Pd/Ga2O3 methanol steam reforming catalysts: Part I. Morphology, composition and structural aspects
The combination of (high-resolution) electron microscopy, selected area diffraction and X-ray diffraction was applied to study the structural, compositional and morphological alterations of two Pd/Ga2O3 catalysts relevant for methanol steam reforming upon different oxidative and reductive treatments...
Saved in:
Published in | Applied catalysis. A, General Vol. 358; no. 2; pp. 193 - 202 |
---|---|
Main Authors | , , , , , , |
Format | Journal Article |
Language | English |
Published |
Kidlington
Elsevier
01.05.2009
|
Subjects | |
Online Access | Get full text |
Cover
Loading…
Abstract | The combination of (high-resolution) electron microscopy, selected area diffraction and X-ray diffraction was applied to study the structural, compositional and morphological alterations of two Pd/Ga2O3 catalysts relevant for methanol steam reforming upon different oxidative and reductive treatments. These systems include well-defined Pd particles grown epitaxially on vacuum-cleaved NaCl(0 0 1) single crystals and subsequently covered by a layer of amorphous Ga2O3 (termed as 'thin film model catalysts'), as well as, for comparison, a conventional Pd/Ga2O3 powder catalyst prepared by incipient wetness impregnation. Both catalysts were subsequently subjected to similar treatments in O2 (1 bar, 1 h) and H2 (1 bar, 1 h) in the temperature range between 373 and 923 K. Oxidation of the thin film model catalyst at 773 K converts the Pd/Ga2O3 film into a mixture of PdO and Pd supported on Ga2O3. Subsequent reduction at 523 K causes the formation of an epitaxial Pd5Ga2 bimetallic phase with suppressed Pd hydride formation, in close correlation to the corresponding Pd/ZnO system. In contrast to the latter, Pd/Ga2O3 thin film model catalysts are prone to sintering at reduction temperatures > =673 K. However, Pd5Ga2 with some Pd probably remaining in the particle cores is still present. The stability of the bimetallic Pd5Ga2 phase in oxygen was observed to depend on the pre-reduction history, that is, oxidation at 673 K of a bimetallic formed at 523 K causes the complete decomposition of the bimetallic phase and formation of PdO/Pd particles supported on Ga2O3, whereas bimetallics formed at higher reduction temperatures (i.e. > =673 K) are only transformed back to Pd/Ga2O3. According to TEM investigations, this is due to the increased mobility of Ga and the subsequent formation of a Ga2O3 surface layer preventing further oxidation to PdO. Reduction of the corresponding Pd/beta-Ga2O3 impregnated powder catalyst between 573 and 773 K causes the formation of a Pd2Ga bimetallic phase, which is further converted to PdGa at reduction temperatures of 923 K. No formation of a Ga2O3 surface layer covering the particles has been observed upon re-oxidation of the bimetallic. This is explained on the basis of the difference in metal (bimetallic)-support contact area. |
---|---|
AbstractList | The combination of (high-resolution) electron microscopy, selected area diffraction and X-ray diffraction was applied to study the structural, compositional and morphological alterations of two Pd/Ga2O3 catalysts relevant for methanol steam reforming upon different oxidative and reductive treatments. These systems include well-defined Pd particles grown epitaxially on vacuum-cleaved NaCl(0 0 1) single crystals and subsequently covered by a layer of amorphous Ga2O3 (termed as 'thin film model catalysts'), as well as, for comparison, a conventional Pd/Ga2O3 powder catalyst prepared by incipient wetness impregnation. Both catalysts were subsequently subjected to similar treatments in O2 (1 bar, 1 h) and H2 (1 bar, 1 h) in the temperature range between 373 and 923 K. Oxidation of the thin film model catalyst at 773 K converts the Pd/Ga2O3 film into a mixture of PdO and Pd supported on Ga2O3. Subsequent reduction at 523 K causes the formation of an epitaxial Pd5Ga2 bimetallic phase with suppressed Pd hydride formation, in close correlation to the corresponding Pd/ZnO system. In contrast to the latter, Pd/Ga2O3 thin film model catalysts are prone to sintering at reduction temperatures > =673 K. However, Pd5Ga2 with some Pd probably remaining in the particle cores is still present. The stability of the bimetallic Pd5Ga2 phase in oxygen was observed to depend on the pre-reduction history, that is, oxidation at 673 K of a bimetallic formed at 523 K causes the complete decomposition of the bimetallic phase and formation of PdO/Pd particles supported on Ga2O3, whereas bimetallics formed at higher reduction temperatures (i.e. > =673 K) are only transformed back to Pd/Ga2O3. According to TEM investigations, this is due to the increased mobility of Ga and the subsequent formation of a Ga2O3 surface layer preventing further oxidation to PdO. Reduction of the corresponding Pd/beta-Ga2O3 impregnated powder catalyst between 573 and 773 K causes the formation of a Pd2Ga bimetallic phase, which is further converted to PdGa at reduction temperatures of 923 K. No formation of a Ga2O3 surface layer covering the particles has been observed upon re-oxidation of the bimetallic. This is explained on the basis of the difference in metal (bimetallic)-support contact area. |
Author | JOCHUM, Wilfrid RAMESHAN, Christoph STÖGER-POLLACH, Michael LORENZ, Harald PENNER, Simon DI WANG KLÖTZER, Bernhard |
Author_xml | – sequence: 1 givenname: Simon surname: PENNER fullname: PENNER, Simon organization: Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, 6020 Innsbruck, Austria – sequence: 2 givenname: Harald surname: LORENZ fullname: LORENZ, Harald organization: Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, 6020 Innsbruck, Austria – sequence: 3 givenname: Wilfrid surname: JOCHUM fullname: JOCHUM, Wilfrid organization: Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, 6020 Innsbruck, Austria – sequence: 4 givenname: Michael surname: STÖGER-POLLACH fullname: STÖGER-POLLACH, Michael organization: University Service Centre for Transmission Electron Microscopy (USTEM), Vienna University of Technology, Wiedner Hauptstrasse 8-10/052, 1040 Vienna, Austria – sequence: 5 surname: DI WANG fullname: DI WANG organization: Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany – sequence: 6 givenname: Christoph surname: RAMESHAN fullname: RAMESHAN, Christoph organization: Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, 6020 Innsbruck, Austria – sequence: 7 givenname: Bernhard surname: KLÖTZER fullname: KLÖTZER, Bernhard organization: Institute of Physical Chemistry, University of Innsbruck, Innrain 52a, 6020 Innsbruck, Austria |
BackLink | http://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=21384543$$DView record in Pascal Francis |
BookMark | eNo9kM9LwzAYhoNMcJv-Bx5y0ZPt8qtZ602GzsFkOyh4C59JunW0TU3Sw_57OzaEF77L-zzwvRM0al1rEbqnJKWEytkhhU5DhJQRUqSEDZFXaEzzOU94Ps9GaEwKJpNcku8bNAnhQAhhosjGSG_NbAlsw3Fj4x5aV-MQLTTY29L5pmp3-GSujyGGZ7wFH_EqxR_Od3tXu93xCWvXdC5UsXIthtYMuO917D3UGEJndQy36LqEOti7y52ir7fXz8V7st4sV4uXdaIFEzEBa0AaLiErbVkyMJIyIzJZcGk0FcBIxkvDjM6ZoPan4JxJyPOsKE8d4HyKHs_ezrvf3oaomipoW9fQWtcHxQXLKeX5UBTnovYuhOFT1fmqAX9UlKjTouqgzouq06KKsCFywB4ufgga6tJDq6vwz7JBLTLB-R_BR3tg |
CitedBy_id | crossref_primary_10_1021_jp3061224 crossref_primary_10_1021_acs_chemrev_6b00099 crossref_primary_10_1016_j_tsf_2014_03_001 crossref_primary_10_1016_j_ijhydene_2016_01_084 crossref_primary_10_1016_j_commatsci_2013_01_033 crossref_primary_10_1007_s10562_018_2491_4 crossref_primary_10_1021_cs500465r crossref_primary_10_1016_j_matchemphys_2012_11_071 crossref_primary_10_1016_j_matchemphys_2013_08_048 crossref_primary_10_1021_acscatal_6b02928 crossref_primary_10_1016_j_jcou_2015_09_002 crossref_primary_10_1016_j_ijhydene_2013_09_150 crossref_primary_10_1021_jp110824n crossref_primary_10_1002_cctc_201200268 crossref_primary_10_1016_j_jnoncrysol_2009_05_007 crossref_primary_10_1002_cctc_201200100 crossref_primary_10_1016_j_apcata_2009_12_007 crossref_primary_10_1134_S0023158416040017 crossref_primary_10_1016_j_susc_2016_03_009 crossref_primary_10_1016_j_apcatb_2010_10_010 crossref_primary_10_1063_1_4874002 crossref_primary_10_1016_j_jcat_2012_03_009 crossref_primary_10_1002_chem_201801957 crossref_primary_10_1016_j_apcata_2012_11_010 crossref_primary_10_1021_ja202869d crossref_primary_10_1007_s10973_016_5525_4 crossref_primary_10_1002_cctc_201200712 crossref_primary_10_1016_j_jcou_2014_11_003 crossref_primary_10_1016_j_solidstatesciences_2012_04_037 crossref_primary_10_1039_c2cp41459g crossref_primary_10_1016_j_jcat_2012_10_003 crossref_primary_10_1063_1_4821148 crossref_primary_10_1149_1945_7111_ac6706 crossref_primary_10_1016_j_cattod_2014_07_050 crossref_primary_10_1021_ar500220v crossref_primary_10_1364_OME_4_000518 crossref_primary_10_3103_S106287381309044X crossref_primary_10_1007_s11426_014_5269_6 crossref_primary_10_1016_j_jcat_2012_05_005 crossref_primary_10_1016_j_cattod_2012_07_037 crossref_primary_10_1021_jp109226r crossref_primary_10_1021_cs300480c crossref_primary_10_1039_C4EE00389F crossref_primary_10_1002_cctc_201402635 crossref_primary_10_1016_j_ces_2016_08_009 crossref_primary_10_18412_1816_0387_2023_6_17_51 crossref_primary_10_1038_nchem_2822 crossref_primary_10_1016_j_apsusc_2014_01_074 crossref_primary_10_1021_acscatal_1c00718 crossref_primary_10_1016_j_matchemphys_2010_03_057 crossref_primary_10_1002_sstr_202100011 crossref_primary_10_1007_s10562_011_0584_4 crossref_primary_10_1021_jp407337q crossref_primary_10_3103_S0361521915010103 crossref_primary_10_1021_jp505458v crossref_primary_10_1002_cctc_201300029 crossref_primary_10_1016_j_cattod_2020_07_048 crossref_primary_10_1016_j_molcata_2012_03_010 crossref_primary_10_1039_D1CY00913C crossref_primary_10_1016_j_jcat_2011_10_007 crossref_primary_10_1039_D0CY00956C crossref_primary_10_1016_j_apcata_2010_04_015 crossref_primary_10_1016_j_jcat_2013_10_002 crossref_primary_10_1039_D3CC06121C crossref_primary_10_1016_j_jcat_2012_05_020 crossref_primary_10_1155_2013_132180 crossref_primary_10_1002_chem_201703627 |
ContentType | Journal Article |
Copyright | 2009 INIST-CNRS |
Copyright_xml | – notice: 2009 INIST-CNRS |
DBID | IQODW AAYXX CITATION 7SR 7U5 8BQ 8FD JG9 L7M |
DOI | 10.1016/j.apcata.2009.02.026 |
DatabaseName | Pascal-Francis CrossRef Engineered Materials Abstracts Solid State and Superconductivity Abstracts METADEX Technology Research Database Materials Research Database Advanced Technologies Database with Aerospace |
DatabaseTitle | CrossRef Materials Research Database Engineered Materials Abstracts Solid State and Superconductivity Abstracts Technology Research Database Advanced Technologies Database with Aerospace METADEX |
DatabaseTitleList | Materials Research Database |
DeliveryMethod | fulltext_linktorsrc |
Discipline | Engineering Chemistry |
EISSN | 1873-3875 |
EndPage | 202 |
ExternalDocumentID | 10_1016_j_apcata_2009_02_026 21384543 |
GroupedDBID | --K --M -~X .~1 0R~ 1B1 1~. 1~5 23M 4.4 457 4G. 53G 5GY 5VS 7-5 71M 8P~ 9JN AABNK AACTN AAEDT AAEDW AAIAV AAIKJ AAKOC AALRI AAOAW AAQFI AAQXK AAXUO ABFNM ABMAC ABNUV ABPIF ABPTK ABXDB ABYKQ ACDAQ ACGFS ACIWK ACRLP ADBBV ADEWK ADEZE ADMUD AEBSH AEKER AFKWA AFTJW AGHFR AGUBO AGYEJ AHHHB AHPOS AI. AIEXJ AIKHN AITUG AJBFU AJOXV AKURH ALMA_UNASSIGNED_HOLDINGS AMFUW AMRAJ ASPBG AVWKF AXJTR AZFZN BBWZM BKOJK BLXMC CS3 EBS EFJIC EJD ENUVR EO8 EO9 EP2 EP3 FDB FEDTE FGOYB FIRID FNPLU FYGXN G-Q GBLVA HLY HZ~ IHE IQODW J1W KOM LX7 M41 MO0 N9A NDZJH O-L O9- OAUVE OZT P-8 P-9 P2P PC. Q38 R2- ROL RPZ SCE SDF SDG SDP SES SEW SPC SPD SSG SSZ T5K VH1 WUQ XFK XPP ZMT ~02 ~G- AAXKI AAYXX CITATION 7SR 7U5 8BQ 8FD JG9 L7M |
ID | FETCH-LOGICAL-c424t-aeda6d36a5feff2ad612d456936dc14a2053fd2dc8241eb93326a8859f5693a33 |
ISSN | 0926-860X |
IngestDate | Fri Aug 16 07:46:46 EDT 2024 Thu Sep 12 19:37:17 EDT 2024 Sun Oct 22 16:10:14 EDT 2023 |
IsDoiOpenAccess | false |
IsOpenAccess | true |
IsPeerReviewed | true |
IsScholarly | true |
Issue | 2 |
Keywords | Binary compound Correlation High resolution Support Selected area electron diffraction Electron diffraction Film X-ray diffraction Alcohol Hydrides Pd2Ga Powder Thin film Particle Chemical reduction Alkanol Oxidation Platinoid Methanol Composition Transition element compounds Pd5Ga2 Transition metal Palladium PdGa Electron microscopy X ray diffraction Bimetallic particles Single crystal Heterogeneous catalysis Impregnation Transmission electron microscopy Morphology Models Steam reforming Catalyst |
Language | English |
License | CC BY 4.0 |
LinkModel | OpenURL |
MergedId | FETCHMERGED-LOGICAL-c424t-aeda6d36a5feff2ad612d456936dc14a2053fd2dc8241eb93326a8859f5693a33 |
Notes | ObjectType-Article-2 SourceType-Scholarly Journals-1 ObjectType-Feature-1 content type line 23 |
OpenAccessLink | https://pure.mpg.de/pubman/item/item_736183_3/component/file_736182/Structure%20paper%20part%20I%20Pd-Ga.pdf |
PQID | 34281138 |
PQPubID | 23500 |
PageCount | 10 |
ParticipantIDs | proquest_miscellaneous_34281138 crossref_primary_10_1016_j_apcata_2009_02_026 pascalfrancis_primary_21384543 |
PublicationCentury | 2000 |
PublicationDate | 2009-05-01 |
PublicationDateYYYYMMDD | 2009-05-01 |
PublicationDate_xml | – month: 05 year: 2009 text: 2009-05-01 day: 01 |
PublicationDecade | 2000 |
PublicationPlace | Kidlington |
PublicationPlace_xml | – name: Kidlington |
PublicationTitle | Applied catalysis. A, General |
PublicationYear | 2009 |
Publisher | Elsevier |
Publisher_xml | – name: Elsevier |
SSID | ssj0002495 |
Score | 2.273775 |
Snippet | The combination of (high-resolution) electron microscopy, selected area diffraction and X-ray diffraction was applied to study the structural, compositional... |
SourceID | proquest crossref pascalfrancis |
SourceType | Aggregation Database Index Database |
StartPage | 193 |
SubjectTerms | Catalysis Chemistry Exact sciences and technology General and physical chemistry Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry |
Title | Pd/Ga2O3 methanol steam reforming catalysts: Part I. Morphology, composition and structural aspects |
URI | https://search.proquest.com/docview/34281138 |
Volume | 358 |
hasFullText | 1 |
inHoldings | 1 |
isFullTextHit | |
isPrint | |
link | http://utb.summon.serialssolutions.com/2.0.0/link/0/eLvHCXMwnV1Lb9QwELaWcgCEEBQqlkfxgduSsLGdF7dSAVvEYyVaaW_RxHZgKzVZNdtDe-DX8EMZ23mVrRBFiqIom7V3PV_G4_E3M4S8lJLFJvutp6cJeAJwzQqg8YpLFD_ghChM7PDnL9HsSHxchIvR6NeAtXS2zn15cWVcyf9IFe-hXE2U7DUk2zWKN_Aa5YtnlDCe_0nGc9PhB2Bfua0EDWVlgj80nExw3qsMy-X7xPpnzuu1pb7NsZHJgY9vMg5vF6diaOUNd8vuJbicsjYfB9hIzHpowrZ2a9PwsvYne867bhNY97q2K-q1POn3-j9Vp7q0TusZGG9Yz-CRP1zJZdRTxemy--Db2uzlv42M83FuQOtqVw3p_q3TIu0pgq33kUVeEk0XQ0XMw2SAODZQq4GrotjM0MzGaG8qf-eHOPZhZUagyUXK8Lgi1_Yfc2DHTGxJb8eZa8WU6UyzKcMjukFusjgNDXHU_9kTiUz1bpvRsflLbYCmZRFu_pZLBtDdFdT4LhauiMqGPWCNnMP75F6zOqF7DmoPyEiX2-TWflsUcJvcGeSvfEjkXL228KMt_KiFH-3gRzv4vaEGfPTApz34XtEB9ChCj_bQow30HpGj9-8O92deU7XDk4KJtQdaQaR4BGGhi4KBQhtaoZme8kjJQABDtV8opmSCxqPOU44LCEiSMC3MM8D5Dtkqq1I_JhQKnuqkEDGYCOg8hjxQuYwVpEKKhAVj4rVDma1ccpbsbwIck91L4919iQU8EdjFmLxoBZDhwJq9Myh1dVZnHJfpAT715JpdPiW3e_w_I1s4ivo5mrHrfNei6DceT59U |
link.rule.ids | 315,786,790,27955,27956 |
linkProvider | Elsevier |
openUrl | ctx_ver=Z39.88-2004&ctx_enc=info%3Aofi%2Fenc%3AUTF-8&rfr_id=info%3Asid%2Fsummon.serialssolutions.com&rft_val_fmt=info%3Aofi%2Ffmt%3Akev%3Amtx%3Ajournal&rft.genre=article&rft.atitle=Pd%2FGa2O3+methanol+steam+reforming+catalysts%3A+Part+I.+Morphology%2C+composition+and+structural+aspects&rft.jtitle=Applied+catalysis.+A%2C+General&rft.au=Penner%2C+Simon&rft.au=Lorenz%2C+Harald&rft.au=Jochum%2C+Wilfrid&rft.au=St%C3%B6ger-Pollach%2C+Michael&rft.date=2009-05-01&rft.issn=0926-860X&rft.volume=358&rft.issue=2&rft.spage=193&rft.epage=202&rft_id=info:doi/10.1016%2Fj.apcata.2009.02.026&rft.externalDBID=n%2Fa&rft.externalDocID=10_1016_j_apcata_2009_02_026 |
thumbnail_l | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/lc.gif&issn=0926-860X&client=summon |
thumbnail_m | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/mc.gif&issn=0926-860X&client=summon |
thumbnail_s | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/sc.gif&issn=0926-860X&client=summon |