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Pt Particles on a Dynamic TiO2 Support in Near-Ambient Conditions-Disentangling Size, Pressure, and Support Effects.

Florian Kraushofer1, Matthias Krinninger1, Marina de la Higuera-Domingo1

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Platinum (Pt) nanoparticles on titanium dioxide (TiO2) exhibit dynamic structural changes under varying oxygen pressures. Support stoichiometry significantly influences Pt oxidation and stability, impacting real catalyst behavior.

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Area of Science:

  • Surface Science
  • Catalysis
  • Materials Science

Background:

  • Platinum (Pt) catalysts on reducible oxide supports, like titanium dioxide (TiO2), form complex, dynamic structures under reaction conditions.
  • These active structures often differ significantly from those observed under ultrahigh vacuum (UHV) or at room temperature.
  • Understanding the oxidation and structural evolution of Pt/TiO2 is crucial for designing efficient catalysts for various chemical reactions.

Purpose of the Study:

  • To investigate the oxidation and structural evolution of subnanometer Pt clusters and nanoparticles on rutile TiO2(110).
  • To examine the influence of oxygen pressure (UHV to 0.1 mbar) and support stoichiometry on Pt behavior.
  • To compare model single-crystal systems with a real-world Pt/TiO2 powder catalyst (P25).

Main Methods:

  • Near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) to probe surface composition and oxidation states.
  • Scanning tunneling microscopy (STM) under UHV and NAP conditions to visualize surface morphology and structure.
  • Low-energy ion scattering (LEIS) for surface-sensitive elemental analysis.

Main Results:

  • Distinct oxidation behaviors and thermal stabilities were observed for Pt nanoparticles versus Pt clusters.
  • Small Pt clusters readily oxidize at room temperature and sinter at 0.1 mbar O2 and elevated temperatures.
  • Well-crystallized Pt nanoparticles on stoichiometric TiO2 showed less oxidation, while those on reduced TiO2 were encapsulated by reoxidized titania layers, differing from classical strong metal-support interaction (SMSI) encapsulation.

Conclusions:

  • Support stoichiometry critically modulates the oxidation state and structural dynamics of Pt nanoparticles and clusters on TiO2.
  • The encapsulation mechanism on reduced TiO2 involves gas-phase interactions, distinct from SMSI.
  • Careful control of model support stoichiometry is essential for accurately replicating the behavior of powder catalysts during redox reactions.