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

Boix, Virginia LU ; Xu, Wenbin ; D'Acunto, Giulio LU ; Stubbe, Johannes ; Gallo, Tamires LU ; Døvre Strømsheim, Marie ; Zhu, Suyun LU ; Scardamaglia, Mattia LU ; Shavorskiy, Andrey LU and Reuter, Karsten , et al. (2022) In Journal of Physical Chemistry C 126(33). p.14116-14124
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... (More)

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.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Physical Chemistry C
volume
126
issue
33
pages
9 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:36060283
  • scopus:85136645535
ISSN
1932-7447
DOI
10.1021/acs.jpcc.2c02293
language
English
LU publication?
yes
id
77722895-f2e2-47c4-9ea4-7faeb22341e9
date added to LUP
2022-10-18 15:35:13
date last changed
2025-03-21 18:38:48
@article{77722895-f2e2-47c4-9ea4-7faeb22341e9,
  abstract     = {{<p>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 O<sub>2</sub>exposure 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 O<sub>2</sub>molecule. 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.</p>}},
  author       = {{Boix, Virginia and Xu, Wenbin and D'Acunto, Giulio and Stubbe, Johannes and Gallo, Tamires and Døvre Strømsheim, Marie and Zhu, Suyun and Scardamaglia, Mattia and Shavorskiy, Andrey and Reuter, Karsten and Andersen, Mie and Knudsen, Jan}},
  issn         = {{1932-7447}},
  language     = {{eng}},
  month        = {{08}},
  number       = {{33}},
  pages        = {{14116--14124}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Journal of Physical Chemistry C}},
  title        = {{Graphene as an Adsorption Template for Studying Double Bond Activation in Catalysis}},
  url          = {{http://dx.doi.org/10.1021/acs.jpcc.2c02293}},
  doi          = {{10.1021/acs.jpcc.2c02293}},
  volume       = {{126}},
  year         = {{2022}},
}