Graphene as an Adsorption Template for Studying Double Bond Activation in Catalysis

Virginia Boix, Wenbin Xu, Giulio D'Acunto, Johannes Stubbe, Tamires Gallo, Marie Døvre Strømsheim, Suyun Zhu, Mattia Scardamaglia, Andrey Shavorskiy, Karsten Reuter, Mie Andersen, Jan Knudsen

Research output: Contribution to journalArticlepeer-review

Abstract

Hydrogenated graphene (H-Gr) is an extensively studied system not only because of its capabilities as a simplified model system for hydrocarbon chemistry but also because hydrogenation is a compelling method for Gr functionalization. However, knowledge of how H-Gr interacts with molecules at higher pressures and ambient conditions is lacking. Here we present experimental and theoretical evidence that room temperature O2exposure at millibar pressures leads to preferential removal of H dimers on H-functionalized graphene, leaving H clusters on the surface. Our density functional theory (DFT) analysis shows that the removal of H dimers is the result of water or hydrogen peroxide formation. For water formation, we show that the two H atoms in the dimer motif attack one end of the physisorbed O2molecule. Moreover, by comparing the reaction pathways in a vacuum with the ones on free-standing graphene and on the graphene/Ir(111) system, we find that the main role of graphene is to arrange the H atoms in geometrical positions, which facilitates the activation of the O═O double bond.

Original languageEnglish
Pages (from-to)14116-14124
Number of pages9
JournalJournal of Physical Chemistry C
Volume126
Issue number33
DOIs
Publication statusPublished - 2022 Aug 25

Subject classification (UKÄ)

  • Inorganic Chemistry
  • Condensed Matter Physics

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