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Status:
Graduated July 7, 2005 (Ph.D.)
Research Area: Biorefining
Hometown: Santa Rosa, CA
Undergraduate Studies: Brigham Young University
Research Summary:
Renewable Hydrogen and Liquid Alkanes from Catalytic Biorefining of
Biomass-derived Carbohydrates
Concerns about global warming, national security and the diminishing supply of fossil fuels are causing our society to search for new renewable sources of transportation fuels. In this respect, we have recently developed two new heterogeneous catalytic processes, operating in the aqueous phase, to convert biomass-derived carbohydrates to H2 and alkanes. Hydrogen can be produced by aqueous-phase reforming (APR) of carbohydrates at low temperatures (423-538 K) in a single reactor over supported metal catalysts. A combination of fundamental and high-throughput studies were undertaken to optimize catalysts and reaction conditions for H production. While Ni-based catalysts produce large amounts of methane from APR of oxygenated hydrocarbons, we have discovered that the addition of Sn to Ni decreases the rate of methane production, while still maintaining high rates of H2 production. A Raney Ni-Sn catalyst was synthesized that exhibited high activity and selectivity for production of H2, with values comparable to Pt based catalysts.
Alkanes ranging from C1 to C6 can be produced by aqueous phase dehydration/hydrogenation (APD/H) of sorbitol (hydrogenated glucose) by a bi-functional pathway. Sorbitol is repeatedly dehydrated by a solid acid(SiO2-Al2O3) or a mineral acid (HCl) catalyst and then hydrogenated on a metal catalyst (Pt or Pd). The biorefining of sugars to alkanes plus CO2 and water is an exothermic process in which the products retain approximately 95 % of the heating value and only 30 % of the mass of the reactant. Larger liquid alkanes ranging from C7-C15, which could be used as a premium, sulfur free diesel fuel, can be produced by APD/H of larger carbohydrate-derived molecules.
-in collaboration with-
Chris Barrett, Juben Chheda, John Shabaker
Publications:
Huber, G. W.; Shabaker, J.W.; Evans, S.T.; and Dumesic, J. A.; “High throughput studies of supported Pt and Pd bimetallic catalysts for Aqueous Phase Reforming of Ethylene Glycol”, (submitted to Applied Catalysis B).
Huber, G. W.; Chheda, J.; Barrett, C. B.; and Dumesic, J. A.; “Production of Liquid Alkanes by Aqueous-Phase Processing of Biomass-Derived Carbohydrates”, Science (accepted 2005).
Gokale, A.; Huber, G.W.; Dumesic, J.A.; and Mavrikakis, M.; “Effect of Sn on the Reactivity of Cu Surfaces”, Journal of Physical Chemistry B, 108, 14062-14073 (2004).
Alcalá, R.; Shabaker, J.W.; Huber, G.W.; Sanchez-Castillo, M.A.; and Dumesic, J.A.; “Experimental and DFT Studies of the Conversion of Ethanol and Acetic Acid on PtSn-based Catalysts”, Journal of Physical Chemistry B (special issue dedicated to M. Boudart), 109, 2074-2085 (2005).
Davda, R.R.; Shabaker, J.W.; Huber, G.W.; and Dumesic, J.A.; “A Review of Catalytic Issues and Process Conditions for Renewable Hydrogen and Alkanes by Aqueous-Phase Reforming of Oxygenated Hydrocarbons over Supported Metal Catalysts”, Applied Catalysis B: Environmental (special issue on H2 Production), 56, 171-186 (2005).
Huber, G.W.; Cortright, R.D.; and Dumesic, J.A.; “Renewable Alkanes by Aqueous-Phase Reforming of Biomass Derived Oxygenates”, Angewandte Chemie International Edition, 43, 1549-1551 (2004).
Shabaker, J.W.; Huber, G.W.; and Dumesic, J.A.; “Aqueous-Phase Reforming of Oxygenated Hydrocarbons Over Sn-Modified Raney Ni Catalysts”, Journal of Catalysis, 222, 180-191 (2004).
Huber, G.W.; Shabaker, J.W.; and Dumesic. J.A.; “Raney Ni-Sn Catalyst for H2 from Biomass-Derived Hydrocarbons”, Science, 300, 2075-2077 (2003).
Davda, R.R.; Alcalá, R.; Shabaker, J.; Huber, G.; Cortright, R.D.; Mavrikakis, M.; and Dumesic, J.A.; “DFT and Experimental Studies of C-C and C-O Bond Cleavage in Ethanol and Ethylene Glycol on Pt Catalysts”, Studies in Surface Science and Catalysis, 45(Science and Technology in Catalysis 2002), 79-84 (2003).
Shabaker, J.W.; Huber, G.W.; Davda, R.R.; Cortright, R.D.; and Dumesic, J.A.; “Aqueous-Phase Reforming of Ethylene Glycol Over Supported Platinum Catalysts”, Catalysis Letters, 88, 1-8 (2003).
Shabaker, J.W.; Davda, R.R.; Huber, G.W.; Cortright, R.D.; and Dumesic, J.A.; “Aqueous-Phase Reforming of Methanol and Ethylene Glycol Over Alumina-Supported Platinum Catalysts”, Journal of Catalysis, 215, 344-352 (2003).
Davda, R.R.; Shabaker, J.W.; Huber, G.W.; Cortright, R.D.; and Dumesic, J.A.; “Aqueous-phase reforming of ethylene glycol on silica-supported metal catalysts”, Applied Catalysis B: Environmental, 43, 13-26 (2003).
Huber, G.W.; Butala, S.J.M.; Lee, M.L.; and Bartholomew, C.H.; “Gd promotion of Co/SiO2 Fischer-Tropsch synthesis catalysts”, Catalysis Letters, 74, 45-48 (2001).
Huber, G.W.; Guymon , C.G.; Conrad, T.L.; Stephenson, B.C.; and Bartholomew, C.H.; “Hydrothermal stability of Co/SiO2 Fischer-Tropsch synthesis catalysts”, Studies in Surface Science and Catalysis, 139(Catalyst Deactivation 2001), 423-430 (2001).
Huber, G.W.; and Bartholomew, C.H.; “Pt promotion of Co/SiO2 Fischer-Tropsch synthesis catalysts”, Studies in Surface Science and Catalysis, 136 (Natural Gas Conversion VI), 283-288 (2001).
