliazucchi, M.
Filiación:Departamento de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos, Aires Cuidad Universitaria, Buenos Aires, 1428, Argentina
DQIAQF, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos, Aires Ciudad Universitaria, Pab. II C1428EHA, Ciudad Autónoma de Buenos Aires, Argentina
Instituto de Nanosistemas, Universidad Nacional de General San Martín, Av. 25 de Mayo y Francia 1650, San Martín, Argentina
INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos, Aires Ciudad Universitaria, Pab. II C1428EHA, Ciudad Autónoma de Buenos Aires, Argentina
Año:2019
Volumen:21
Número:5
Página de inicio:2743
Página de fin:2754
DOI: http://dx.doi.org/10.1039/c8cp07192f
Título revista:Physical Chemistry Chemical Physics
Título revista abreviado:Phys. Chem. Chem. Phys.
ISSN:14639076
CODEN:PPCPF
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_14639076_v21_n5_p2743_SaintAndre

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Citas:

---------- APA ----------
Saint-André, S., Albanese, F., Soler-Illia, G.J.A.A. & Tagliazucchi, M. (2019) . Charge percolation in redox-active thin membrane hybrids of mesoporous silica and poly(viologens). Physical Chemistry Chemical Physics, 21(5), 2743-2754.
http://dx.doi.org/10.1039/c8cp07192f
---------- CHICAGO ----------
Saint-André, S., Albanese, F., Soler-Illia, G.J.A.A., Tagliazucchi, M. "Charge percolation in redox-active thin membrane hybrids of mesoporous silica and poly(viologens)" . Physical Chemistry Chemical Physics 21, no. 5 (2019) : 2743-2754.
http://dx.doi.org/10.1039/c8cp07192f
---------- MLA ----------
Saint-André, S., Albanese, F., Soler-Illia, G.J.A.A., Tagliazucchi, M. "Charge percolation in redox-active thin membrane hybrids of mesoporous silica and poly(viologens)" . Physical Chemistry Chemical Physics, vol. 21, no. 5, 2019, pp. 2743-2754.
http://dx.doi.org/10.1039/c8cp07192f
---------- VANCOUVER ----------
Saint-André, S., Albanese, F., Soler-Illia, G.J.A.A., Tagliazucchi, M. Charge percolation in redox-active thin membrane hybrids of mesoporous silica and poly(viologens). Phys. Chem. Chem. Phys. 2019;21(5):2743-2754.
http://dx.doi.org/10.1039/c8cp07192f