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dc.contributor.author
Corral-Pérez, Juan José
dc.contributor.author
Bansode, Atul
dc.contributor.author
Praveen, C.S.
dc.contributor.author
Kokalj, Anton
dc.contributor.author
Reymond, Helena
dc.contributor.author
Comas Vives, Aleix
dc.contributor.author
VandeVondele, Joost
dc.contributor.author
Copéret, Christophe
dc.contributor.author
Rudolf von Rohr, Philipp
dc.contributor.author
Urakawa, Atsushi
dc.date.accessioned
2018-11-08T08:10:12Z
dc.date.available
2018-10-16T12:36:40Z
dc.date.available
2018-10-16T13:12:32Z
dc.date.available
2018-11-07T15:13:09Z
dc.date.available
2018-11-08T08:10:12Z
dc.date.issued
2018-10-24
dc.identifier.issn
0002-7863
dc.identifier.issn
1520-5126
dc.identifier.other
10.1021/jacs.8b08505
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/296267
dc.identifier.doi
10.3929/ethz-b-000296267
dc.description.abstract
Methyl formate synthesis by hydrogenation of carbon dioxide in the presence of methanol offers a promising path to valorize carbon dioxide. In this work, silica-supported silver nanoparticles are shown to be a significantly more active catalyst for the continuous methyl formate synthesis than the known gold and copper counterparts, and the origin of the unique reactivity of Ag is clarified. Transient in situ and operando vibrational spectroscopy and DFT calculations shed light on the reactive intermediates and reaction mechanisms: a key feature is the rapid formation of surface chemical species in equilibrium with adsorbed carbon dioxide. Such species is assigned to carbonic acid interacting with water/hydroxyls on silica and promoting the esterification of formic acid with adsorbed methanol at the perimeter sites of Ag on SiO2 to yield methyl formate. This study highlights the importance of employing combined methodologies to verify the location and nature of active sites and to uncover fundamental catalytic reaction steps taking place at metal–support interfaces.
en_US
dc.format
application/pdf
en_US
dc.language.iso
en
en_US
dc.publisher
American Chemical Society (ACS)
en_US
dc.rights.uri
http://rightsstatements.org/page/InC-NC/1.0/
dc.title
Decisive Role of Perimeter Sites in Silica-Supported Ag Nanoparticles in Selective Hydrogenation of CO2 to Methyl Formate in the Presence of Methanol
en_US
dc.type
Journal Article
dc.rights.license
In Copyright - Non-Commercial Use Permitted
dc.date.published
2018-09-30
ethz.journal.title
Journal of the American Chemical Society
ethz.journal.volume
140
en_US
ethz.journal.issue
24
en_US
ethz.journal.abbreviated
J Am Chem Soc
ethz.pages.start
13884
en_US
ethz.pages.end
13891
en_US
ethz.version.deposit
publishedVersion
en_US
ethz.grant
Carbon Dioxide Hydrogenation: New Synthetic Perspectives for Chemical Energy Carriers
en_US
ethz.identifier.wos
ethz.identifier.scopus
ethz.publication.place
Washington, DC
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.::02629 - Institut für Verfahrenstechnik / Institute of Process Engineering::03348 - Rudolf von Rohr, Philipp (emeritus) / Rudolf von Rohr, Philipp (emeritus)
en_US
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.::02629 - Institut für Verfahrenstechnik / Institute of Process Engineering::03348 - Rudolf von Rohr, Philipp (emeritus) / Rudolf von Rohr, Philipp (emeritus)
en_US
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
154448
ethz.grant.fundername
SNF
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.program
ethz.date.deposited
2018-10-16T12:36:45Z
ethz.source
FORM
ethz.eth
yes
en_US
ethz.availability
Open access
en_US
ethz.rosetta.installDate
2018-11-07T15:13:18Z
ethz.rosetta.lastUpdated
2019-02-03T08:37:54Z
ethz.rosetta.exportRequired
true
ethz.rosetta.versionExported
true
ethz.COinS
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