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dc.contributor.author
Castro-Fernández, Pedro
dc.contributor.author
Mance, Deni
dc.contributor.author
Liu, Chong
dc.contributor.author
Abdala, Paula Macarena
dc.contributor.author
Willinger, Elena
dc.contributor.author
Rossinelli, Aurelio A.
dc.contributor.author
Serykh, Alexander I.
dc.contributor.author
Pidko, Evgeny A.
dc.contributor.author
Copéret, Christophe
dc.contributor.author
Fedorov, Alexey
dc.contributor.author
Müller, Christoph R.
dc.date.accessioned
2022-06-17T05:56:13Z
dc.date.available
2022-03-25T06:19:34Z
dc.date.available
2022-06-17T05:56:13Z
dc.date.issued
2022-04
dc.identifier.issn
0021-9517
dc.identifier.issn
1090-2694
dc.identifier.other
10.1016/j.jcat.2022.02.025
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/539225
dc.identifier.doi
10.3929/ethz-b-000539225
dc.description.abstract
Three γ/β-Ga2O3 nanoparticle catalysts that differ in the relative ratio of γ-Ga2O3 to β-Ga2O3 were prepared to evaluate the effect of H2 treatment (500 °C, 2 h) on the coordination environment of bulk and surface Ga sites, Lewis acidity and catalytic activity in propane dehydrogenation (PDH). Independent of the H2 treatment, the initial PDH activity of the γ/β-Ga2O3 catalysts increases with the fraction of the β-Ga2O3 phase. This is explained by the presence of weak Lewis acid sites (LAS) in β-Ga2O3 while such sites are absent in γ-Ga2O3. Treatment with H2 increases the catalytic activity of all three γ/β-Ga2O3 catalysts but for different reasons. For catalysts with higher fractions of β-Ga2O3, H2 treatment increases further the relative abundance of weak LAS, likely by generating coordinatively unsaturated Ga sites (such as tricoordinated Ga sites nearby oxygen vacancies). In contrast, H2 treatment of a catalyst containing a predominant fraction of γ-Ga2O3 phase induces disorder in the sub-surface structure of the nanoparticle, that is, it forms gallium and oxygen vacancies in the bulk and favors migration of gallium, and likely also of oxygen, to the surface. This induces a surface reconstruction that notably increases the fraction of strong LAS (and proportionally decreases the fraction of medium LAS), while creating no weak LAS in γ-Ga2O3-H2. Therefore, the increase in the catalytic activity of H2-treated γ-Ga2O3 is explained by the higher density of surface Ga sites in γ-Ga2O3-H2 relative to calcined γ-Ga2O3. H2-treated catalysts that contain a higher relative amount of weak LAS also feature a higher relative abundance of gallium hydride species associated with a low frequency FTIR band at ca. 1931–1939 cm−1, that is, weak LAS likely give weakly-bound hydrides in β-Ga2O3. Our results highlight that weak LAS in unsupported Ga2O3 catalysts are more active in PDH than mild or strong LAS.
en_US
dc.format
application/pdf
en_US
dc.language.iso
en
en_US
dc.publisher
Elsevier
en_US
dc.rights.uri
http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.subject
Propane dehydrogenation
en_US
dc.subject
Gallium oxide
en_US
dc.subject
Oxygen vacancies
en_US
dc.subject
Lewis acidity
en_US
dc.subject
Surface reconstruction
en_US
dc.title
Bulk and surface transformations of Ga2O3 nanoparticle catalysts for propane dehydrogenation induced by a H2 treatment
en_US
dc.type
Journal Article
dc.rights.license
Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
dc.date.published
2022-03-19
ethz.journal.title
Journal of Catalysis
ethz.journal.volume
408
en_US
ethz.journal.abbreviated
J Catal
ethz.pages.start
155
en_US
ethz.pages.end
164
en_US
ethz.version.deposit
publishedVersion
en_US
ethz.grant
Advancing CO2 Capture Materials by Atomic Scale Design: the Quest for Understanding
en_US
ethz.identifier.scopus
ethz.publication.place
San Diego, CA
en_US
ethz.publication.status
published
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02130 - Dep. Maschinenbau und Verfahrenstechnik / Dep. of Mechanical and Process Eng.::02668 - Inst. f. Energie- und Verfahrenstechnik / Inst. Energy and Process Engineering::03865 - Müller, Christoph R. / Müller, Christoph R.
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02513 - Laboratorium für Anorganische Chemie / Laboratory of Inorganic Chemistry::03872 - Copéret, Christophe / Copéret, Christophe
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02130 - Dep. Maschinenbau und Verfahrenstechnik / Dep. of Mechanical and Process Eng.::02668 - Inst. f. Energie- und Verfahrenstechnik / Inst. Energy and Process Engineering::03865 - Müller, Christoph R. / Müller, Christoph R.
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02513 - Laboratorium für Anorganische Chemie / Laboratory of Inorganic Chemistry::03872 - Copéret, Christophe / Copéret, Christophe
ethz.grant.agreementno
819573
ethz.grant.fundername
EC
ethz.grant.funderDoi
10.13039/501100000780
ethz.grant.program
H2020
ethz.date.deposited
2022-03-25T06:19:44Z
ethz.source
SCOPUS
ethz.eth
yes
en_US
ethz.availability
Open access
en_US
ethz.rosetta.installDate
2022-06-17T05:56:19Z
ethz.rosetta.lastUpdated
2023-02-07T03:34:52Z
ethz.rosetta.versionExported
true
ethz.COinS
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