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Donnan permselectivity in layer-by-layer self-assembled redox polyelectrolye thin films.

Ernesto J Calvo1, Alejandro Wolosiuk

  • 1INQUIMAE, Departamento de Química Inorgánica, Analítica y Química Física, Facultad de Ciencias Exactas y Naturales, Pabellón 2 Ciudad Universitaria, AR-1428 Buenos Aires, Argentina. calvo@q1.fcen.uba.ar

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Summary

Redox polyelectrolyte multilayers exhibit tunable electrochemical properties. Ion and solvent exchange, monitored by electrochemical quartz crystal microbalance, depend on film charge, pH, and electrolyte concentration, influencing redox potential.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Polymer Science

Background:

  • Layer-by-layer (LBL) deposition is a versatile technique for assembling redox polyelectrolyte multilayers.
  • Osmium-based redox polymers are crucial for electrochemical applications, but their behavior in multilayer films requires detailed investigation.
  • Understanding ion and solvent transport within these films is essential for controlling their electrochemical response.

Purpose of the Study:

  • To investigate the electrochemical behavior of redox polyelectrolyte multilayers assembled using LBL deposition.
  • To explore the influence of electrolyte concentration, pH, and outermost layer charge on the redox potential of the Os(II)/Os(III) couple.
  • To characterize ion and solvent exchange during redox switching using electrochemical quartz crystal microbalance (EQCM).

Main Methods:

  • Layer-by-layer (LBL) deposition to assemble multilayer films using cationic poly(allylamine) modified with Os(bpy)(2)ClPyCHO (PAH-Os) and anionic poly(styrene)sulfonate (PSS) or poly(vinyl)sulfonate (PVS).
  • Cyclic voltammetry to determine the formal redox potential of the Os(II)/Os(III) couple.
  • Electrochemical quartz crystal microbalance (EQCM) to monitor mass changes associated with ion and solvent exchange.

Main Results:

  • Formal redox potential of the Os(II)/Os(III) couple is sensitive to the outermost layer's charge, electrolyte concentration, and pH.
  • At low ionic strength, Donnan permselectivity governs ion exclusion, dependent on film charge and pH.
  • At high electrolyte concentrations, Donnan breakdown occurs, and redox potential approaches the solution value. EQCM revealed distinct ion and water exchange mechanisms under permselective and Donnan breakdown conditions.

Conclusions:

  • Redox polyelectrolyte multilayers offer tunable electrochemical properties through control of assembly conditions and environment.
  • Donnan equilibrium principles explain ion transport at low electrolyte concentrations, while high concentrations lead to film swelling and altered ion transport.
  • EQCM is a powerful tool for elucidating the complex interplay between redox switching, ion flux, and solvent uptake in polyelectrolyte multilayers.