Selectivity of bio-oils catalytic hydrotreatment assessed by petroleomic and GC*GC/MS-FID analysis
Identifieur interne : 000A19 ( Hal/Curation ); précédent : 000A18; suivant : 000A20Selectivity of bio-oils catalytic hydrotreatment assessed by petroleomic and GC*GC/MS-FID analysis
Auteurs : Roberto Olcese [France] ; Vincent Carré [France] ; Frederic Aubriet [France] ; Anthony Dufour [France]Source :
- Energy and Fuels [ 0887-0624 ] ; 2013-04-18.
Descripteurs français
- Wicri :
- topic : Fer.
English descriptors
- 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
Selectivity of bio-oils catalytic hydrotreatment assessed by petroleomic and GC*GC/MS-FID analysisWe 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:
DOI: 10.1021/ef302145g
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<profileDesc><textClass><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>
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<front><div type="abstract" xml:lang="en">Selectivity of bio-oils catalytic hydrotreatment assessed by petroleomic and GC*GC/MS-FID analysisWe 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.</div>
</front>
</TEI>
<hal api="V3"><titleStmt><title xml:lang="en">Selectivity of bio-oils catalytic hydrotreatment assessed by petroleomic and GC*GC/MS-FID analysis</title>
<author role="aut"><persName><forename type="first">Roberto</forename>
<surname>Olcese</surname>
</persName>
<email></email>
<idno type="halauthor">806471</idno>
<affiliation ref="#struct-402153"></affiliation>
</author>
<author role="aut"><persName><forename type="first">Vincent</forename>
<surname>Carré</surname>
</persName>
<email></email>
<idno type="halauthor">605517</idno>
<affiliation ref="#struct-439404"></affiliation>
</author>
<author role="aut"><persName><forename type="first">Frederic</forename>
<surname>Aubriet</surname>
</persName>
<email></email>
<idno type="halauthor">457644</idno>
<affiliation ref="#struct-439404"></affiliation>
</author>
<author role="aut"><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>
<funder>Région Lorraine</funder>
</titleStmt>
<editionStmt><edition n="v1" type="current"><date type="whenSubmitted">2013-09-25 15:17:13</date>
<date type="whenModified">2016-05-10 16:53:24</date>
<date type="whenReleased">2013-09-25 15:17:13</date>
<date type="whenProduced">2013-04-18</date>
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<name key="179637"><persName><forename>Gabriel</forename>
<surname>Wild</surname>
</persName>
<email>gabriel.wild@univ-lorraine.fr</email>
</name>
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<idno type="halId">hal-00865994</idno>
<idno type="halUri">https://hal.archives-ouvertes.fr/hal-00865994</idno>
<idno type="halBibtex">olcese:hal-00865994</idno>
<idno type="halRefHtml">Energy and Fuels, American Chemical Society, 2013, 27 (4), pp.2135-2145. <10.1021/ef302145g></idno>
<idno type="halRef">Energy and Fuels, American Chemical Society, 2013, 27 (4), pp.2135-2145. <10.1021/ef302145g></idno>
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<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="LRGP-UL">LRGP</idno>
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<notesStmt><note type="audience" n="2">International</note>
<note type="popular" n="0">No</note>
<note type="peer" n="1">Yes</note>
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<sourceDesc><biblStruct><analytic><title xml:lang="en">Selectivity of bio-oils catalytic hydrotreatment assessed by petroleomic and GC*GC/MS-FID analysis</title>
<author role="aut"><persName><forename type="first">Roberto</forename>
<surname>Olcese</surname>
</persName>
<idno type="halAuthorId">806471</idno>
<affiliation ref="#struct-402153"></affiliation>
</author>
<author role="aut"><persName><forename type="first">Vincent</forename>
<surname>Carré</surname>
</persName>
<idno type="halAuthorId">605517</idno>
<affiliation ref="#struct-439404"></affiliation>
</author>
<author role="aut"><persName><forename type="first">Frederic</forename>
<surname>Aubriet</surname>
</persName>
<idno type="halAuthorId">457644</idno>
<affiliation ref="#struct-439404"></affiliation>
</author>
<author role="aut"><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>
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<monogr><idno type="halJournalId" status="VALID">4619</idno>
<idno type="issn">0887-0624</idno>
<idno type="eissn">1520-5029</idno>
<title level="j">Energy and Fuels</title>
<imprint><publisher>American Chemical Society</publisher>
<biblScope unit="volume">27</biblScope>
<biblScope unit="issue">4</biblScope>
<biblScope unit="pp">2135-2145</biblScope>
<date type="datePub">2013-04-18</date>
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<idno type="doi">10.1021/ef302145g</idno>
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<profileDesc><langUsage><language ident="en">English</language>
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<textClass><keywords scheme="author"><term xml:lang="en">Catalytic hydrotreatment</term>
<term xml:lang="en">Catalytic treatment</term>
<term xml:lang="en">Fourier transform ion cyclotron resonance</term>
<term xml:lang="en">High resolution mass spectrometry</term>
<term xml:lang="en">Hydrotreatment catalysts</term>
<term xml:lang="en">Ionization detectors</term>
<term xml:lang="en">Iron-based catalyst</term>
<term xml:lang="en">Laser desorption ionization</term>
<term xml:lang="en">Activated carbon</term>
<term xml:lang="en">Chemical analysis</term>
<term xml:lang="en">Iron</term>
<term xml:lang="en">Lignin</term>
<term xml:lang="en">Mass spectrometry</term>
<term xml:lang="en">Oligomers</term>
<term xml:lang="en">Silica</term>
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<classCode scheme="halDomain" n="spi.gproc">Engineering Sciences [physics]/Chemical and Process Engineering</classCode>
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<classCode scheme="halTypology" n="ART">Journal articles</classCode>
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<abstract xml:lang="en">Selectivity of bio-oils catalytic hydrotreatment assessed by petroleomic and GC*GC/MS-FID analysisWe 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.</abstract>
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