Gas-phase hydrodeoxygenation of guaiacol over iron-based catalysts. Effect of gases composition, iron load and supports (silica and activated carbon)
Identifieur interne : 000543 ( Hal/Curation ); précédent : 000542; suivant : 000544Gas-phase hydrodeoxygenation of guaiacol over iron-based catalysts. Effect of gases composition, iron load and supports (silica and activated carbon)
Auteurs : Roberto N. Olcese [France] ; M. M. Bettahar [France] ; Bernard Malaman [France] ; Jaafar Ghanbaja [France] ; L. Tibavizco [France] ; Dominique Petitjean [France] ; Anthony Dufour [France]Source :
- Applied Catalysis B: Environmental [ 0926-3373 ] ; 2013-01-07.
Descripteurs français
- Wicri :
- topic : Fer.
English descriptors
- mix :
- Activated carbon, Active site, Alcohols, Aromatic, Atmospheric pressure, Benzene, Benzene and Toluene, Biorefineries, Biorefinery, Carbides, Carbon deposites, Carbon dioxide, Carbon yield, Carbonaceous deposits, Catalyst activity, Chemicals, Deposits, Feed streams, Gases, Gasphase, Hydrodeoxygenation, Hydrotreatment, Iron, Iron Particles, Iron loading, Iron-based catalyst, Lignin, Lignin pyrolysis, Metallic compounds, Methane, Model compound, Molybdenum oxide, Paramagnetism, Phenols, Reaction mechanism, Selective catalysts, Silica, Spent catalyst, Ssbauer spectroscopies, TEM observations, Toluene, XRD.
Abstract
Fe/SiO2 is shown to be a selective catalyst for guaiacol hydrodeoxygenation (HDO). Guaiacol is used as a model compound to study the conversion of lignin pyrolysis vapours into aromatics (benzene, phenols). The effect of each individual gas present in a pyrolysis gas (H2, CO, CO2, H2O, CH4) on the selectivity of a 10wt% Fe/SiO2 catalyst is studied (673K, atmospheric pressure, 50mol% H2, 1/WHSV=0.6gcath/ggua). The speciation of the iron phase (metallic (α-Fe), carbide (Fe5C2), oxide (Fe3O4), and super-paramagnetic) in spent catalysts is revealed by XRD and Mössbauer spectroscopy as a function of gases composition. At least 3 types of carbonaceous deposit were evidenced by TPO analysis. TEM observations showed that iron particles size is not markedly affected by the reaction and that carbon deposit mainly occurs in the vicinity of iron particles. When all the gases except methane (Guaiacol+H2+CO+CO2+H2O) are simultaneously in the feed stream, the conditions are still sufficiently reducing to maintain the activity of the catalyst (66% of benzene and toluene carbon yield, 7.5gcath/ggua). The effects of support (silica or activated carbon-AC) and iron loading (5, 10, 15wt% Fe/SiO2) were also studied. 10wt% Fe/AC has a higher selectivity in phenol and cresols production than Fe/SiO2. Active sites and reaction mechanisms are discussed.
Url:
DOI: 10.1016/j.apcatb.2012.09.043
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ENSIC, 1 rue de Grandville BP 20451, 54001 Nancy Cedex</addrLine><country key="FR"></country></address><ref type="url">http://lrgp.univ-lorraine.fr/</ref></desc><listRelation><relation active="#struct-413289" type="direct"></relation><relation name="UMR7274" active="#struct-441569" type="direct"></relation></listRelation></org></tutelle><tutelle active="#struct-413289" type="indirect"><org type="institution" xml:id="struct-413289" status="VALID"><idno type="IdRef">157040569</idno><idno type="IdUnivLorraine">[UL]100--</idno><orgName>Université de Lorraine</orgName><orgName type="acronym">UL</orgName><date type="start">2012-01-01</date><desc><address><addrLine>34 cours Léopold - CS 25233 - 54052 Nancy cedex</addrLine><country key="FR"></country></address><ref type="url">http://www.univ-lorraine.fr/</ref></desc></org></tutelle><tutelle name="UMR7274" active="#struct-441569" type="indirect"><org type="institution" xml:id="struct-441569" status="VALID"><idno type="ISNI">0000000122597504</idno><idno type="IdRef">02636817X</idno><orgName>Centre National de la Recherche Scientifique</orgName><orgName type="acronym">CNRS</orgName><date type="start">1939-10-19</date><desc><address><country key="FR"></country></address><ref type="url">http://www.cnrs.fr/</ref></desc></org></tutelle></tutelles></hal:affiliation><country>France</country><placeName><settlement type="city">Nancy</settlement><settlement type="city">Metz</settlement><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author></analytic><idno type="DOI">10.1016/j.apcatb.2012.09.043</idno><series><title level="j">Applied Catalysis B: Environmental</title><idno type="ISSN">0926-3373</idno><imprint><date type="datePub">2013-01-07</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass><keywords scheme="mix" xml:lang="en"><term>Activated carbon</term><term>Active site</term><term>Alcohols</term><term>Aromatic</term><term>Atmospheric pressure</term><term>Benzene</term><term>Benzene and Toluene</term><term>Biorefineries</term><term>Biorefinery</term><term>Carbides</term><term>Carbon deposites</term><term>Carbon dioxide</term><term>Carbon yield</term><term>Carbonaceous deposits</term><term>Catalyst activity</term><term>Chemicals</term><term>Deposits</term><term>Feed streams</term><term>Gases</term><term>Gasphase</term><term>Hydrodeoxygenation</term><term>Hydrotreatment</term><term>Iron</term><term>Iron Particles</term><term>Iron loading</term><term>Iron-based catalyst</term><term>Lignin</term><term>Lignin pyrolysis</term><term>Metallic compounds</term><term>Methane</term><term>Model compound</term><term>Molybdenum oxide</term><term>Paramagnetism</term><term>Phenols</term><term>Reaction mechanism</term><term>Selective catalysts</term><term>Silica</term><term>Spent catalyst</term><term>Ssbauer spectroscopies</term><term>TEM observations</term><term>Toluene</term><term>XRD</term></keywords><keywords scheme="Wicri" type="topic" xml:lang="fr"><term>Fer</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Fe/SiO2 is shown to be a selective catalyst for guaiacol hydrodeoxygenation (HDO). Guaiacol is used as a model compound to study the conversion of lignin pyrolysis vapours into aromatics (benzene, phenols). The effect of each individual gas present in a pyrolysis gas (H2, CO, CO2, H2O, CH4) on the selectivity of a 10wt% Fe/SiO2 catalyst is studied (673K, atmospheric pressure, 50mol% H2, 1/WHSV=0.6gcath/ggua). The speciation of the iron phase (metallic (α-Fe), carbide (Fe5C2), oxide (Fe3O4), and super-paramagnetic) in spent catalysts is revealed by XRD and Mössbauer spectroscopy as a function of gases composition. At least 3 types of carbonaceous deposit were evidenced by TPO analysis. TEM observations showed that iron particles size is not markedly affected by the reaction and that carbon deposit mainly occurs in the vicinity of iron particles. When all the gases except methane (Guaiacol+H2+CO+CO2+H2O) are simultaneously in the feed stream, the conditions are still sufficiently reducing to maintain the activity of the catalyst (66% of benzene and toluene carbon yield, 7.5gcath/ggua). The effects of support (silica or activated carbon-AC) and iron loading (5, 10, 15wt% Fe/SiO2) were also studied. 10wt% Fe/AC has a higher selectivity in phenol and cresols production than Fe/SiO2. Active sites and reaction mechanisms are discussed.</div></front></TEI><hal api="V3"><titleStmt><title xml:lang="en">Gas-phase hydrodeoxygenation of guaiacol over iron-based catalysts. Effect of gases composition, iron load and supports (silica and activated carbon)</title><author role="aut"><persName><forename type="first">Roberto N.</forename><surname>Olcese</surname></persName><email></email><idno type="halauthor">892198</idno><affiliation ref="#struct-402153"></affiliation></author><author role="aut"><persName><forename type="first">M. M.</forename><surname>Bettahar</surname></persName><email></email><idno type="halauthor">892193</idno><affiliation ref="#struct-162285"></affiliation></author><author role="aut"><persName><forename type="first">Bernard</forename><surname>Malaman</surname></persName><email></email><idno type="halauthor">172069</idno><affiliation ref="#struct-104710"></affiliation></author><author role="aut"><persName><forename type="first">Jaafar</forename><surname>Ghanbaja</surname></persName><email></email><idno type="halauthor">447890</idno><affiliation ref="#struct-104710"></affiliation></author><author role="aut"><persName><forename type="first">L.</forename><surname>Tibavizco</surname></persName><email></email><idno type="halauthor">892208</idno><affiliation ref="#struct-211875"></affiliation></author><author role="aut"><persName><forename type="first">Dominique</forename><surname>Petitjean</surname></persName><email></email><idno type="halauthor">892174</idno><affiliation ref="#struct-402153"></affiliation></author><author role="crp"><persName><forename type="first">Anthony</forename><surname>Dufour</surname></persName><email>anthony.dufour@univ-lorraine.fr</email><idno type="halauthor">806469</idno><affiliation ref="#struct-402153"></affiliation></author><editor role="depositor"><persName><forename>Gabriel</forename><surname>Wild</surname></persName><email>gabriel.wild@univ-lorraine.fr</email></editor></titleStmt><editionStmt><edition n="v1" type="current"><date type="whenSubmitted">2013-09-25 15:40:53</date><date type="whenWritten">2012</date><date type="whenModified">2016-05-10 16:53:59</date><date type="whenReleased">2013-09-25 15:40:53</date><date type="whenProduced">2013-01-07</date></edition><respStmt><resp>contributor</resp><name key="179637"><persName><forename>Gabriel</forename><surname>Wild</surname></persName><email>gabriel.wild@univ-lorraine.fr</email></name></respStmt></editionStmt><publicationStmt><distributor>CCSD</distributor><idno type="halId">hal-00866008</idno><idno type="halUri">https://hal.archives-ouvertes.fr/hal-00866008</idno><idno type="halBibtex">olcese:hal-00866008</idno><idno type="halRefHtml">Applied Catalysis B: Environmental, Elsevier, 2013, 129, pp.528-538. <10.1016/j.apcatb.2012.09.043></idno><idno type="halRef">Applied Catalysis B: Environmental, Elsevier, 2013, 129, pp.528-538. <10.1016/j.apcatb.2012.09.043></idno></publicationStmt><seriesStmt><idno type="stamp" n="CNRS">CNRS - Centre national de la recherche scientifique</idno><idno type="stamp" n="UNIV-LORRAINE">Université de Lorraine</idno><idno type="stamp" n="INC-CNRS">Institut de Chimie du CNRS</idno><idno type="stamp" n="IJL-UL">Institut Jean Lamour</idno><idno type="stamp" n="LRGP-UL">LRGP</idno></seriesStmt><notesStmt><note type="audience" n="2">International</note><note type="popular" n="0">No</note><note type="peer" n="1">Yes</note></notesStmt><sourceDesc><biblStruct><analytic><title xml:lang="en">Gas-phase hydrodeoxygenation of guaiacol over iron-based catalysts. Effect of gases composition, iron load and supports (silica and activated carbon)</title><author role="aut"><persName><forename type="first">Roberto N.</forename><surname>Olcese</surname></persName><idno type="halAuthorId">892198</idno><affiliation ref="#struct-402153"></affiliation></author><author role="aut"><persName><forename type="first">M. M.</forename><surname>Bettahar</surname></persName><idno type="halAuthorId">892193</idno><affiliation ref="#struct-162285"></affiliation></author><author role="aut"><persName><forename type="first">Bernard</forename><surname>Malaman</surname></persName><idno type="halAuthorId">172069</idno><affiliation ref="#struct-104710"></affiliation></author><author role="aut"><persName><forename type="first">Jaafar</forename><surname>Ghanbaja</surname></persName><idno type="halAuthorId">447890</idno><affiliation ref="#struct-104710"></affiliation></author><author role="aut"><persName><forename type="first">L.</forename><surname>Tibavizco</surname></persName><idno type="halAuthorId">892208</idno><affiliation ref="#struct-211875"></affiliation></author><author role="aut"><persName><forename type="first">Dominique</forename><surname>Petitjean</surname></persName><idno type="halAuthorId">892174</idno><affiliation ref="#struct-402153"></affiliation></author><author role="crp"><persName><forename type="first">Anthony</forename><surname>Dufour</surname></persName><email>anthony.dufour@univ-lorraine.fr</email><idno type="halAuthorId">806469</idno><affiliation ref="#struct-402153"></affiliation></author></analytic><monogr><idno type="halJournalId" status="VALID">10609</idno><idno type="issn">0926-3373</idno><title level="j">Applied Catalysis B: Environmental</title><imprint><publisher>Elsevier</publisher><biblScope unit="volume">129</biblScope><biblScope unit="pp">528-538</biblScope><date type="datePub">2013-01-07</date></imprint></monogr><idno type="doi">10.1016/j.apcatb.2012.09.043</idno></biblStruct></sourceDesc><profileDesc><langUsage><language ident="en">English</language></langUsage><textClass><keywords scheme="author"><term xml:lang="en">TEM observations</term><term xml:lang="en">Ssbauer spectroscopies</term><term xml:lang="en">Spent catalyst</term><term xml:lang="en">Biorefinery</term><term xml:lang="en">Chemicals</term><term xml:lang="en">Hydrotreatment</term><term xml:lang="en">Lignin</term><term xml:lang="en">Active site</term><term xml:lang="en">Aromatic</term><term xml:lang="en">Benzene and Toluene</term><term xml:lang="en">Biorefineries</term><term xml:lang="en">Carbon deposites</term><term xml:lang="en">Carbon yield</term><term xml:lang="en">Carbonaceous deposits</term><term xml:lang="en">Feed streams</term><term xml:lang="en">Gasphase</term><term xml:lang="en">Hydrodeoxygenation</term><term xml:lang="en">Iron loading</term><term xml:lang="en">Iron Particles</term><term xml:lang="en">Iron-based catalyst</term><term xml:lang="en">Lignin pyrolysis</term><term xml:lang="en">Model compound</term><term xml:lang="en">Reaction mechanism</term><term xml:lang="en">Selective catalysts</term><term xml:lang="en">Methane</term><term xml:lang="en">Molybdenum oxide</term><term xml:lang="en">Paramagnetism</term><term xml:lang="en">Phenols</term><term xml:lang="en">Silica</term><term xml:lang="en">Toluene</term><term xml:lang="en">Metallic compounds</term><term xml:lang="en">Gases</term><term xml:lang="en">Iron</term><term xml:lang="en">Deposits</term><term xml:lang="en">Catalyst activity</term><term xml:lang="en">Carbon dioxide</term><term xml:lang="en">Carbides</term><term xml:lang="en">Benzene</term><term xml:lang="en">Atmospheric pressure</term><term xml:lang="en">Activated carbon</term><term xml:lang="en">Alcohols</term><term xml:lang="en">XRD</term></keywords><classCode scheme="halDomain" n="spi.gproc">Engineering Sciences [physics]/Chemical and Process Engineering</classCode><classCode scheme="halDomain" n="chim.cata">Chemical Sciences/Catalysis</classCode><classCode scheme="halDomain" n="phys.cond.cm-ms">Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]</classCode><classCode scheme="halDomain" n="chim.inor">Chemical Sciences/Inorganic chemistry</classCode><classCode scheme="halTypology" n="ART">Journal articles</classCode></textClass><abstract xml:lang="en">Fe/SiO2 is shown to be a selective catalyst for guaiacol hydrodeoxygenation (HDO). Guaiacol is used as a model compound to study the conversion of lignin pyrolysis vapours into aromatics (benzene, phenols). The effect of each individual gas present in a pyrolysis gas (H2, CO, CO2, H2O, CH4) on the selectivity of a 10wt% Fe/SiO2 catalyst is studied (673K, atmospheric pressure, 50mol% H2, 1/WHSV=0.6gcath/ggua). The speciation of the iron phase (metallic (α-Fe), carbide (Fe5C2), oxide (Fe3O4), and super-paramagnetic) in spent catalysts is revealed by XRD and Mössbauer spectroscopy as a function of gases composition. At least 3 types of carbonaceous deposit were evidenced by TPO analysis. TEM observations showed that iron particles size is not markedly affected by the reaction and that carbon deposit mainly occurs in the vicinity of iron particles. When all the gases except methane (Guaiacol+H2+CO+CO2+H2O) are simultaneously in the feed stream, the conditions are still sufficiently reducing to maintain the activity of the catalyst (66% of benzene and toluene carbon yield, 7.5gcath/ggua). The effects of support (silica or activated carbon-AC) and iron loading (5, 10, 15wt% Fe/SiO2) were also studied. 10wt% Fe/AC has a higher selectivity in phenol and cresols production than Fe/SiO2. Active sites and reaction mechanisms are discussed.</abstract></profileDesc></hal></record>Pour manipuler ce document sous Unix (Dilib)
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