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Title: Comparison of HMF hydrodeoxygenation over different metal catalysts in a continuous flow reactor

Abstract

The three-phase hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) and hydrogenation of 2,5-dimethylfuran (DMF) were studied over six carbon-supported metal catalysts (Pt, Pd, Ir, Ru, Ni, and Co) using a tubular flow reactor with 1-propanol solvent, at 180 °C and 33 bar. By varying the space time in the reactor, the reaction of HMF is shown to be sequential, with HMF reacting first to furfuryl ethers and other partially hydrogenated products, which then form 2,5-dimethylfuran (DMF). Ring-opened products and 2,5-dimethyltetrahydrofuran (DMTHF) were produced only from reaction of DMF. Rate constants for the pseudo-first-order sequential reactions were obtained for each of the metals. The selectivities for the reaction of DMF varied with the metal catalyst, with Pd forming primarily DMTHF, Ir forming a mixture of DMTHF and open-ring products, and the other metals forming primarily open-ring products. Catalyst stabilities followed the order Pt ~ Ir > Pd > Ni > Co > Ru. Since the stability order correlated with carbon balances in the product (>93% for Pt; <75% for Ru), deactivation appears to be caused by deposition of humins on the catalyst.

Authors:
 [1];  [1];  [1];  [2];  [2];  [1]
  1. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemical and Biomolecular Engineering
  2. Univ. of Pennsylvania, Philadelphia, PA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1387337
Alternate Identifier(s):
OSTI ID: 1250114
Grant/Contract Number:  
SC0001004
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Catalysis. A, General
Additional Journal Information:
Journal Volume: 508; Journal Issue: C; Related Information: CCEI partners with the University of Delaware (lead); Brookhaven National Laboratory; California Institute of Technology; Columbia University; University of Delaware; Lehigh University; University of Massachusetts, Amherst; Massachusetts Institute of Technology; University of Minnesota; Pacific Northwest National Laboratory; University of Pennsylvania; Princeton University; Rutgers University; Journal ID: ISSN 0926-860X
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); biofuels (including algae and biomass); bio-inspired; hydrogen and fuel cells; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Luo, Jing, Arroyo-Ramírez, Lisandra, Wei, Jifeng, Yun, Hongseok, Murray, Christopher B., and Gorte, Raymond J. Comparison of HMF hydrodeoxygenation over different metal catalysts in a continuous flow reactor. United States: N. p., 2015. Web. doi:10.1016/j.apcata.2015.10.009.
Luo, Jing, Arroyo-Ramírez, Lisandra, Wei, Jifeng, Yun, Hongseok, Murray, Christopher B., & Gorte, Raymond J. Comparison of HMF hydrodeoxygenation over different metal catalysts in a continuous flow reactor. United States. doi:10.1016/j.apcata.2015.10.009.
Luo, Jing, Arroyo-Ramírez, Lisandra, Wei, Jifeng, Yun, Hongseok, Murray, Christopher B., and Gorte, Raymond J. Thu . "Comparison of HMF hydrodeoxygenation over different metal catalysts in a continuous flow reactor". United States. doi:10.1016/j.apcata.2015.10.009. https://www.osti.gov/servlets/purl/1387337.
@article{osti_1387337,
title = {Comparison of HMF hydrodeoxygenation over different metal catalysts in a continuous flow reactor},
author = {Luo, Jing and Arroyo-Ramírez, Lisandra and Wei, Jifeng and Yun, Hongseok and Murray, Christopher B. and Gorte, Raymond J.},
abstractNote = {The three-phase hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) and hydrogenation of 2,5-dimethylfuran (DMF) were studied over six carbon-supported metal catalysts (Pt, Pd, Ir, Ru, Ni, and Co) using a tubular flow reactor with 1-propanol solvent, at 180 °C and 33 bar. By varying the space time in the reactor, the reaction of HMF is shown to be sequential, with HMF reacting first to furfuryl ethers and other partially hydrogenated products, which then form 2,5-dimethylfuran (DMF). Ring-opened products and 2,5-dimethyltetrahydrofuran (DMTHF) were produced only from reaction of DMF. Rate constants for the pseudo-first-order sequential reactions were obtained for each of the metals. The selectivities for the reaction of DMF varied with the metal catalyst, with Pd forming primarily DMTHF, Ir forming a mixture of DMTHF and open-ring products, and the other metals forming primarily open-ring products. Catalyst stabilities followed the order Pt ~ Ir > Pd > Ni > Co > Ru. Since the stability order correlated with carbon balances in the product (>93% for Pt; <75% for Ru), deactivation appears to be caused by deposition of humins on the catalyst.},
doi = {10.1016/j.apcata.2015.10.009},
journal = {Applied Catalysis. A, General},
issn = {0926-860X},
number = C,
volume = 508,
place = {United States},
year = {2015},
month = {10}
}

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