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Modulating Iridium Coordination to Control the Oxygen Evolution Reaction Pathway.

Wenrui Li1, Jiajia Zhang1, Chenyu Yang2

  • 1Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Key Laboratory of Cluster Science, Ministry of Education, Frontiers Science Center for High Energy Material, Advanced Technology Research Institute (Jinan), School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, P. R. China.

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|October 22, 2025
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Summary
This summary is machine-generated.

Researchers engineered iridium-doped cobalt oxide catalysts by precisely controlling the coordination number of iridium active sites. This strategy enhances the lattice oxygen mechanism (LOM) for the oxygen evolution reaction (OER), leading to superior catalytic activity and stability.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • The oxygen evolution reaction (OER) is crucial for energy conversion technologies.
  • Tailoring active site coordination can shift OER pathways from adsorbate evolution mechanism (AEM) to the more active lattice oxygen mechanism (LOM).
  • Effective synthesis strategies for controlling coordination environments are needed.

Purpose of the Study:

  • To develop a phase transformation strategy for precise engineering of iridium (Ir) coordination numbers in zeolitic imidazolate frameworks (ZIFs).
  • To investigate the impact of different Ir coordination numbers on the OER pathway and performance.
  • To establish a correlation between coordination environment and catalytic activity for OER.

Main Methods:

  • Phase transformation of Ir-loaded ZIFs via air calcination to produce Ir-doped Co3O4 with distinct Ir coordination numbers (Ir1Ox-Co3O4, x=4, 6).
  • Comprehensive electrochemical characterization to evaluate OER performance (overpotential, stability, mass activity).
  • Analysis of reaction mechanisms, including density functional theory calculations and in-situ spectroscopic studies (implied).

Main Results:

  • Successfully synthesized two types of Ir-doped Co3O4 catalysts: Ir1O6-Co3O4 and Ir1O4-Co3O4, with different Ir coordination numbers.
  • Ir1O6-Co3O4, with a higher coordination number, promotes the dual-metal-site lattice oxygen mechanism (DMSM-LOM), exhibiting lower overpotential (253 mV at 10 mA cm-2) and enhanced stability (>200 h).
  • Ir1O6-Co3O4 demonstrated significantly higher mass activity compared to Ir1O4-Co3O4 and commercial IrO2 (3.4x and 17.3x, respectively).

Conclusions:

  • The phase transformation strategy effectively engineers the coordination number of active sites for OER.
  • A higher Ir coordination number in Ir1O6-Co3O4 facilitates the DMSM-LOM pathway, leading to superior OER performance.
  • This work provides insights into rational catalyst design for high-performance OER by correlating coordination environment with reaction mechanisms.