Carbide-Modified Pd on ZrO2 as Active Phase for CO2-Reforming of Methane—A Model Phase Boundary Approach

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dc.contributor.authorKöpfle, Norbert
dc.contributor.authorPloner, Kevin
dc.contributor.authorLackner, Peter
dc.contributor.authorGötsch, Thomas
dc.contributor.authorThurner, Christoph
dc.contributor.authorCarbonio, Emilia
dc.contributor.authorHävecker, Michael
dc.contributor.authorKnop-Gericke, Axel
dc.contributor.authorSchlicker, Lukas
dc.contributor.authorDoran, Andrew
dc.contributor.authorKober, Delf
dc.contributor.authorGurlo, Aleksander
dc.contributor.authorWillinger, Marc
dc.contributor.authorPenner, Simon
dc.contributor.authorSchmid, Michael
dc.contributor.authorKlötzer, Bernhard
dc.date.accessioned2020-11-06T12:45:42Z
dc.date.available2020-11-06T12:45:42Z
dc.date.issued2020-09-02
dc.date.updated2020-10-07T12:21:49Z
dc.description.abstractStarting from subsurface Zr0-doped “inverse” Pd and bulk-intermetallic Pd0Zr0 model catalyst precursors, we investigated the dry reforming reaction of methane (DRM) using synchrotron-based near ambient pressure in-situ X-ray photoelectron spectroscopy (NAP-XPS), in-situ X-ray diffraction and catalytic testing in an ultrahigh-vacuum-compatible recirculating batch reactor cell. Both intermetallic precursors develop a Pd0–ZrO2 phase boundary under realistic DRM conditions, whereby the oxidative segregation of ZrO2 from bulk intermetallic PdxZry leads to a highly active composite layer of carbide-modified Pd0 metal nanoparticles in contact with tetragonal ZrO2. This active state exhibits reaction rates exceeding those of a conventional supported Pd–ZrO2 reference catalyst and its high activity is unambiguously linked to the fast conversion of the highly reactive carbidic/dissolved C-species inside Pd0 toward CO at the Pd/ZrO2 phase boundary, which serves the role of providing efficient CO2 activation sites. In contrast, the near-surface intermetallic precursor decomposes toward ZrO2 islands at the surface of a quasi-infinite Pd0 metal bulk. Strongly delayed Pd carbide accumulation and thus carbon resegregation under reaction conditions leads to a much less active interfacial ZrO2–Pd0 state.en
dc.description.sponsorshipEC/H2020/730872/EU/Convenient Access to Light Sources Open to Innovation, Science and to the World/CALIPSOplusen
dc.identifier.eissn2073-4344
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/11857
dc.identifier.urihttp://dx.doi.org/10.14279/depositonce-10747
dc.language.isoenen
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/en
dc.subject.ddc540 Chemie und zugeordnete Wissenschaftende
dc.subject.otherpalladium carbideen
dc.subject.othergraphiteen
dc.subject.othermetal-support interactionen
dc.subject.othercokingen
dc.subject.otherpalladium-zirconium intermetallic phaseen
dc.subject.otherin-situ X-ray photoelectron spectroscopyen
dc.subject.otherin-situ X-ray diffractionen
dc.subject.otherhigh resolution electron microscopyen
dc.subject.otherdry reforming of methaneen
dc.subject.othercarbon dioxide activationen
dc.titleCarbide-Modified Pd on ZrO2 as Active Phase for CO2-Reforming of Methane—A Model Phase Boundary Approachen
dc.typeArticleen
dc.type.versionpublishedVersionen
dcterms.bibliographicCitation.articlenumber1000en
dcterms.bibliographicCitation.doi10.3390/catal10091000en
dcterms.bibliographicCitation.issue9en
dcterms.bibliographicCitation.journaltitleCatalystsen
dcterms.bibliographicCitation.originalpublishernameMDPIen
dcterms.bibliographicCitation.originalpublisherplaceBaselen
dcterms.bibliographicCitation.volume10en
tub.accessrights.dnbfreeen
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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