Role of surface reconstruction on Cu/TiO2 nanotubes for CO2 conversion

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dc.check.date2021-05-16
dc.check.infoAccess to this article is restricted until 24 months after publication by request of the publisher.en
dc.contributor.authorLiu, Chao
dc.contributor.authorNauert, Scott L.
dc.contributor.authorAlsina, Marco A.
dc.contributor.authorWang, Dingdi
dc.contributor.authorGrant, Alexander
dc.contributor.authorHe, Kai
dc.contributor.authorWeitz, Eric
dc.contributor.authorNolan, Michael
dc.contributor.authorGray, Kimberly A.
dc.contributor.authorNotestein, Justin M.
dc.contributor.funderNational Science Foundationen
dc.contributor.funderU.S. Department of Energyen
dc.contributor.funderNorthwestern Universityen
dc.contributor.funderScience Foundation Irelanden
dc.contributor.funderHigher Education Authorityen
dc.contributor.funderEuropean Cooperation in Science and Technologyen
dc.date.accessioned2019-08-15T13:39:44Z
dc.date.available2019-08-15T13:39:44Z
dc.date.issued2019-05-16
dc.date.updated2019-08-15T13:24:19Z
dc.description.abstractCarbon dioxide hydrogenation to CO via the reverse water gas shift (RWGS) reaction is one route to integrate CO2 utilization into the chemical industry. TiO2 supported Cu catalysts are known to be active for RWGS, but Cu is shown here to behave differently on TiO2 nanotubes (TiNT) vs TiO2 nanoparticles (TiNP). Whereas nanoparticle supports give low rates that are hardly changed by added Cu, the nanotube supports yield much higher activity and three distinct behaviors as the Cu surface density increases. At low surface densities (0.3 Cu/nm2), active Cu-O-Ti sites are created that have low apparent activation energies. At high surface densities (6 Cu/nm2), Cu nanoparticles on TiNT are formed, and reaction barriers are lowered when both Cu and TiNT surfaces are accessible. At intermediate surface densities, metallic Cu domains are engulfed by a TiOx overlayer formed during H2 pretreatment, akin to those formed by classical strong metal support interactions (SMSI). These reduced layers are markedly more active for RWGS than the initial TiNT surfaces, but have similar activation barriers, which are higher than those for which both Cu and TiNP surfaces are exposed. These catalytic findings are supported by computational modeling, in situ IR, UV–vis, and X-ray absorption spectroscopies, and they provide insight into an important reaction for CO2 utilization.en
dc.description.sponsorshipNational Science Foundation ((CBET-1438721); MRSEC program (DMR-1121262, DMR-1720139) and the Soft and HybridNanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205)); Department of Energy (DE-FG02-03ER15457; CleanCat core facility (DRIFTS and TPR)); Northwestern University (Institute for Sustainability and Energy); European Cooperation in Science and Technology (COST Action CM1104“ReducibleMetal Oxides, Structure and Function)en
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.articleid117754en
dc.identifier.citationLiu, C., Nauert, S. L., Alsina, M. A., Wang, D., Grant, A., He, K., Weitz, E., Nolan, M., Gray, K. A. and Notestein, J. M. (2019) 'Role of surface reconstruction on Cu/TiO2 nanotubes for CO2 conversion', Applied Catalysis B: Environmental, 255, 117754 (9 pp). doi: 10.1016/j.apcatb.2019.117754en
dc.identifier.doi10.1016/j.apcatb.2019.117754en
dc.identifier.endpage9en
dc.identifier.issn0926-3373
dc.identifier.journaltitleApplied Catalysis B: Environmentalen
dc.identifier.startpage1en
dc.identifier.urihttps://hdl.handle.net/10468/8340
dc.identifier.volume255en
dc.language.isoenen
dc.publisherElsevieren
dc.relation.projectinfo:eu-repo/grantAgreement/SFI/SFI US Ireland R&D Partnership/14/US/E2915/IE/SusChEM: Using theory-driven design to tailor novel nanocomposite oxides for solar fuel production/en
dc.relation.urihttp://www.sciencedirect.com/science/article/pii/S092633731930493X
dc.rights© 2019 Elsevier B.V. All rights reserved. This manuscript version is made available under the CC-BY-NC-ND 4.0 licenseen
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subjectReverse water-gas shiften
dc.subjectSMSIen
dc.subjectSupported metalsen
dc.subjectSpectroscopyen
dc.subjectCO2 conversionen
dc.titleRole of surface reconstruction on Cu/TiO2 nanotubes for CO2 conversionen
dc.typeArticle (peer-reviewed)en
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