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Ligand-Mediated Nucleation and Growth of Palladium Metal Nanoparticles
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Σ3(111) Grain Boundaries Accelerate Hydrogen Insertion into Palladium Nanostructures.

K A U Madhushani1, Hyoju Park2, Hua Zhou3

  • 1Department of Chemistry, University of Utah, Salt Lake City, Utah 84112, United States.

Nano Letters
|October 10, 2025
PubMed
Summary

Grain boundaries (GBs) accelerate hydrogen absorption and release in palladium (Pd) nanostructures. This study reveals GBs are preferential sites for hydrogen insertion, enhancing metal hydride formation kinetics.

Keywords:
Grain BoundariesHydrogen InsertionPalladium NanostructuresTensile Strain

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Area of Science:

  • Materials Science
  • Nanotechnology
  • Physical Chemistry

Background:

  • Grain boundaries (GBs) are critical defect sites in nanomaterials.
  • Their role in metal hydride formation, particularly in palladium (Pd), is not fully understood.
  • Understanding GBs is crucial for developing advanced functional materials.

Purpose of the Study:

  • To investigate the influence of well-defined Σ3(111) grain boundaries (GBs) on hydrogen insertion in Pd nanostructures.
  • To elucidate the mechanisms governing hydrogen kinetics at GBs.
  • To explore GB-engineered Pd-based materials for enhanced hydride formation.

Main Methods:

  • Synthesis of Pd nanostructures enriched with Σ3(111) GBs using electrolysis-driven nanoparticle assembly.
  • In situ synchrotron X-ray diffraction to study hydriding/dehydriding kinetics.
  • Environmental transmission electron microscopy for strain mapping.
  • Density functional theory (DFT) calculations for mechanistic insights.

Main Results:

  • Pd nanostructures with GBs (PdGB) showed significantly faster hydriding and dehydriding kinetics.
  • Strain was localized at GBs and intensified upon hydrogen exposure, indicating preferential hydrogen insertion.
  • DFT calculations confirmed energetically favorable hydrogen insertion near GBs and the effect of tensile strain.

Conclusions:

  • Grain boundaries act as preferential sites for hydrogen insertion in palladium nanostructures.
  • GBs dramatically accelerate metal hydride formation and decomposition kinetics.
  • GB engineering offers a promising strategy for designing advanced Pd-based functional materials.