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Free gold clusters: beyond the static, monostructure description.

Elizabeth C Beret1, Luca M Ghiringhelli, Matthias Scheffler

  • 1Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Dahlem, Germany.

Faraday Discussions
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PubMed
Summary
This summary is machine-generated.

This study explores the stability and behavior of gold clusters, revealing entropic effects influence their structure and identifying a reaction pathway for CO oxidation catalysis.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Computational Chemistry

Background:

  • Understanding the thermodynamic stability of gold clusters is crucial for catalysis.
  • Gold clusters exhibit complex structural dynamics, especially at finite temperatures.
  • The interaction of gold clusters with atmospheric gases like O2 and CO influences their catalytic activity.

Purpose of the Study:

  • To investigate the thermodynamical stability of free gold clusters and cluster+ligands complexes.
  • To elucidate the structural preferences (3D vs. planar) of Au13 clusters at finite temperatures.
  • To identify potential reaction pathways for CO oxidation catalyzed by small gold clusters in an O2 + CO atmosphere.

Main Methods:

  • Utilizing parallel tempering and ab initio atomistic thermodynamics for stability studies.
  • Analyzing the fluxional behavior of the Au13 cluster across a range of temperatures.
  • Applying thermodynamic principles to model cluster-gas interactions and catalytic pathways.

Main Results:

  • Au13 clusters display significant fluxional behavior, with multiple structures dynamically interconverting even at 100 K.
  • Entropic effects dictate the preference for three-dimensional over planar structures for Au13 at finite temperatures.
  • A likely reaction pathway for CO oxidation catalyzed by small gold clusters (Au1-4) has been identified.

Conclusions:

  • Thermodynamical stability and structural dynamics of gold clusters are temperature-dependent and influenced by entropy.
  • Small gold clusters can catalyze the oxidation of CO in the presence of O2.
  • The identified reaction path provides insights into gold-catalyzed oxidation mechanisms.