High-pressure vapor-phase hydrodeoxygenation of lignin-derived oxygenates to hydrocarbons by a PtMo bimetallic catalyst: Product selectivity, reaction pathway, and structural characterization

Journal Article · Thu Dec 01 00:00:00 EST 2016 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2016.10.009· OSTI ID:1338995

Yohe, Sara L. ^[1]; Choudhari, Harshavardhan J. ^[1]; Mehta, Dhairya D. ^[1]; Dietrich, Paul J. ^[1]; Detwiler, Michael D. ^[1]; Akatay, Cem M. ^[1]; Stach, Eric A. ^[2]; Miller, Jeffrey T. ^[1]; Delgass, W. Nicholas ^[1]; Agrawal, Rakesh ^[1]; Ribeiro, Fabio H. ^[1]

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1. Purdue Univ., West Lafayette, IN (United States)
2. Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

High-pressure, vapor-phase, hydrodeoxygenation (HDO) reactions of dihydroeugenol (2-methoxy-4-propylphenol), as well as other phenolic, lignin-derived compounds, were investigated over a bimetallic platinum and molybdenum catalyst supported on multi-walled carbon nanotubes (5%Pt2.5%Mo/MWCNT). Hydrocarbons were obtained in 100% yield from dihydroeugenol, including 98% yield of the hydrocarbon propylcyclohexane. The final hydrocarbon distribution was shown to be a strong function of hydrogen partial pressure. Kinetic analysis showed three main dihydroeugenol reaction pathways: HDO, hydrogenation, and alkylation. The major pathway occurred via Pt catalyzed hydrogenation of the aromatic ring and methoxy group cleavage to form 4-propylcyclohexanol, then Mo catalyzed removal of the hydroxyl group by dehydration to form propylcyclohexene, followed by hydrogenation of propylcyclohexene on either the Pt or Mo to form the propylcyclohexane. Transalkylation by the methoxy group occurred as a minor side reaction. Catalyst characterization techniques including chemisorption, scanning transmission electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy were employed to characterize the catalyst structure. Catalyst components identified were Pt particles, bimetallic PtMo particles, a Mo carbide-like phase, and Mo oxide phases.

• Research Organization: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Energy Frontier Research Centers (EFRC) (United States). Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio). Institute for Atom-efficient Chemical Transformations (IACT)
• Sponsoring Organization: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
• Grant/Contract Number: AC02-06CH11357; AC02-98CH10886; FG36-08GO18087; SC0000997; SC0012704
• OSTI ID: 1338995
• Alternate ID(s): OSTI ID: 1388499; OSTI ID: 1398577
• Journal Information: Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: C Vol. 344; ISSN 0021-9517
• Publisher: Elsevier
• Country of Publication: United States
• Language: ENGLISH

Related Subjects

2-methoxy-4-propylphenol
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
bimetallic catalysts
dihydroeugenol
hydrodeoxygenation (HDO)
lignin
molybdenum
platinum
pyrolysis upgrading