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A Water-Promoted Mars-van Krevelen Reaction Dominates Low-Temperature CO Oxidation over Au-Fe2O3 but Not over Au-TiO2.
Holm, Alexander; Davies, Bernadette; Boscolo Bibi, Sara; Moncada, Felix; Halldin-Stenlid, Joakim; Paskevicius, Laurynas; Claman, Vincent; Slabon, Adam; Tai, Cheuk-Wai; Campos Dos-Santos, Egon; Koroidov, Sergey.
Afiliação
  • Holm A; Department of Physics, AlbaNova University Center, Stockholm University, 106 91 Stockholm, Sweden.
  • Davies B; Department of Materials and Environmental Chemistry, Stockholm University, Svante Arrhenius väg 16C, 114 18 Stockholm, Sweden.
  • Boscolo Bibi S; Laboratory of Organic Electronics, Department of Science and Technology (ITN), Linköping University, Norrköping, SE-60174 Sweden.
  • Moncada F; Department of Physics, AlbaNova University Center, Stockholm University, 106 91 Stockholm, Sweden.
  • Halldin-Stenlid J; Department of Materials and Environmental Chemistry, Stockholm University, Svante Arrhenius väg 16C, 114 18 Stockholm, Sweden.
  • Paskevicius L; Department of Physics, AlbaNova University Center, Stockholm University, 106 91 Stockholm, Sweden.
  • Claman V; Department of Physics, AlbaNova University Center, Stockholm University, 106 91 Stockholm, Sweden.
  • Slabon A; KBR, Inc., Intelligent Systems Division, NASA Ames Research Center, Moffett Field, California 94035, United States.
  • Tai CW; Department of Physics, AlbaNova University Center, Stockholm University, 106 91 Stockholm, Sweden.
  • Campos Dos-Santos E; Department of Physics, AlbaNova University Center, Stockholm University, 106 91 Stockholm, Sweden.
  • Koroidov S; Department of Materials and Environmental Chemistry, Stockholm University, Svante Arrhenius väg 16C, 114 18 Stockholm, Sweden.
ACS Catal ; 14(5): 3191-3197, 2024 Mar 01.
Article em En | MEDLINE | ID: mdl-38449533
ABSTRACT
We provide experimental evidence that is inconsistent with often proposed Langmuir-Hinshelwood (LH) mechanistic hypotheses for water-promoted CO oxidation over Au-Fe2O3. Passing CO and H2O, but no O2, over Au-γ-Fe2O3 at 25 °C, we observe significant CO2 production, inconsistent with LH mechanistic hypotheses. Experiments with H218O further show that previous LH mechanistic proposals cannot account for water-promoted CO oxidation over Au-γ-Fe2O3. Guided by density functional theory, we instead postulate a water-promoted Mars-van Krevelen (w-MvK) reaction. Our proposed w-MvK mechanism is consistent both with observed CO2 production in the absence of O2 and with CO oxidation in the presence of H218O and 16O2. In contrast, for Au-TiO2, our data is consistent with previous LH mechanistic hypotheses.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Ano de publicação: 2024 Tipo de documento: Article