Huber, George

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Dr
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Huber
First Name
George
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Chemical Engineering
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Introduction
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, domestically available biomass has been proposed as part of the solution to our dependence on fossil fuels. While biomass has potential to replace a large fraction of imported petroleum based products, the main obstacle to the more widespread utilization of our low-cost biomass resources is the absence of low-cost processing technologies. The objective of our research is to develop highly efficient and low-cost catalytic processes, catalytic materials and reactors for biomass conversion to fuels and chemicals utilizing aqueous-phase processing. Aqueous-phase technology is advantageous for biomass conversion strategies in that high energy efficiencies are obtained, recyclable-heterogeneous catalysts are used, and biomass-derived molecules, which have a high degree of functionality and low thermal stability, can be processed.
New catalytic materials and processes are developed in our group by using a combination of high-throughput and fundamental studies. High-throughput studies allow the rapid testing of a large number of catalysts, thereby significantly decreasing catalyst development time. We also seek to understand the fundamental chemistry and reaction pathways occurring under reaction conditions. The relationship between the structure of the catalyst and activity/selectivity is investigated using modern in-situ catalytic characterization techniques. New catalytic synthesis techniques, which allow the design of catalyst at the molecular level with controlled adsorption properties, are used to develop highly active catalysts for aqueous-phase processes. We believe it is vital to our nation's energy, economic and environmental future to continue to develop these low-cost strategies for biomass conversion.
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Now showing 1 - 5 of 5
  • Publication
    Chemistry and Kinetics of Furan Conversion into Aromatics and Olefins over ZSM-5: A Model Biomass Conversion Reaction
    Cheng, Yu-Ting; Huber, George W.
    The conversion of furan (a model of cellulosic biomass) over ZSM-5 was studied in a TGA/TPD-MS system, an in-situ FTIR, and in a continuous flow fixed-bed reactor. The furan adsorbs as oligomers at room temperature with a 1.73 of adsorbed furan/Al ratio. These oligomers are converted to CO, CO2, olefins and aromatics at temperatures from 400 – 600 ºC. We have measured the effects of space velocity, temperature, and partial pressure for furan conversion to help us understand the chemistry of biomass conversion inside zeolite catalysts. The selectivity of aromatics and olefins products did not change significantly with space velocity. The apparent reaction order for furan consumption with respect to furan was lower (1.2) than the apparent reaction orders for aromatics (1.7) and olefins formation (1.5). The apparent activation energies of furan consumption (26 kJ/mol) and coke formation (22 kJ/mol) were lower than the apparent activation energies for formation of olefins and aromatics (50-60 kJ/mol). Coke deposition was fast and dramatically deactivated the catalyst in 1 hour. Kinetic data obtained in this study is strongly pore-diffusion controlled and is far from thermodynamic equilibrium. We have proposed some key elementary reactions that may occur for this process.
  • Publication
    Green Gasoline from Aqueous Phase Hydrodeoxygenation of Carbohydrate
    Li, Ning; Tempsett, Geoffrey A; Huber, George W
    Aqueous-phase hydrodeoxygenation (APHDO) is a promising technology to convert biomass-derived oxygenates into alkanes and oxygenates. Selectively breaking the C-O bond without C-C bond cleavage is the biggest challenge and key for this project. In the previous work of Dumesic’s group, it was shown that sorbitol can be converted to gasoline by APHDO over bifunctional catalysts (Pt/SiO2-Al2O3) that contain both metal and acid sites. However, the low octane number, high Reid vapor pressure and low yield of gasoline range compounds produced in such a process limited the real application of this technology. As the first part of this work, we investigated the reaction chemistry for the APHDO of sorbitol over Pt/SiO2-Al2O3 catalyst. From the analysis of gas phase and liquid phase products, more than 40 different compounds were identified. These compounds include dehydrated sorbitol (1,4-sorbitan, isosorbide), polyols, cyclic-ether alcohols, ketones, alkanes and CO2. From the APHDO of sorbitol and a series of model intermediates, it was found that the APHDO is mainly composed of three unit reaction: 1) C-C breaking reactions by decarbonyldration or retro-aldol reactions. 2) C-O bond cleavage (dehydration followed by hydrogenation). 3) Hydrogenation reactions. Then we investigated the effect of reaction conditions (temperature, pressure, and sorbitol concentration) and different acidic support. Base on the experience we got in above work, we achieved up to 70 % gasoline product by APHDO of sorbitol over Pt/Zirconium phosphate catalyst which was proved to be the best among the catalysts we investigated. The octane number and Reid vapor pressure were also improved by the new catalytic process.
  • Publication
    The Intrinsic Kinetics and Heats of Reactions for Cellulose Pyrolysis and Char Formation
    Cho, Joungmo; Lin, Yenhan; Davis, Jeffrey M.; Huber, George W.
    The conversion of biomass into biofuel products by pyrolysis has attracted tremendous interests due to high availability and potential to provide sustainable liquid fuels. Cellulose is the most abundant polymeric carbohydrate compound, which comprise the largest fraction of biomass. During the pyrolysis, cellulose undergoes multiple decomposition pathways depending on the thermal conditions and produces different classes of compounds including non-condensible gases, condensable vapors that are condensed into a liquid mixture, solid chars. In spite of numerous efforts to understand reaction mechanism for cellulose pyrolysis, a reliable reaction model describing both heat release and intrinsic themokinetic behavior is not developed yet due to the lack of means to quantify the heat involvement of individual steps. In the present study, cellulose pyrolysis experiments at isothermal and dynamic conditions are carried out to characterize the evolution of products depending on thermal conditions. Observed decomposition behaviors are compared with an intrinsic kinetic model to estimate the reaction rates and heats of reactions for individual reaction steps.
  • Publication
    Optimizing the Shape Selectivity of Zeolite Catalysts for Biomass Conversion: The Kinetic Diameter
    Jae, Jungho; Tompsett, Geoffrey A; Foster, Andrew J; Auerbach, Scott M; Lobo, Raul F; Huber, George W
    We have studied the influence of catalyst pore size and morphology on the conversion of glucose to aromatics by catalytic fast pyrolysis using over 15 different zeolite catalysts having a variety of shapes and pore sizes. The estimated kinetic diameter for the catalytic pyrolysis products and reactants was used to determine the optimal pore size for zeolite catalysts for catalytic fast pyrolysis. Smaller oxygenate pyrolysis products including furans, hydroxyaldehydes, and organic acids are sufficiently small in diameter to diffuse easily into ZSM-5 (6.3 Å). Of the aromatic products only benzene, toluene, indane, indene, naphthalene, ethylbenzene and xylenes are of a sufficiently small size compared to the ZSM-5 pore. Zeolites type catalysts with a range of pore size 3.9-7.4Å were used for catalytic testing. From these an optimum pore size range of 5.7-6.6Å is identified to maximize aromatic yield. In addition to pore window size, zeolite pore structure and intersections are critical for the reaction mechanism. It is likely that this small pore size also limits the formation of larger aromatics including coke in the pores. Key words: Zeolite, Catalytic Fast Pyrolysis, Kinetic Diameter, Aromatics.
  • Publication
    Production of Green Aromatics and Olefins by Catalytic Fast Pyrolysis of Wood
    Carlson, Torren R; Cheng, Yu-Ting; Jae, Jungho; Cho, Jungmo; Huber, George W
    Catalytic fast pyrolysis (CFP) is a promising process for the direct conversion of solid biomass into gasoline range aromatics. This novel process has significant advantages compared to other technologies for biomass conversion including low capital and operating costs and it makes a product that already fits into existing infrastructure. The CFP of pine wood and furan with ZSM-5 catalyst was studied under different reaction conditions with several different reactors including a fluidized bed reactor, a fixed bed reactor and a semi-batch pyroprobe reactor to optimize CFP for aromatic production. The highest aromatic yield of 14 % carbon was obtained at low space velocity and 600 oC. The aromatic product consists mainly of benzene (24.8 % carbon), toluene (34.1% carbon), xylene (15.4% carbon) and naphthalene (14.9 % carbon). The aromatic yield and selectivity is a function of reactor temperature. However, the olefin yield was not a function of temperature. The selectivity for benzene and naphthalene increases at temperature increases. The more valuable aromatics toluene and xylene are selectively produced at lower temperature. We also studied furan conversion in a fixed bed reactor to help identify the catalytic chemistry. Our results from the fixed bed indicate that furan is a good model compound to study CFP with wood. The maximum aromatic yield (24% carbon) from furan was obtained at 600 °C which is consistent with the fluidized bed results. Olefins can be recycled to the reactor inlet to produce more aromatics. Co-feeding olefins with wood increases both the aromatic yield and conversion of feed. With co-feed the selectivity of small aromatics (such as toluene and benzene) increases while the selectivity for naphthalenes decreases. In this poster presentation we estimate the aromatic yields that could be achieved by CFP when we include olefin recycle.