Journal
JOURNAL OF CATALYSIS
Volume 306, Issue -, Pages 58-67Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2013.06.003
Keywords
Dehydroaromatization; Methane; Hydrogen transfer; Oxygenates; Acetic acid; Molybdenum carbide; H-ZSM-5; Dehydrogenation; Deoxygenation; Kinetic coupling
Categories
Funding
- Catalysis Center for Energy Innovation, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001004]
- National Science Foundation Emerging Frontiers in Research and Innovation - Hydrocarbons from Biomass (NSF EFRI HyBi) [0937706]
- DOE Early Career Program [DE-SC0008418]
- Emerging Frontiers & Multidisciplinary Activities
- Directorate For Engineering [0937706] Funding Source: National Science Foundation
- U.S. Department of Energy (DOE) [DE-SC0008418] Funding Source: U.S. Department of Energy (DOE)
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The co-processing of acetic acid with methane (CH3COOH/CH4 = 0.04-0.10) on Mo/ZSM-5 formulations at 950 K and atmospheric pressure in an effort to couple deoxygenation and dehydrogenation reaction sequences results instead in a stratified reactor bed with upstream CH4 reforming with acetic acid and downstream CH4 pyrolysis. X-ray absorption spectroscopy and chemical transient experiments show that molybdenum carbide is formed inside zeolite micropores during CH4 reactions. The introduction of acetic acid oxidizes a fraction of these carbide moieties upstream while producing H-2 and CO mixtures until completely consumed. Forward rates of CH4 pyrolysis are unperturbed in the presence of an acetic acid or hydrogen co-feed after rigorously accounting for the reversibility of pyrolysis rates and the fraction of molybdenum carbide oxidized by CH3COOH implying that all consequences of CH3COOH and H-2 co-feeds can be interpreted in terms of an approach to equilibrium. (C) 2013 Elsevier Inc. All rights reserved.
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