Cu-modified SrTiO3 perovskites toward enhanced water–gas shift catalysis: A combined experimental and computational study

dc.contributor.authorColetta, Vitor C.
dc.contributor.authorGonçalves, Renato V.
dc.contributor.authorBernardi, Maria I. B.
dc.contributor.authorHanaor, Dorian A. H.
dc.contributor.authorAssadi, M. Hussein N.
dc.contributor.authorMarcos, Francielle C. F.
dc.contributor.authorNogueira, Francisco G. E.
dc.contributor.authorAssaf, Elisabete M.
dc.contributor.authorMastelaro, Valmor R.
dc.date.accessioned2021-04-01T08:02:09Z
dc.date.available2021-04-01T08:02:09Z
dc.date.issued2020-12-23
dc.description.abstractA water–gas shift reaction (WGS) is important and widely applied in the production of H2. Cu-modified perovskites are promising catalysts for WGS reactions in hydrogen generation. However, the structure-dependent stability and reaction pathways of such materials remain unclear. Herein, we report catalytically active Cu-modified SrTiO3 (nominally SrTi1–xCuxO3) prepared by a modified polymeric precursor method. Microstructural analysis revealed a partially segregated CuO phase in the as-prepared materials. Operando X-ray diffraction and absorption spectroscopy showed the reduction of CuO into a stable metallic phase under conditions of WGS reactions for all compositions. Among the characterized materials, the x = 0.20 composition showed the highest turnover frequency, lowest activation energy, and the highest WGS rate at 300 °C. According to density functional calculations, the formation of CuO is energetically less favorable compared with SrTiO3, explaining why the segregated CuO phase on the SrTiO3 surface is reduced to Cu during the catalytic reaction, while SrTiO3 remains. For x = 0.20, the size of the segregated CuO phase is optimum for facilitating the catalytic reaction. In contrast, a higher Cu content (x = 0.3) results in an aggregation of smaller CuO particles, resulting in fewer surface active sites and a net decrease in catalytic performance.en
dc.identifier.eissn2574-0962
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/12925
dc.identifier.urihttp://dx.doi.org/10.14279/depositonce-11726
dc.language.isoenen
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/en
dc.subject.ddc540 Chemie und zugeordnete Wissenschaftende
dc.subject.otherwater−gas shiften
dc.subject.otherSrTiO3en
dc.subject.otherDFT calculationsen
dc.subject.otherperovskite catalystsen
dc.subject.otheroperando XASen
dc.subject.otherXRDen
dc.subject.otherCu dopingen
dc.subject.otherCuO formationen
dc.titleCu-modified SrTiO3 perovskites toward enhanced water–gas shift catalysis: A combined experimental and computational studyen
dc.typeArticleen
dc.type.versionacceptedVersionen
dcterms.bibliographicCitation.doi10.1021/acsaem.0c02371en
dcterms.bibliographicCitation.issue1en
dcterms.bibliographicCitation.journaltitleACS Applied Energy Materialsen
dcterms.bibliographicCitation.originalpublishernameAmerican Chemical Society (ACS)en
dcterms.bibliographicCitation.originalpublisherplaceWashington, DCen
dcterms.bibliographicCitation.pageend461en
dcterms.bibliographicCitation.pagestart452en
dcterms.bibliographicCitation.volume4en
tub.accessrights.dnbdomain*
tub.affiliationFak. 3 Prozesswissenschaften>Inst. Werkstoffwissenschaften und -technologien>FG Keramische Werkstoffede
tub.affiliation.facultyFak. 3 Prozesswissenschaftende
tub.affiliation.groupFG Keramische Werkstoffede
tub.affiliation.instituteInst. Werkstoffwissenschaften und -technologiende
tub.publisher.universityorinstitutionTechnische Universität Berlinen
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