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Area of Science:

  • Surface science
  • Chemical kinetics
  • Computational chemistry

Background:

  • Methane dissociation on transition metals is key to hydrogen production via steam reforming.
  • A specific reaction parameter functional (SRP32-vdW) has shown accuracy for normal incidence methane dissociation.

Purpose of the Study:

  • To validate the SRP32-vdW functional for off-normal incidence angles.
  • To investigate the angular dependence and site-specific reactivity of methane dissociation on Pt(211).

Main Methods:

  • Ab initio molecular dynamics calculations using the SRP32-vdW functional.
  • Comparison of calculated initial sticking coefficients (S0) with experimental King and Wells measurements.
  • Analysis of reactivity trends based on surface site coordination numbers.

Main Results:

  • SRP32-vdW accurately predicts initial sticking coefficients for CHD3 dissociation on Pt(211) at various incidence angles.
  • An asymmetry in reactivity was observed, with higher sticking coefficients when incidence is directed towards the (100) step edge.
  • Reactivity correlates with surface atom coordination, favoring less coordinated step sites.

Conclusions:

  • The SRP32-vdW functional is reliable for describing methane dissociation dynamics beyond normal incidence.
  • Surface step sites, particularly those with lower coordination, are preferential for methane dissociation.
  • Understanding site-specific reactivity is crucial for optimizing catalytic processes like steam reforming.