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Pt Nanoparticle Disintegration at Oxide Interfaces Enhances CO Oxidation Catalysis.

Eunji Kang1, Jieun Yun1, Hyuk Choi1

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Supported platinum nanoparticles (NPs) disintegrate into single atoms (SAs) on ceria-titania during CO oxidation. This dynamic transformation, driven by interfacial oxygen, enhances catalytic activity, offering new avenues for catalyst design.

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CO oxidationdynamic structural evolutionheterogeneous catalysisin situ X‐ray analysisinterfacesingle atom catalyst

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Area of Science:

  • Materials Science
  • Catalysis
  • Surface Chemistry

Background:

  • Supported metal nanoparticles (NPs) are crucial in catalysis, but their dynamic evolution under reaction conditions remains poorly understood.
  • Controlling nanoparticle morphology is key to optimizing catalytic function.

Purpose of the Study:

  • To elucidate the mechanism of dynamic disintegration of platinum nanoparticles (Pt NPs) supported on ceria-x-titania (CT).
  • To understand how this disintegration leads to the formation of single atoms (SAs) and sub-nanometer clusters during CO oxidation.
  • To correlate structural changes with catalytic performance.

Main Methods:

  • Density Functional Theory (DFT) calculations to investigate Pt-CO interactions and stabilization mechanisms.
  • In situ spectroscopic analyses to monitor nanoparticle transformation under reaction conditions.
  • Kinetic trapping and surface diffusion studies involving oxygen vacancies.

Main Results:

  • Strong Pt-CO interactions weaken Pt-Pt cohesion, facilitating NP disintegration.
  • Electronic coupling between Pt and Ce ions stabilizes intermediates at the oxide interface.
  • Oxygen vacancies play a role in trapping intermediates, with replenishment enabling surface diffusion and reorganization.
  • Observed oxygen-driven transformation of Pt NPs correlated with a threefold increase in mass-specific activity at 150°C.

Conclusions:

  • Interfacial oxygen dynamics and metal-support interactions can induce nanoparticle disintegration.
  • This process can be leveraged to optimize catalytic performance by forming single atoms or clusters.
  • Interface-engineered Pt nanostructures show significant catalytic potential.