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Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
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Published on: April 12, 2019

Ion-size effect within the aqueous solution interface at the Pt(111) surface: molecular dynamics studies.

Aljaž Godec1, Miran Gaberšček, Janko Jamnik

  • 1National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, Slovenia.

Physical Chemistry Chemical Physics : PCCP
|September 22, 2010
PubMed
Summary

Lithium ions stabilize interfacial water structure on platinum surfaces, hindering catalytic activity. This "freezing effect" of Li+ on water layers reduces access for other molecules, impacting reactions.

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Area of Science:

  • Computational Chemistry
  • Surface Science
  • Physical Chemistry

Background:

  • Understanding interfacial water structure is crucial for heterogeneous catalysis.
  • Electrolyte interactions at metal surfaces influence surface properties and reactivity.

Purpose of the Study:

  • To investigate the structure and dynamics of interfacial water at a platinum surface.
  • To elucidate the role of LiOH and KOH electrolytes on water ordering and ion adsorption.
  • To explain the impact of interfacial water modification on platinum catalytic activity.

Main Methods:

  • Employed all-atom classical force-field based molecular dynamics simulations.
  • Simulated pure water, 1 M LiOH, and 1 M KOH aqueous solutions.
  • Analyzed interfacial water structure and dynamics at an uncharged Pt(111) surface.

Main Results:

  • Water ordering extended up to 9 Å from the Pt surface, involving three molecular layers.
  • Both Li+ and K+ ions adsorbed directly onto the Pt surface.
  • Li+ ions significantly increased water-dipole autocorrelation and reduced translational motion, indicating a stabilizing effect on the water adlayer.

Conclusions:

  • Li+ ions exert a strong stabilizing influence on interfacial water molecules, akin to a 'freezing effect'.
  • This reduced water mobility impedes the access of other compounds to the Pt surface.
  • The observed 'freezing effect' of Li+ on interfacial water explains the reduced catalytic activity of Pt(111) in LiOH solutions.