Selectivity of Bio-oils Catalytic Hydrotreatment Assessed by Petroleomic and GC*GC/MS-FID Analysis
Identifieur interne : 000708 ( Main/Exploration ); précédent : 000707; suivant : 000709Selectivity of Bio-oils Catalytic Hydrotreatment Assessed by Petroleomic and GC*GC/MS-FID Analysis
Auteurs : Roberto Olcese [France] ; Vincent Carre [France] ; Frédéric Aubriet [France] ; Anthony Dufour (génie des procédés) [France]Source :
- Energy & fuels [ 0887-0624 ] ; 2013.
Descripteurs français
- Pascal (Inist)
- Hydrotraitement, Sélectivité catalyseur, Haute résolution, Spectrométrie masse, Transformation Fourier, Résonance cyclotronique, Détecteur ionisation flamme, Méthanol, Lignine, Pyrolyse, Fer, Catalyseur sur support, Norme, Désorption laser, Ionisation, Lit fixe, Silice, Charbon actif, Teneur oxygène, Oligomère.
- Wicri :
English descriptors
- KwdEn :
- Activated carbon, Catalyst selectivity, Cyclotron resonance, Fixed bed, Flame ionization detector, Fourier transformation, High resolution, Hydrotreating, Ionization, Iron, Laser desorption, Lignin, Mass spectrometry, Methanol, Oligomer, Oxygen content, Pyrolysis, Silica, Standards, Supported catalyst.
- mix :
- Activated carbon, Catalytic hydrotreatment, Catalytic treatment, Chemical analysis, Fourier transform ion cyclotron resonance, High resolution mass spectrometry, Hydrotreatment catalysts, Ionization detectors, Iron, Iron-based catalyst, Laser desorption ionization, Lignin, Mass spectrometry, Oligomers, Silica.
Abstract
We propose to assess the selectivity of hydrotreatment catalysts by two complementary analytical methods: (1) high-resolution mass spectrometry (MS), called "petroleomic" analysis, by Fourier transform ion cyclotron resonance (FT ICR, 9.4T) MS for species heavier than m/z of about 200 Da and (2) quantitative GC*GC (heart-cutting)/MS-flame ionization detector (FID) analysis of lighter species. The methodology is illustrated on methanol-soluble bio-oils produced by lignin pyrolysis and hydrotreated by iron-based catalysts. GC*GC analysis is calibrated by a combination of internal standard and prediction of response factors on the FID. Laser desorption ionization (LDI) and electro spray ionization (ESI) in negative-ion mode are combined for the petroleomic analysis. The selectivity of hydrotreatment (catalytic fixed bed, 1 atm, 400 °C) is assessed as a function of catalyst loads and iron support (silica and activated carbon). Hundreds of species are analyzed by GC*GC and petroleomic and mapped in Van Krevelen diagrams. The high selectivity of reduced iron for the hydrodeoxygenation of lignin pyrolysis vapors is demonstrated. The effect of the catalytic treatment on oxygen content and unsaturation is studied for a broad range of species: from C2 to C14 by GC analysis and from C8 to C37 by petroleomic. Many heavy lignin oligomers produced by the pyrolysis are trapped by the catalytic bed, highlighting the need of new catalytic systems to convert them into valuable fuels or chemicals.
Url:
Affiliations:
- France
- Grand Est, Lorraine (région)
- Metz, Nancy
- Centre national de la recherche scientifique, Laboratoire réactions et génie des procédés, Université de Lorraine
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Metz</s2><s3>FRA</s3><sZ>2 aut.</sZ><sZ>3 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">Metz</settlement></placeName></affiliation></author><author><name sortKey="Dufour, Anthony" sort="Dufour, Anthony" uniqKey="Dufour A" first="Anthony" last="Dufour">Anthony Dufour (génie des procédés)</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Reactions and Processes Engineering Laboratory, CNRS, Lorraine University, ENSIC, 1 rue Grandville</s1><s2>54000 Nancy</s2><s3>FRA</s3><sZ>1 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">Nancy</settlement></placeName><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">Energy & fuels</title><title level="j" type="abbreviated">Energy fuels</title><idno type="ISSN">0887-0624</idno><imprint><date when="2013">2013</date></imprint></series></biblStruct></sourceDesc><seriesStmt><title level="j" type="main">Energy & fuels</title><title level="j" type="abbreviated">Energy fuels</title><idno type="ISSN">0887-0624</idno></seriesStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Activated carbon</term><term>Catalyst selectivity</term><term>Cyclotron resonance</term><term>Fixed bed</term><term>Flame ionization detector</term><term>Fourier transformation</term><term>High resolution</term><term>Hydrotreating</term><term>Ionization</term><term>Iron</term><term>Laser desorption</term><term>Lignin</term><term>Mass spectrometry</term><term>Methanol</term><term>Oligomer</term><term>Oxygen content</term><term>Pyrolysis</term><term>Silica</term><term>Standards</term><term>Supported catalyst</term></keywords><keywords scheme="Pascal" xml:lang="fr"><term>Hydrotraitement</term><term>Sélectivité catalyseur</term><term>Haute résolution</term><term>Spectrométrie masse</term><term>Transformation Fourier</term><term>Résonance cyclotronique</term><term>Détecteur ionisation flamme</term><term>Méthanol</term><term>Lignine</term><term>Pyrolyse</term><term>Fer</term><term>Catalyseur sur support</term><term>Norme</term><term>Désorption laser</term><term>Ionisation</term><term>Lit fixe</term><term>Silice</term><term>Charbon actif</term><term>Teneur oxygène</term><term>Oligomère</term></keywords><keywords scheme="Wicri" type="topic" xml:lang="fr"><term>Fer</term><term>Méthanol</term><term>Fer</term><term>Norme</term></keywords><keywords scheme="mix" xml:lang="en"><term>Activated carbon</term><term>Catalytic hydrotreatment</term><term>Catalytic treatment</term><term>Chemical analysis</term><term>Fourier transform ion cyclotron resonance</term><term>High resolution mass spectrometry</term><term>Hydrotreatment catalysts</term><term>Ionization detectors</term><term>Iron</term><term>Iron-based catalyst</term><term>Laser desorption ionization</term><term>Lignin</term><term>Mass spectrometry</term><term>Oligomers</term><term>Silica</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">We propose to assess the selectivity of hydrotreatment catalysts by two complementary analytical methods: (1) high-resolution mass spectrometry (MS), called "petroleomic" analysis, by Fourier transform ion cyclotron resonance (FT ICR, 9.4T) MS for species heavier than m/z of about 200 Da and (2) quantitative GC<sup>*</sup>GC (heart-cutting)/MS-flame ionization detector (FID) analysis of lighter species. The methodology is illustrated on methanol-soluble bio-oils produced by lignin pyrolysis and hydrotreated by iron-based catalysts. GC<sup>*</sup>GC analysis is calibrated by a combination of internal standard and prediction of response factors on the FID. Laser desorption ionization (LDI) and electro spray ionization (ESI) in negative-ion mode are combined for the petroleomic analysis. The selectivity of hydrotreatment (catalytic fixed bed, 1 atm, 400 °C) is assessed as a function of catalyst loads and iron support (silica and activated carbon). Hundreds of species are analyzed by GC<sup>*</sup>GC and petroleomic and mapped in Van Krevelen diagrams. The high selectivity of reduced iron for the hydrodeoxygenation of lignin pyrolysis vapors is demonstrated. The effect of the catalytic treatment on oxygen content and unsaturation is studied for a broad range of species: from C<sub>2</sub> to C<sub>14</sub> by GC analysis and from C<sub>8</sub> to C<sub>37</sub> by petroleomic. Many heavy lignin oligomers produced by the pyrolysis are trapped by the catalytic bed, highlighting the need of new catalytic systems to convert them into valuable fuels or chemicals.</div></front></TEI><affiliations><list><country><li>France</li></country><region><li>Grand Est</li><li>Lorraine (région)</li></region><settlement><li>Metz</li><li>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, Roberto" sort="Olcese, Roberto" uniqKey="Olcese R" first="Roberto" last="Olcese">Roberto Olcese</name></region><name sortKey="Aubriet, Frederic" sort="Aubriet, Frederic" uniqKey="Aubriet F" first="Frédéric" last="Aubriet">Frédéric Aubriet</name><name sortKey="Carre, Vincent" sort="Carre, Vincent" uniqKey="Carre V" first="Vincent" last="Carre">Vincent Carre</name><name sortKey="Dufour, Anthony" sort="Dufour, Anthony" uniqKey="Dufour A" first="Anthony" last="Dufour">Anthony Dufour (génie des procédés)</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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