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CO oxidation on electrically charged gold nanotips.

J-S McEwen1, P Gaspard

  • 1Center for Nonlinear Phenomena and Complex Systems, Université Libre de Bruxelles, Code Postal 231, Campus Plaine, B-1050 Brussels, Belgium. jmcewen@ulb.ac.be

The Journal of Chemical Physics
|December 15, 2006
PubMed
Summary

We studied carbon monoxide (CO) oxidation on gold nanotips under strong electric fields. CO oxidation occurs on negatively charged gold clusters, influenced by field-dependent oxygen and CO binding.

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Area of Science:

  • Surface science
  • Physical chemistry
  • Nanotechnology

Background:

  • Carbon monoxide (CO) oxidation is a critical reaction in catalysis.
  • Understanding surface reactions under external stimuli like electric fields is crucial.
  • Gold nanoparticles exhibit unique catalytic properties.

Purpose of the Study:

  • To investigate the oxidation of CO on a gold nanotip under high electrostatic fields.
  • To develop a kinetic model explaining the field-dependent reaction mechanism.
  • To correlate experimental observations with theoretical predictions.

Main Methods:

  • Density Functional Theory (DFT) calculations to determine binding energies as a function of electric field.
  • Development of a field-dependent kinetic model based on the Langmuir-Hinshelwood mechanism.
  • Analysis of field ion microscopy experimental data.

Main Results:

  • Dissociative adsorption of oxygen on gold occurs only below a negative critical electric field value.
  • Binding of CO on gold is enhanced for positive electric field values.
  • The model explains wave propagation observed in field ion microscopy.

Conclusions:

  • CO oxidation on gold nanotips is strongly influenced by electrostatic fields.
  • The reaction is predicted to occur preferentially on negatively charged gold clusters.
  • This study provides insights into field-controlled catalysis on nanomaterials.