Gas-phase hydrodeoxygenation of guaiacol over iron-based catalysts. Effect of gases composition, iron load and supports (silica and activated carbon)

Autor: Dominique Petitjean, Roberto N. Olcese, Bernard Malaman, Mohammed M. Bettahar, L. Tibavizco, Anthony Dufour, Jaafar Ghanbaja
Přispěvatelé: GREENER, Laboratoire Réactions et Génie des Procédés (LRGP), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Structure et Réactivité des Systèmes Moléculaires Complexes (SRSMC), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Institut Jean Lamour (IJL), Université de Lorraine (UL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS)
Rok vydání: 2013
Předmět:
XRD
Iron loading
TEM observations
Lignin pyrolysis
Heterogeneous catalysis
Lignin
7. Clean energy
01 natural sciences
chemistry.chemical_compound
Feed streams
Benzene
Selective catalysts
Spent catalyst
Reaction mechanism
General Environmental Science
Carbon yield
Silica
Biorefineries
Catalyst activity
[PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci]
Atmospheric pressure
Chemicals
Gases
Carbides
Methane
Pyrolysis
Hydrodeoxygenation
Ssbauer spectroscopies
medicine.drug
Iron
Activated carbon
Inorganic chemistry
Oxide
Carbon deposites
[CHIM.INOR]Chemical Sciences/Inorganic chemistry
010402 general chemistry
Paramagnetism
Catalysis
Carbonaceous deposits
Iron-based catalyst
Gasphase
Metallic compounds
Phenols
medicine
Iron Particles
[SPI.GPROC]Engineering Sciences [physics]/Chemical and Process Engineering
Hydrotreatment
010405 organic chemistry
Active site
Process Chemistry and Technology
Benzene and Toluene
[CHIM.CATA]Chemical Sciences/Catalysis
Model compound
Molybdenum oxide
Biorefinery
0104 chemical sciences
Carbon dioxide
chemistry
13. Climate action
Alcohols
Deposits
Guaiacol
Aromatic
Toluene
Zdroj: Applied Catalysis B: Environmental
Applied Catalysis B: Environmental, Elsevier, 2013, 129, pp.528-538. ⟨10.1016/j.apcatb.2012.09.043⟩
ISSN: 0926-3373
DOI: 10.1016/j.apcatb.2012.09.043
Popis: 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 10 wt% 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 Mossbauer 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, 7.5 gcat h/ggua). The effects of support (silica or activated carbon-AC) and iron loading (5, 10, 15 wt% Fe/SiO2) were also studied. 10 wt% Fe/AC has a higher selectivity in phenol and cresols production than Fe/SiO2. Active sites and reaction mechanisms are discussed.
Databáze: OpenAIRE
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