CO(2)-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy.
Identifieur interne : 000F68 ( Main/Exploration ); précédent : 000F67; suivant : 000F69CO(2)-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy.
Auteurs : RBID : pubmed:23226689Abstract
In situ X-ray photoelectron spectroscopy (in situ XPS) was used to study the structural and catalytic properties of Pd-In near-surface intermetallic phases in correlation with previously studied PdZn and PdGa.Room temperature deposition of ∼4 monolayer equivalents (MLEs) of In metal on Pd foil and subsequent annealing to 453 K in vacuum yields a ∼1:1 Pd/In near-surface multilayer intermetallic phase. This Pd(1)In(1) phase exhibits a similar "Cu-like" electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd(1)Zn(1) counterpart.Catalytic characterization of the multilayer Pd(1)In(1) phase in MSR yielded a CO(2)-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In(2)O(3)-supported PdIn nanoparticles and pure In(2)O(3), intermediate formaldehyde is only partially converted to CO(2) using this Pd(1)In(1) phase. Strongly correlated with PdZn, on an In-diluted PdIn intermetallic phase with "Pd-like" electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed.To achieve CO(2)-TOF values on the isolated Pd(1)In(1) intermetallic phase as high as on supported PdIn/In(2)O(3), at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO(2) conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd(1)In(1) inhibited inverse water-gas-shift reaction on In(2)O(3) and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO(2)-selectivity of the supported catalyst.
DOI: 10.1016/j.jcat.2012.08.008
PubMed: 23226689
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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en">CO(2)-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy.</title><author><name sortKey="Rameshan, Christoph" uniqKey="Rameshan C">Christoph Rameshan</name><affiliation wicri:level="3"><nlm:affiliation>Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, A-6020 Innsbruck, Austria ; Department of Inorganic Chemistry, Fritz-Haber-Institute of the Max-Planck-Society, Faradayweg 4-6, D-14195 Berlin, Germany.</nlm:affiliation><country xml:lang="fr">Allemagne</country><wicri:regionArea>Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, A-6020 Innsbruck, Austria ; Department of Inorganic Chemistry, Fritz-Haber-Institute of the Max-Planck-Society, Faradayweg 4-6, D-14195 Berlin</wicri:regionArea><placeName><region type="land" nuts="3">Berlin</region><settlement type="city">Berlin</settlement></placeName></affiliation></author><author><name sortKey="Lorenz, Harald" uniqKey="Lorenz H">Harald Lorenz</name></author><author><name sortKey="Mayr, Lukas" uniqKey="Mayr L">Lukas Mayr</name></author><author><name sortKey="Penner, Simon" uniqKey="Penner S">Simon Penner</name></author><author><name sortKey="Zemlyanov, Dmitry" uniqKey="Zemlyanov D">Dmitry Zemlyanov</name></author><author><name sortKey="Arrigo, Rosa" uniqKey="Arrigo R">Rosa Arrigo</name></author><author><name sortKey="Haevecker, Michael" uniqKey="Haevecker M">Michael Haevecker</name></author><author><name sortKey="Blume, Raoul" uniqKey="Blume R">Raoul Blume</name></author><author><name sortKey="Knop Gericke, Axel" uniqKey="Knop Gericke A">Axel Knop-Gericke</name></author><author><name sortKey="Schl Gl, Robert" uniqKey="Schl Gl R">Robert Schlögl</name></author><author><name sortKey="Kl Tzer, Bernhard" uniqKey="Kl Tzer B">Bernhard Klötzer</name></author></titleStmt><publicationStmt><date when="2012">2012</date><idno type="doi">10.1016/j.jcat.2012.08.008</idno><idno type="RBID">pubmed:23226689</idno><idno type="pmid">23226689</idno><idno type="wicri:Area/Main/Corpus">000899</idno><idno type="wicri:Area/Main/Curation">000899</idno><idno type="wicri:Area/Main/Exploration">000F68</idno></publicationStmt></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">In situ X-ray photoelectron spectroscopy (in situ XPS) was used to study the structural and catalytic properties of Pd-In near-surface intermetallic phases in correlation with previously studied PdZn and PdGa.Room temperature deposition of ∼4 monolayer equivalents (MLEs) of In metal on Pd foil and subsequent annealing to 453 K in vacuum yields a ∼1:1 Pd/In near-surface multilayer intermetallic phase. This Pd(1)In(1) phase exhibits a similar "Cu-like" electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd(1)Zn(1) counterpart.Catalytic characterization of the multilayer Pd(1)In(1) phase in MSR yielded a CO(2)-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In(2)O(3)-supported PdIn nanoparticles and pure In(2)O(3), intermediate formaldehyde is only partially converted to CO(2) using this Pd(1)In(1) phase. Strongly correlated with PdZn, on an In-diluted PdIn intermetallic phase with "Pd-like" electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed.To achieve CO(2)-TOF values on the isolated Pd(1)In(1) intermetallic phase as high as on supported PdIn/In(2)O(3), at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO(2) conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd(1)In(1) inhibited inverse water-gas-shift reaction on In(2)O(3) and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO(2)-selectivity of the supported catalyst.</div></front></TEI><pubmed><MedlineCitation Status="Publisher" Owner="NLM"><PMID Version="1">23226689</PMID><DateCreated><Year>2012</Year><Month>12</Month><Day>10</Day></DateCreated><Article PubModel="Print"><Journal><ISSN IssnType="Print">0021-9517</ISSN><JournalIssue CitedMedium="Print"><Volume>295</Volume><Issue>2-3</Issue><PubDate><Year>2012</Year><Month>Nov</Month></PubDate></JournalIssue><Title>Journal of catalysis</Title><ISOAbbreviation>J Catal</ISOAbbreviation></Journal><ArticleTitle>CO(2)-selective methanol steam reforming on In-doped Pd studied by in situ X-ray photoelectron spectroscopy.</ArticleTitle><Pagination><MedlinePgn>186-194</MedlinePgn></Pagination><Abstract><AbstractText>In situ X-ray photoelectron spectroscopy (in situ XPS) was used to study the structural and catalytic properties of Pd-In near-surface intermetallic phases in correlation with previously studied PdZn and PdGa.Room temperature deposition of ∼4 monolayer equivalents (MLEs) of In metal on Pd foil and subsequent annealing to 453 K in vacuum yields a ∼1:1 Pd/In near-surface multilayer intermetallic phase. This Pd(1)In(1) phase exhibits a similar "Cu-like" electronic structure and indium depth distribution as its methanol steam reforming (MSR)-selective multilayer Pd(1)Zn(1) counterpart.Catalytic characterization of the multilayer Pd(1)In(1) phase in MSR yielded a CO(2)-selectivity of almost 100% between 493 and 550 K. In contrast to previously studied In(2)O(3)-supported PdIn nanoparticles and pure In(2)O(3), intermediate formaldehyde is only partially converted to CO(2) using this Pd(1)In(1) phase. Strongly correlated with PdZn, on an In-diluted PdIn intermetallic phase with "Pd-like" electronic structure, prepared by thermal annealing at 623 K, methanol steam reforming is suppressed and enhanced CO formation via full methanol dehydrogenation is observed.To achieve CO(2)-TOF values on the isolated Pd(1)In(1) intermetallic phase as high as on supported PdIn/In(2)O(3), at least 593 K reaction temperature is required. A bimetal-oxide synergism, with both bimetallic and oxide synergistically contributing to the observed catalytic activity and selectivity, manifests itself by accelerated formaldehyde-to-CO(2) conversion at markedly lowered temperatures as compared to separate oxide and bimetal. Combination of suppression of full methanol dehydrogenation to CO on Pd(1)In(1) inhibited inverse water-gas-shift reaction on In(2)O(3) and fast water activation/conversion of formaldehyde is the key to the low-temperature activity and high CO(2)-selectivity of the supported catalyst.</AbstractText></Abstract><AuthorList><Author><LastName>Rameshan</LastName><ForeName>Christoph</ForeName><Initials>C</Initials><Affiliation>Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, A-6020 Innsbruck, Austria ; Department of Inorganic Chemistry, Fritz-Haber-Institute of the Max-Planck-Society, Faradayweg 4-6, D-14195 Berlin, Germany.</Affiliation></Author><Author><LastName>Lorenz</LastName><ForeName>Harald</ForeName><Initials>H</Initials></Author><Author><LastName>Mayr</LastName><ForeName>Lukas</ForeName><Initials>L</Initials></Author><Author><LastName>Penner</LastName><ForeName>Simon</ForeName><Initials>S</Initials></Author><Author><LastName>Zemlyanov</LastName><ForeName>Dmitry</ForeName><Initials>D</Initials></Author><Author><LastName>Arrigo</LastName><ForeName>Rosa</ForeName><Initials>R</Initials></Author><Author><LastName>Haevecker</LastName><ForeName>Michael</ForeName><Initials>M</Initials></Author><Author><LastName>Blume</LastName><ForeName>Raoul</ForeName><Initials>R</Initials></Author><Author><LastName>Knop-Gericke</LastName><ForeName>Axel</ForeName><Initials>A</Initials></Author><Author><LastName>Schlögl</LastName><ForeName>Robert</ForeName><Initials>R</Initials></Author><Author><LastName>Klötzer</LastName><ForeName>Bernhard</ForeName><Initials>B</Initials></Author></AuthorList><Language>ENG</Language><PublicationTypeList><PublicationType>JOURNAL ARTICLE</PublicationType></PublicationTypeList></Article><MedlineJournalInfo><MedlineTA>J Catal</MedlineTA><NlmUniqueID>0374756</NlmUniqueID><ISSNLinking>0021-9517</ISSNLinking></MedlineJournalInfo></MedlineCitation><PubmedData><History><PubMedPubDate PubStatus="received"><Year>2012</Year><Month>5</Month><Day>31</Day></PubMedPubDate><PubMedPubDate PubStatus="revised"><Year>2012</Year><Month>8</Month><Day>1</Day></PubMedPubDate><PubMedPubDate PubStatus="accepted"><Year>2012</Year><Month>8</Month><Day>12</Day></PubMedPubDate><PubMedPubDate PubStatus="entrez"><Year>2012</Year><Month>12</Month><Day>11</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="pubmed"><Year>2012</Year><Month>12</Month><Day>12</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="medline"><Year>2012</Year><Month>12</Month><Day>12</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate></History><PublicationStatus>ppublish</PublicationStatus><ArticleIdList><ArticleId IdType="doi">10.1016/j.jcat.2012.08.008</ArticleId><ArticleId IdType="pii">YJCAT10931</ArticleId><ArticleId IdType="pubmed">23226689</ArticleId><ArticleId IdType="pmc">PMC3485566</ArticleId></ArticleIdList><pmc-dir>pmcsd</pmc-dir>
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