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Understanding solid-gas reaction mechanisms by operando soft X-ray absorption spectroscopy at ambient pressure

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dc.contributor.author Braglia, Lucca
dc.contributor.author Fracchia, Martina
dc.contributor.author Ghigna, Paolo
dc.contributor.author Minguzzi, Alessandro
dc.contributor.author Meroni, Daniela
dc.contributor.author Edla, Raju
dc.contributor.author Vandichel, Matthias
dc.contributor.author Ahlberg, Elisabet
dc.contributor.author Cerrato, Giuseppina
dc.contributor.author Torelli, Piero
dc.date.accessioned 2020-07-27T15:09:41Z
dc.date.issued 2020
dc.identifier.citation Braglia, Luca,Fracchia, Martina,Ghigna, Paolo,Minguzzi, Alessandro,Meroni, Daniela,Edla, Raju,Vandichel, Matthias,Ahlberg, Elisabet,Cerrato, Giuseppina,Torelli, Piero (2020) 'Understanding Solid-gas Reaction Mechanisms by Operando Soft X-ray Absorption Spectroscopy at Ambient Pressure'. The Journal of Physical Chemistry C, . en_US
dc.identifier.issn 1932-7447
dc.identifier.uri http://hdl.handle.net/10344/9048
dc.description peer-reviewed en_US
dc.description The full text of this article will not be available in ULIR until the embargo expires on the 05/06/2021
dc.description.abstract Ambient-pressure operando soft X-ray absorption spectroscopy (soft-XAS) was applied to study the reactivity of hydroxylated SnO2 nanoparticles toward reducing gases. H2 was first used as a test case, showing that the gas phase and surface states can be simultaneously probed: Soft-XAS at the O K-edge gains sensitivity toward the gas phase, while at the Sn M4,5-edges, tin surface states are explicitly probed. Results obtained by flowing hydrocarbons (CH4 and CH3CHCH2) unequivocally show that these gases react with surface hydroxyl groups to produce water without producing carbon oxides and release electrons that localize on Sn to eventually form SnO. The partially reduced SnO2 – x layer at the surface of SnO2 is readily reoxidized to SnO2 by treating the sample with O2 at mild temperatures (>200 °C), revealing the nature of “electron sponge” of tin oxide. The experiments, combined with DFT calculations, allowed devising of a mechanism for dissociative hydrocarbon adsorption on SnO2, involving direct reduction of Sn sites at the surface via cleavage of C–H bonds and the formation of methoxy- and/or methyl-tin species at the surface. en_US
dc.language.iso eng en_US
dc.publisher American Chemical Society en_US
dc.relation.ispartofseries The Journal of Physical Chemistry C;124 (26), pp. 14202-14212
dc.relation.uri https://doi.org/10.1021/acs.jpcc.0c02546
dc.rights © 2020 ACS This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry C, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcc.0c02546 en_US
dc.subject solid gas reaction en_US
dc.title Understanding solid-gas reaction mechanisms by operando soft X-ray absorption spectroscopy at ambient pressure en_US
dc.type info:eu-repo/semantics/article en_US
dc.type.supercollection all_ul_research en_US
dc.type.supercollection ul_published_reviewed en_US
dc.date.updated 2020-07-27T14:57:40Z
dc.description.version ACCEPTED
dc.identifier.doi 10.1021/acs.jpcc.0c02546
dc.contributor.sponsor Italian Ministry of Research (MIUR) en_US
dc.relation.projectid 2017516
dc.relation.projectid 2017516
dc.date.embargoEndDate 2021-06-05
dc.embargo.terms 2021-06-05 en_US
dc.rights.accessrights info:eu-repo/semantics/embargoedAccess en_US
dc.internal.rssid 2958885
dc.internal.copyrightchecked Yes
dc.identifier.journaltitle The Journal of Physical Chemistry C
dc.description.status peer-reviewed


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