Cooperative defect-enriched SiO2 for oxygen activation and organic dehydrogenation

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dc.contributor.authorSaputera, Wibawa Hendra
dc.contributor.authorTahini, H. A.
dc.contributor.authorLovell, Emma
dc.contributor.authorTan, Tze Hao
dc.contributor.authorRawal, Aditya
dc.contributor.authorAguey-Zinsou, Kondo- Francois
dc.contributor.authorFriedmann, Donia
dc.contributor.authorSmith, Sean
dc.contributor.authorAmal, Rose
dc.contributor.authorScott, J
dc.date.accessioned2020-06-03T03:06:58Z
dc.date.issued2019
dc.date.updated2019-12-19T07:10:39Z
dc.description.abstractTailoring oxide functionalities via defect engineering is an effective approach in many advanced materials. Here we report that introducing defect sites in SiO2 via sequential hydrogenation and UV light pre-treatment steps can invoke synergism for oxygen activation and organic dehydrogenation under ambient conditions in the absence of light. The hydrogenation step is proposed to break SiOSi bonds to give an E′δ center – silanol pair. UV light pre-treatment then serves to dehydroxylate the silanol group to give a non-bridging oxygen hole centers (NBOHC). The two defect sites work in harmony to activate oxygen and in turn oxidize formic acid. First-principles calculations indicated that UV light pre-treatment lowered the energy barrier for oxygen activation and formic acid decomposition on the defect sites. Re-illuminating the used SiO2 led to partial recovery of the defect sites and hence oxidation performance. The study demonstrates the capacity for generating synergistic defects in simple metal oxides as an effective way to enhance performance for oxidation processes.en_AU
dc.description.sponsorshipThe work was supported by the Australian Research Council under The Laureate Fellowship Scheme – FL140100081. W.H. Saputera thanks the Indonesia Endowment Fund for Education (LPDP), Republic of Indonesia for his personal PhD fellowship.en_AU
dc.format.mimetypeapplication/pdfen_AU
dc.identifier.issn0021-9517en_AU
dc.identifier.urihttp://hdl.handle.net/1885/204777
dc.language.isoen_AUen_AU
dc.publisherElsevieren_AU
dc.relationhttp://purl.org/au-research/grants/arc/FL140100081en_AU
dc.rights© 2019 Elsevier Inc.en_AU
dc.sourceJournal of Catalysisen_AU
dc.titleCooperative defect-enriched SiO2 for oxygen activation and organic dehydrogenationen_AU
dc.typeJournal articleen_AU
local.bibliographicCitation.lastpage179en_AU
local.bibliographicCitation.startpage168en_AU
local.contributor.affiliationSaputera, Wibawa Hendra, The University of New South Walesen_AU
local.contributor.affiliationTahini, Hassan, College of Science, ANUen_AU
local.contributor.affiliationLovell, Emma, University of New South Walesen_AU
local.contributor.affiliationTan, Tze Hao, University of New South Walesen_AU
local.contributor.affiliationRawal, Aditya, University of New South Walesen_AU
local.contributor.affiliationAguey-Zinsou, Kondo- Francois, The University of New South Walesen_AU
local.contributor.affiliationFriedmann, Donia, University of New South Walesen_AU
local.contributor.affiliationSmith, Sean, College of Science, ANUen_AU
local.contributor.affiliationAmal, Rose, University of New South Walesen_AU
local.contributor.affiliationScott, J, University of New South Walesen_AU
local.contributor.authoremailrepository.admin@anu.edu.auen_AU
local.contributor.authoruidTahini, Hassan, u1057037en_AU
local.contributor.authoruidSmith, Sean, u1056946en_AU
local.description.embargo2037-12-31
local.description.notesImported from ARIESen_AU
local.identifier.absfor030601 - Catalysis and Mechanisms of Reactionsen_AU
local.identifier.absseo970103 - Expanding Knowledge in the Chemical Sciencesen_AU
local.identifier.ariespublicationu3102795xPUB4212en_AU
local.identifier.citationvolume376en_AU
local.identifier.doi10.1016/j.jcat.2019.07.006en_AU
local.identifier.scopusID2-s2.0-85069586689
local.identifier.uidSubmittedByu3102795en_AU
local.publisher.urlhttps://www.elsevier.com/en-auen_AU
local.type.statusPublished Versionen_AU

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