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Area of Science:

  • Surface science
  • Computational chemistry
  • Chemical kinetics

Background:

  • Adsorbates on surfaces exhibit lateral interactions, leading to a distribution of adsorption energies.
  • These adsorbate-adsorbate interactions significantly impact surface reaction kinetics, necessitating accurate modeling.
  • Understanding these interactions is crucial for developing predictive models in surface chemistry.

Purpose of the Study:

  • To investigate the effect of adsorbate distribution on carbon monoxide (CO) adsorption and desorption from a platinum (Pt(111)) surface.
  • To develop and validate a computational model that accurately accounts for adsorbate-adsorbate interactions.
  • To provide a guideline for incorporating these interactions into existing kinetic models.

Main Methods:

  • Utilizing density functional theory (DFT) calculations to determine adsorption energies.
  • Employing Monte Carlo simulations to model adsorbate behavior and surface processes.
  • Comparing simulated results with experimental data from calorimetry and temperature-programmed desorption.

Main Results:

  • The mean of the average adsorption energy governs the adsorption process of CO on Pt(111).
  • The low-energy portion of the adsorbate stability distribution effectively describes the desorption process.
  • Simulated results show excellent agreement with experimental measurements.

Conclusions:

  • Adsorbate-adsorbate interactions are critical for accurately modeling adsorption and desorption kinetics.
  • The developed model successfully captures the influence of adsorbate distribution on CO surface processes.
  • This work offers a framework for enhancing density functional theory-based mean-field kinetic models by including lateral interactions.