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Area of Science:

  • Materials Science
  • Catalysis
  • Surface Chemistry

Background:

  • Atomically dispersed metals on oxide supports are crucial for catalysis, but their precise roles and reactivity remain debated.
  • Understanding the behavior of single atoms versus clusters or nanoparticles on supports like ceria is challenging.
  • Controversies exist regarding the reactivity and stability of supported single atoms, especially on ceria.

Purpose of the Study:

  • To differentiate and understand the distinct behaviors of atomically dispersed platinum (Pt) on ceria supports.
  • To investigate how different anchoring sites and mobilities of single Pt atoms influence their catalytic activity.
  • To clarify the role of surface defects and activation treatments on the stability and reactivity of single Pt atoms.

Main Methods:

  • Strong electrostatic adsorption was used to load Pt single atoms onto conventionally synthesized ceria supports.
  • Modulation of Pt loading amounts was employed to obtain different atomically dispersed Pt species.
  • Reduction-reoxidation treatments were utilized to assess the stability and mobility of the single Pt atoms.
  • CO oxidation reaction was performed to evaluate the catalytic activity of the different Pt species.

Main Results:

  • Two distinct types of atomically dispersed Pt atoms were successfully synthesized with similar Pt-O coordination and CO adsorption characteristics.
  • One type of Pt atom, anchored on the ceria surface, exhibited mobility and could aggregate into PtOx clusters upon activation, catalyzing CO oxidation.
  • The second type of Pt atom, trapped by ceria defects, remained isolated and stable during activation, showing no catalytic activity for CO oxidation.

Conclusions:

  • The location and mobility of single atoms on oxide supports significantly impact their catalytic performance.
  • Ceria surface defects can stabilize single Pt atoms, rendering them inactive for CO oxidation.
  • Careful control over single-atom loading and support interactions is essential for designing efficient heterogeneous catalysts.