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Cation Substitution in High-Entropy Layered Double Hydroxide Driving D-Band Center Tuning for Oxygen Evolution

Pinnan Li1, Jingwei Li2, Christophe Colbeau-Justin1

  • 1Université Paris-Saclay, CNRS UMR 8000, Institut de Chimie Physique, Orsay, 91400, France.

Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|November 20, 2025
PubMed
Summary

This study optimized high-entropy layered double hydroxides (HE-LDHs) as electrocatalysts for the oxygen evolution reaction (OER). Tuning the d-band center position significantly reduced OER overpotential, enhancing catalytic efficiency.

Keywords:
OERd‐band centerhigh‐entropy layered double hydroxideprecious‐metals‐free electrocatalyst

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Optimizing electrocatalysts for the oxygen evolution reaction (OER) requires balancing intermediate adsorption and energy barriers.
  • High-entropy layered double hydroxides (HE-LDHs) offer tunable electronic structures for catalytic applications.

Purpose of the Study:

  • To modulate the d-band center position of HE-LDHs by incorporating various transition metals.
  • To investigate the effect of d-band center tuning on OER kinetics and overpotential.

Main Methods:

  • Substitution of Mg²⁺ sites in HE-LDHs with Fe²⁺, Cu²⁺, Co²⁺, and Ni²⁺.
  • Characterization of the electronic structure and OER performance of the modified HE-LDHs.

Main Results:

  • The d-band center position was successfully tuned, achieving optimal energy in (FeCuCoNi)₆Al₂-LDH.
  • Incorporated transition metals significantly influenced OH⁻ adsorption and reduced OER overpotential by 55% compared to native LDH.
  • Stepwise substitution, particularly with Fe²⁺, induced charge carrier transfer, enhancing OER kinetics.

Conclusions:

  • Adjusting the d-band center position via multication insertion is an effective strategy to decrease OER overpotential.
  • Tuning the d-band center shifts materials towards optimal binding strength, improving catalytic performance.
  • This approach provides a pathway for designing efficient electrocatalysts for OER.