Methanol Partial Oxidation on Ag(1 1 1) from First Principles

Hassan Aljama, Jong Suk Yoo, Jens K. Nørskov, Frank Abild-Pedersen, Felix Studt

Research output: Contribution to journalArticlepeer-review

15 Scopus citations

Abstract

In this work, we examine the thermochemistry and kinetics of the partial oxidation of methanol to formaldehyde on silver surfaces. Periodic density functional theory calculations employing the BEEF-vdW functional are used to identify the most stable phases of the silver surface under relevant reaction conditions and the reaction energetics are obtained on these surfaces. The calculated binding energies and transition state energies are used as input in a mean-field microkinetic model providing the reaction kinetics on silver surfaces under different reaction conditions. Our results show that, under conditions pertaining to methanol partial oxidation, oxygen is present at low concentrations and it plays a critical role in the catalytic reaction. Surface oxygen promotes the reaction by activating the OH bond in methanol, thus forming a methoxy intermediate, which can react further to form formaldehyde. The dissociation of molecular oxygen is identified as the most critical step.

Original languageEnglish
Pages (from-to)3621-3625
Number of pages5
JournalChemCatChem
Volume8
Issue number23
DOIs
StatePublished - 7 Dec 2016

Keywords

  • density functional theory calculations
  • heterogeneous catalysis
  • methanol
  • microkinetic model
  • oxidation

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