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Hydrodeoxygenation of phenolics in liquid phase over supported MoO3 and carburized analogues

Rune Lodeng, Chanakya Ranga UGent, Tapas Rajkhowa UGent, Vaios Alexiadis UGent, Hilde Bjørkan, Svatopluk Chytil, Ingeborg Svenum, John Walmsley and Joris Thybaut UGent (2017) BIOMASS CONVERSION AND BIOREFINERY. 7(3). p.343-359
abstract
Catalytic hydrodeoxygenation (HDO) of monoaromatic components of increasing structural and chemical complexity, represented by phenol (−OH), anisole (−OCH3), and guaiacol (−OH + −OCH3), was performed in a down-flow trickle-bed reactor. ZrO2 supported Mo oxide with nominal loadings of 7, 15, and 25 wt% Mo were prepared and carburized analogues were synthesized at two thermal severity levels in a mixture of 20% CH4 in H2. HDO performance was compared with ZrO2 and Al2O3 supported CoMo-oxide reference catalysts. Performance was studied in the temperature range 573–648 K and a pressure of 6 MPa at liquid hourly space velocities (LHSVs) of 0.25–4.9 greactant/gcat, h at a H2/ phenolic molar ratio of ca. 108. The intermediate Mo loading oxide catalysts showed superior performance. The parent Mo oxides were also more active than their carburized analogues and dominating hydrogenolysis pathways gave similar products and distribution. Carburization caused structural changes by reduction of MoO3 and formation of minor amounts of surface carbon. The weak hydrogenation activity did not change significantly. Reaction pathways were elucidated and ca. 100% selectivity to non-oxygenates in a wide conversion range was obtained from phenol. Anisole HDO was proceeding with ca. 85% selectivity to non-oxygenates. Structural complexity of guaiacol was causing even less efficient deoxygenation with a selectivity to non-oxygenates of only 5–10%. Catalysts were characterized by, N2-BET, CO-chemisorption, ICP-OES, XRD, TPR, XPS, (S)TEM-EDX, combustion-IR, and correlated to kinetic performance.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
keyword
PHOSPHIDE HYDROPROCESSING CATALYSTS, TRANSITION-METAL PHOSPHIDES, FAST PYROLYSIS OIL, MOLYBDENUM OXIDE, HYDROTREATING CATALYSTS, MODEL COMPOUNDS, BIO-OIL, BIOMASS, HYDRODESULFURIZATION, NITRIDES
journal title
BIOMASS CONVERSION AND BIOREFINERY
volume
7
issue
3
pages
343 - 359
Web of Science type
Article
ISSN
2190-6815
DOI
10.1007/s13399-017-0252-z
language
English
UGent publication?
yes
classification
A2
id
8537475
handle
http://hdl.handle.net/1854/LU-8537475
date created
2017-11-14 15:36:36
date last changed
2017-11-17 10:13:33
@article{8537475,
  abstract     = {Catalytic hydrodeoxygenation (HDO) of monoaromatic components of increasing structural and chemical
complexity, represented by phenol (\ensuremath{-}OH), anisole (\ensuremath{-}OCH3), and guaiacol (\ensuremath{-}OH + \ensuremath{-}OCH3), was performed in a down-flow trickle-bed reactor. ZrO2 supported Mo oxide with nominal loadings of 7, 15, and 25 wt\% Mo were prepared and carburized analogues were synthesized at two thermal severity levels in a mixture of 20\% CH4 in H2. HDO performance
was compared with ZrO2 and Al2O3 supported CoMo-oxide reference catalysts. Performance was studied in the temperature range 573--648 K and a pressure of 6 MPa at liquid hourly space velocities (LHSVs) of 0.25--4.9 greactant/gcat, h at a H2/ phenolic molar ratio of ca. 108. The intermediate Mo loading oxide catalysts showed superior performance. The parent Mo oxides were also more active than their carburized analogues and dominating hydrogenolysis pathways gave similar products and distribution. Carburization caused structural changes by reduction of MoO3 and formation of minor amounts of surface carbon. The weak hydrogenation activity did not change significantly. Reaction pathways were elucidated and ca. 100\% selectivity to non-oxygenates in a wide conversion
range was obtained from phenol. Anisole HDO was proceeding with ca. 85\% selectivity to non-oxygenates. Structural
complexity of guaiacol was causing even less efficient deoxygenation with a selectivity to non-oxygenates of only
5--10\%. Catalysts were characterized by, N2-BET, CO-chemisorption, ICP-OES, XRD, TPR, XPS, (S)TEM-EDX, combustion-IR, and correlated to kinetic performance.},
  author       = {Lodeng, Rune and Ranga, Chanakya and Rajkhowa, Tapas and Alexiadis, Vaios and Bj{\o}rkan, Hilde and Chytil, Svatopluk and Svenum, Ingeborg and Walmsley, John and Thybaut, Joris},
  issn         = {2190-6815 },
  journal      = {BIOMASS CONVERSION AND BIOREFINERY},
  keyword      = {PHOSPHIDE HYDROPROCESSING CATALYSTS,TRANSITION-METAL PHOSPHIDES,FAST PYROLYSIS OIL,MOLYBDENUM OXIDE,HYDROTREATING CATALYSTS,MODEL COMPOUNDS,BIO-OIL,BIOMASS,HYDRODESULFURIZATION,NITRIDES},
  language     = {eng},
  number       = {3},
  pages        = {343--359},
  title        = {Hydrodeoxygenation of phenolics in liquid phase over supported MoO3 and carburized analogues},
  url          = {http://dx.doi.org/10.1007/s13399-017-0252-z},
  volume       = {7},
  year         = {2017},
}

Chicago
Lodeng, Rune, Chanakya Ranga, Tapas Rajkhowa, Vaios Alexiadis, Hilde Bjørkan, Svatopluk Chytil, Ingeborg Svenum, John Walmsley, and Joris Thybaut. 2017. “Hydrodeoxygenation of Phenolics in Liquid Phase over Supported MoO3 and Carburized Analogues.” Biomass Conversion and Biorefinery 7 (3): 343–359.
APA
Lodeng, R., Ranga, C., Rajkhowa, T., Alexiadis, V., Bjørkan, H., Chytil, S., Svenum, I., et al. (2017). Hydrodeoxygenation of phenolics in liquid phase over supported MoO3 and carburized analogues. BIOMASS CONVERSION AND BIOREFINERY, 7(3), 343–359.
Vancouver
1.
Lodeng R, Ranga C, Rajkhowa T, Alexiadis V, Bjørkan H, Chytil S, et al. Hydrodeoxygenation of phenolics in liquid phase over supported MoO3 and carburized analogues. BIOMASS CONVERSION AND BIOREFINERY. 2017;7(3):343–59.
MLA
Lodeng, Rune, Chanakya Ranga, Tapas Rajkhowa, et al. “Hydrodeoxygenation of Phenolics in Liquid Phase over Supported MoO3 and Carburized Analogues.” BIOMASS CONVERSION AND BIOREFINERY 7.3 (2017): 343–359. Print.