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A computational study on the electrified Pt(111) surface by the cluster model.

Jian Yang1

  • 1Science Institute, University of Iceland, Dunhagi 3, 107 Reykjavík, Iceland. jianyang@hi.is.

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|March 1, 2019
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Summary
This summary is machine-generated.

Density functional theory investigated nitrogen monoxide (NO) adsorption and reduction on platinum (Pt) surfaces. The study found HNO is kinetically favored over NOH for NO reduction, with implications for electrochemical reactions.

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Area of Science:

  • Computational Chemistry
  • Surface Science
  • Electrochemistry

Background:

  • Nitrogen monoxide (NO) adsorption and reduction on platinum surfaces are crucial for catalytic converters and electrochemical applications.
  • Understanding the reaction mechanisms and intermediates is key to optimizing catalytic performance.

Purpose of the Study:

  • To investigate NO adsorption and reduction on a Pt37 cluster model of the Pt(111) surface using density functional theory.
  • To explore the influence of applied potential and solvation on NO reduction pathways.
  • To determine the relative stability and reactivity of surface intermediates like HNO and NOH.

Main Methods:

  • Density functional theory (DFT) calculations.
  • Application of a hemispherical cuboctahedral Pt37 cluster model.
  • Utilizing neutral charge and constant potential methods.
  • Incorporation of the Conductor-like Polarizable Continuum Model (CPCM) for solvation effects.

Main Results:

  • The Pt37 cluster model accurately reproduces experimental NO adsorption features on Pt(111).
  • The constant potential method with CPCM predicts potential-dependent reactivities.
  • HNO is found to be more stable at higher potentials and kinetically favored over NOH during NO reduction.
  • NOH is predicted to be unstable in aqueous solution compared to HNO.

Conclusions:

  • The study provides insights into the potential-dependent mechanisms of NO reduction on Pt(111) surfaces.
  • The Pt37 cluster model combined with electrochemical methods offers a reliable approach for studying surface reactions.
  • HNO is identified as a more favorable intermediate for NO reduction kinetics, influencing the overall reaction pathway towards ammonia formation.