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Chemical Stability of Mesoporous Oxide Thin Film Electrodes under Electrochemical Cycling: from Dissolution to Stabilization

  • Sebastián Alberti
    Sebastián Alberti
    Gerencia Química − Centro Atómico Constituyentes, Comisión Nacional de Energía Atómica, CONICET, Avenida General Paz 1499, 1650 San Martín, Buenos Aires, Argentina
    Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA) − Universidad Nacional de La Plata − CONICET, CC 16 Suc. 4, 1900 La Plata, Buenos Aires, Argentina
  • Paula Y. Steinberg
    Paula Y. Steinberg
    Gerencia Química − Centro Atómico Constituyentes, Comisión Nacional de Energía Atómica, CONICET, Avenida General Paz 1499, 1650 San Martín, Buenos Aires, Argentina
  • Gustavo Giménez
    Gustavo Giménez
    Centro de Micro y Nanoelectrónica del Bicentenario, INTI-CMNB, Instituto Nacional de Tecnología Industrial, Avenida General Paz 5445, B1650WAB San Martín, Buenos Aires, Argentina
  • Heinz Amenitsch
    Heinz Amenitsch
    Institute for Inorganic Chemistry, Graz University of Technology, Stremayrgasse 9/IV, 8010 Graz, Austria
  • Gabriel Ybarra
    Gabriel Ybarra
    Unidad Técnica Nanomateriales, INTI-Procesos Superficiales, Instituto Nacional de Tecnología Industrial, Avenida General Paz 5445, B1650WAB San Martín, Buenos Aires, Argentina
  • Omar Azzaroni
    Omar Azzaroni
    Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA) − Universidad Nacional de La Plata − CONICET, CC 16 Suc. 4, 1900 La Plata, Buenos Aires, Argentina
  • Paula C. Angelomé
    Paula C. Angelomé
    Gerencia Química − Centro Atómico Constituyentes, Comisión Nacional de Energía Atómica, CONICET, Avenida General Paz 1499, 1650 San Martín, Buenos Aires, Argentina
  • , and 
  • Galo J. A. A. Soler-Illia*
    Galo J. A. A. Soler-Illia
    Instituto de Nanosistemas, UNSAM, CONICET, Avenida 25 de Mayo 1021, 1650 San Martín, Buenos Aires, Argentina
    *E-mail: [email protected]; [email protected]
Cite this: Langmuir 2019, 35, 19, 6279–6287
Publication Date (Web):April 15, 2019
https://doi.org/10.1021/acs.langmuir.9b00224
Copyright © 2019 American Chemical Society

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    Abstract

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    Mesoporous oxide thin films (MOTF) present very high surface areas and highly controlled monodisperse pores in the nanometer range. These features spurred their possible applications in separation membranes and permselective electrodes. However, their performance in real applications is limited by their reactivity. Here, we perform a basic study of the stability of MOTF toward dissolution in aqueous media using a variety of characterization techniques. In particular, we focus in their stability behavior under the influence of ionic strength, adsorption of electrochemical probes, and applied electrode potential. Mesoporous silica thin films present a limited chemical stability after electrochemical cycling, particularly under high ionic strength, due to their high specific surface area and the interactions between the electrochemical probes and the surface. In contrast, TiO2 or Si0.9Zr0.1O2 matrices present higher stability; thus, they are an adequate alternative to produce accessible, sensitive, and robust permselective electrodes or membranes that perform under a wide variety of conditions.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.langmuir.9b00224.

    • Film thicknesses, voltammograms, peak current, pore and neck size distributions, peak current density, and SEM image of Si0.9Zr0.1O2 MOTF surface over gold electrode (PDF)

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