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Local Hollandite Phase Inducing Oxygen Path Mechanism Enables Durable PEM Electrolysis.

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Summary

Developing new catalysts for proton-exchange-membrane water electrolyzers (PEMWEs) is key for green hydrogen. This study introduces a novel (La)IrOx catalyst that enhances the oxide path mechanism, enabling efficient and stable hydrogen production with reduced iridium use.

Keywords:
amorphous iridium oxideshigh‐valence Ir specieshollandite phaseoxygen evolution reactionoxygen path mechanism

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Proton-exchange-membrane water electrolyzers (PEMWEs) are crucial for green hydrogen, but iridium loading in anodes is a major obstacle.
  • Existing amorphous IrOx catalysts face limitations with either stability (lattice oxygen mechanism) or high overpotential (adsorbate evolution mechanism).
  • The oxide path mechanism (OPM) offers potential for direct *O─*O coupling but is difficult to activate in pure IrOx due to large Ir-Ir distances.

Purpose of the Study:

  • To develop a novel catalyst that facilitates the oxide path mechanism (OPM) for enhanced proton-exchange-membrane water electrolyzer (PEMWE) performance.
  • To overcome the limitations of existing catalysts by enabling efficient *O─*O coupling at reduced iridium loading.

Main Methods:

  • Synthesis of a porous amorphous (La)IrOx catalyst featuring a local unconventional hollandite phase.
  • Incorporation of abundant water molecules within the catalyst's lattice tunnels to influence its structure and activity.
  • Characterization of the catalyst's structure, including Ir-Ir distance and oxidation states, and evaluation in a PEMWE setup.

Main Results:

  • The unique short-range ordered structure of (La)IrOx shortens the Ir-Iredge distance and generates highly active Ir≥5+ species.
  • These structural modifications promote the oxide path mechanism (OPM), leading to significantly enhanced catalytic performance.
  • The assembled PEMWE demonstrated a low cell voltage (1.62 V at 1 A cm-2) with a low iridium loading (0.2 mgIr cm-2) and over 500 hours of stable operation.

Conclusions:

  • The developed (La)IrOx porous amorphous catalyst effectively utilizes the oxide path mechanism for efficient water splitting.
  • This catalyst offers a promising solution for durable and low-iridium proton-exchange-membrane water electrolyzers, crucial for green hydrogen production.
  • Further validation through accelerated stress tests at even lower iridium loading (0.1 mgIr cm-2) confirms its durability and potential viability.