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A Water-Promoted Mars-van Krevelen Reaction Dominates Low-Temperature CO Oxidation over Au-Fe2O3 but Not over Au-TiO2
Stockholm University, Faculty of Science, Department of Physics. Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). Linköping University, Sweden.ORCID iD: 0000-0002-3660-4389
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0001-7122-2231
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-1378-8760
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0001-9701-2099
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Number of Authors: 112024 (English)In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 14, no 5, p. 3191-3197Article in journal (Refereed) Published
Abstract [en]

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. 

Place, publisher, year, edition, pages
2024. Vol. 14, no 5, p. 3191-3197
Keywords [en]
CO oxidation, Mars−van Krevelen, Langmuir−Hinshelwood, mechanism, Au Fe2O3, TiO2
National Category
Physical Chemistry Inorganic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-227301DOI: 10.1021/acscatal.3c05978ISI: 001166445100001PubMedID: 38449533Scopus ID: 2-s2.0-85185599124OAI: oai:DiVA.org:su-227301DiVA, id: diva2:1845599
Available from: 2024-03-19 Created: 2024-03-19 Last updated: 2024-03-19Bibliographically approved

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Holm, AlexanderDavies, BernadetteBoscolo Bibi, SaraMoncada, FelixSlabon, AdamTai, Cheuk-WaiKoroidov, Sergey

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Holm, AlexanderDavies, BernadetteBoscolo Bibi, SaraMoncada, FelixSlabon, AdamTai, Cheuk-WaiKoroidov, Sergey
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Department of PhysicsDepartment of Materials and Environmental Chemistry (MMK)
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ACS Catalysis
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