Gas-phase hydrodeoxygenation of guaiacol over iron-based catalysts. Effect of gases composition, iron load and supports (silica and activated carbon)
Identifieur interne : 000771 ( Main/Merge ); précédent : 000770; suivant : 000772Gas-phase hydrodeoxygenation of guaiacol over iron-based catalysts. Effect of gases composition, iron load and supports (silica and activated carbon)
Auteurs : R. Olcese [France] ; M. M. Bettahar [France] ; B. Malaman [France] ; J. Ghanbaja [France] ; L. Tibavizco [France] ; D. Petitjean [France] ; Anthony Dufour (génie des procédés) [France]Source :
- Applied catalysis. B, Environmental [ 0926-3373 ] ; 2013.
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Abstract
Fe/Si02 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 (673 K, atmospheric pressure, 50 mol% H2, 1/WHSV = 0.6 gcat h/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 + H20) 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, 7.5 gcat h/ggua). The effects of support (silica or activated carbon-AC) and iron loading (5, 10, 15 wt% Fe/Si02) 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.
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Effect of gases composition, iron load and supports (silica and activated carbon)</title><author><name sortKey="Olcese, R" sort="Olcese, R" uniqKey="Olcese R" first="R." last="Olcese">R. Olcese</name><affiliation wicri:level="4"><inist:fA14 i1="01"><s1>LRGP, CNRS, Université de Lorraine, ENSIC, 1, Rue Grandville</s1><s2>Nancy</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>7 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region">Grand Est</region><region type="old region">Lorraine (région)</region><settlement type="city">Nancy</settlement></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author><author><name sortKey="Bettahar, M M" sort="Bettahar, M M" uniqKey="Bettahar M" first="M. M." last="Bettahar">M. M. Bettahar</name><affiliation wicri:level="4"><inist:fA14 i1="02"><s1>SRSMC, CNRS, Université de Lorraine, Faculté des Sciences, Bvd. des Aiguillettes</s1><s2>54506 Vandoeuvre-les-Nancy</s2><s3>FRA</s3><sZ>2 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region><settlement type="city">Vandoeuvre-les-Nancy</settlement></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author><author><name sortKey="Malaman, B" sort="Malaman, B" uniqKey="Malaman B" first="B." last="Malaman">B. Malaman</name><affiliation wicri:level="4"><inist:fA14 i1="03"><s1>IJL, CNRS, Université de Lorraine, Faculté des Sciences, Bv. Des Aiguillettes</s1><s2>Vandoeuvre-les-Nancy</s2><s3>FRA</s3><sZ>3 aut.</sZ><sZ>4 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region><settlement type="city">Vandœuvre-lès-Nancy</settlement><settlement type="city" wicri:auto="agglo">Nancy</settlement></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author><author><name sortKey="Ghanbaja, J" sort="Ghanbaja, J" uniqKey="Ghanbaja J" first="J." last="Ghanbaja">J. Ghanbaja</name><affiliation wicri:level="4"><inist:fA14 i1="03"><s1>IJL, CNRS, Université de Lorraine, Faculté des Sciences, Bv. Des Aiguillettes</s1><s2>Vandoeuvre-les-Nancy</s2><s3>FRA</s3><sZ>3 aut.</sZ><sZ>4 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region><settlement type="city">Vandœuvre-lès-Nancy</settlement><settlement type="city" wicri:auto="agglo">Nancy</settlement></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author><author><name sortKey="Tibavizco, L" sort="Tibavizco, L" uniqKey="Tibavizco L" first="L." last="Tibavizco">L. Tibavizco</name><affiliation wicri:level="4"><inist:fA14 i1="01"><s1>LRGP, CNRS, Université de Lorraine, ENSIC, 1, Rue Grandville</s1><s2>Nancy</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>7 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region">Grand Est</region><region type="old region">Lorraine (région)</region><settlement type="city">Nancy</settlement></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author><author><name sortKey="Petitjean, D" sort="Petitjean, D" uniqKey="Petitjean D" first="D." last="Petitjean">D. Petitjean</name><affiliation wicri:level="4"><inist:fA14 i1="01"><s1>LRGP, CNRS, Université de Lorraine, ENSIC, 1, Rue Grandville</s1><s2>Nancy</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>7 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region">Grand Est</region><region type="old region">Lorraine (région)</region><settlement type="city">Nancy</settlement></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author><author><name sortKey="Dufour, A" sort="Dufour, A" uniqKey="Dufour A" first="A." last="Dufour">Anthony Dufour (génie des procédés)</name><affiliation wicri:level="4"><inist:fA14 i1="01"><s1>LRGP, CNRS, Université de Lorraine, ENSIC, 1, Rue Grandville</s1><s2>Nancy</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>5 aut.</sZ><sZ>6 aut.</sZ><sZ>7 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region">Grand Est</region><region type="old region">Lorraine (région)</region><settlement type="city">Nancy</settlement></placeName><orgName type="university">Université de Lorraine</orgName><placeName><settlement type="city">Nancy</settlement><region type="region" nuts="2">Grand Est</region><region type="region" nuts="2">Lorraine (région)</region></placeName><orgName type="laboratoire" n="5">Laboratoire réactions et génie des procédés</orgName><orgName type="university">Université de Lorraine</orgName><orgName type="institution">Centre national de la recherche scientifique</orgName></affiliation></author></analytic><series><title level="j" type="main">Applied catalysis. B, Environmental</title><title level="j" type="abbreviated">Appl. catal., B Environ.</title><idno type="ISSN">0926-3373</idno><imprint><date when="2013">2013</date></imprint></series></biblStruct></sourceDesc><seriesStmt><title level="j" type="main">Applied catalysis. B, Environmental</title><title level="j" type="abbreviated">Appl. catal., B Environ.</title><idno type="ISSN">0926-3373</idno></seriesStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Activated carbon</term><term>Catalyst</term><term>Composition</term><term>Environmental protection</term><term>Gas phase</term><term>Gases</term><term>Guaiacol</term><term>Heterogeneous catalysis</term><term>Iron</term><term>Lignin</term><term>Silica</term><term>Supported catalyst</term></keywords><keywords scheme="Pascal" xml:lang="fr"><term>Phase gazeuse</term><term>Guaiacol</term><term>Fer</term><term>Catalyseur</term><term>Gaz</term><term>Composition</term><term>Silice</term><term>Charbon actif</term><term>Lignine</term><term>Catalyse hétérogène</term><term>Protection environnement</term><term>Catalyseur sur support</term><term>SiO2</term></keywords><keywords scheme="Wicri" type="topic" xml:lang="fr"><term>Fer</term><term>Gaz</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Fe/Si0<sub>2</sub> 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 (H<sub>2</sub>, CO, CO<sub>2</sub>, H<sub>2</sub>O, CH<sub>4</sub>) on the selectivity of a 10wt% Fe/SiO<sub>2</sub> catalyst is studied (673 K, atmospheric pressure, 50 mol% H<sub>2</sub>, 1/WHSV = 0.6 g<sub>cat</sub> h/g<sub>gua</sub>). The speciation of the iron phase (metallic (α-Fe), carbide (Fe<sub>5</sub>C<sub>2</sub>), oxide (Fe<sub>3</sub>O<sub>4</sub>), 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 + H<sub>2</sub> + CO + CO<sub>2</sub> + H<sub>2</sub>0) 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, 7.5 g<sub>cat</sub> h/g<sub>gua</sub>). The effects of support (silica or activated carbon-AC) and iron loading (5, 10, 15 wt% Fe/Si0<sub>2</sub>) were also studied. 10wt% Fe/AC has a higher selectivity in phenol and cresols production than Fe/SiO<sub>2</sub>. Active sites and reaction mechanisms are discussed.</div></front></TEI><affiliations><list><country><li>France</li></country><region><li>Grand Est</li><li>Lorraine (région)</li></region><settlement><li>Nancy</li><li>Vandoeuvre-les-Nancy</li><li>Vandœuvre-lès-Nancy</li></settlement><orgName><li>Centre national de la recherche scientifique</li><li>Laboratoire réactions et génie des procédés</li><li>Université de Lorraine</li></orgName></list><tree><country name="France"><region name="Grand Est"><name sortKey="Olcese, R" sort="Olcese, R" uniqKey="Olcese R" first="R." last="Olcese">R. Olcese</name></region><name sortKey="Bettahar, M M" sort="Bettahar, M M" uniqKey="Bettahar M" first="M. M." last="Bettahar">M. M. Bettahar</name><name sortKey="Dufour, A" sort="Dufour, A" uniqKey="Dufour A" first="A." last="Dufour">Anthony Dufour (génie des procédés)</name><name sortKey="Ghanbaja, J" sort="Ghanbaja, J" uniqKey="Ghanbaja J" first="J." last="Ghanbaja">J. Ghanbaja</name><name sortKey="Malaman, B" sort="Malaman, B" uniqKey="Malaman B" first="B." last="Malaman">B. Malaman</name><name sortKey="Petitjean, D" sort="Petitjean, D" uniqKey="Petitjean D" first="D." last="Petitjean">D. Petitjean</name><name sortKey="Tibavizco, L" sort="Tibavizco, L" uniqKey="Tibavizco L" first="L." last="Tibavizco">L. Tibavizco</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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