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Boosting water oxidation layer-by-layer.

Jonnathan C Hidalgo-Acosta1, Micheál D Scanlon, Manuel A Méndez

  • 1Laboratoire d'Electrochimie Physique et Analytique (LEPA), École Polytechnique Fédérale de Lausanne (EPFL), Valais Wallis, Rue de l'Industrie 17, Case Postale 440, 1951 Sion, Switzerland. hubert.girault@epfl.ch.

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Summary
This summary is machine-generated.

This study demonstrates a novel method for electrocatalysis of water oxidation using iridium oxide nanoparticles (IrO2 NPs) layered with a polymer on fluorinated tin oxide electrodes. This approach offers tunable surface coverage and efficient oxygen evolution across a wide pH range.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Nanotechnology

Background:

  • Electrocatalysis is crucial for water splitting and renewable energy technologies.
  • Developing efficient and stable electrocatalysts for the oxygen evolution reaction (OER) remains a significant challenge.
  • Iridium oxide (IrO2) is a promising OER catalyst, but its application in stable electrode architectures needs further investigation.

Purpose of the Study:

  • To develop a novel layer-by-layer (LbL) assembly method for fabricating iridium oxide nanoparticle (IrO2 NP) modified electrodes.
  • To investigate the effect of LbL deposition on IrO2 NP surface coverage and electrochemical properties.
  • To evaluate the electrocatalytic performance and stability of the modified electrodes for the oxygen evolution reaction (OER) across various pH conditions.

Main Methods:

  • Fabrication of modified electrodes using layer-by-layer deposition of citrate-stabilized IrO2 NPs and poly(diallyldimethylammonium chloride) (PDDA) on fluorinated tin oxide (FTO) substrates.
  • Characterization of IrO2 NP films using UV/vis spectroscopy and spectro-electrochemical techniques to determine surface coverage.
  • Electrochemical evaluation of the modified electrodes for OER activity, including cyclic voltammetry and bulk electrolysis across a pH range (1-13).

Main Results:

  • LbL deposition allowed fine-tuning of IrO2 NP surface coverage, increasing linearly with the number of bilayers.
  • The modified electrodes exhibited voltammetric behavior characteristic of hydrous iridium oxide films with a pH-independent OER overpotential (0.22–0.28 V at 0.1 mA cm(-2)).
  • The IrO2/PDDA films showed excellent stability and high Faradaic efficiencies (approaching 100%) for OER in acidic and neutral conditions, with good performance in alkaline solutions (88%).

Conclusions:

  • The LbL approach provides a versatile platform for controlled fabrication of IrO2 NP-based electrocatalysts for OER.
  • The developed electrodes demonstrate efficient and stable oxygen evolution with minimal pH dependence, highlighting their potential for various electrochemical applications.
  • This method lays the groundwork for scalable OER electrode development using advanced deposition techniques like inkjet printing.