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Assessing and Managing the Risks of Fuel Compounds: Ethanol Case Study

Description: We have implemented a suite of chemical transport and fate models that provide diagnostic information about the behavior of ethanol (denoted EtOH) and other fuel-related chemicals released to the environment. Our principal focus is on the impacts to water resources, as this has been one of the key issues facing the introduction of new fuels and additives. We present analyses comparing the transport and fate of EtOH, methyl tertiary butyl ether (MTBE), and 2,2,4 trimethyl pentane (TMP) for the following cases (1) discharges to stratified lakes, subsurface release in a surficial soil, (3) cross-media transfer from air to ground water, and (4) fate in a regional landscape. These compounds have significantly different properties that directly influence their behavior in the environment. EtOH, for example, has a low Henry's law constant, which means that it preferentially partitions to the water phase instead of air. An advantageous characteristic of EtOH is its rapid biodegradation rate in water; unlike MTBE or TMP, which degrade slowly. As a consequence, EtOH does not pose a significant risk to water resources. Preliminary health-protective limits for EtOH in drinking water suggest that routine releases to the environment will not result in levels that threaten human health.
Date: February 4, 2002
Creator: Layton, D.W. & Rice, D.W.
Partner: UNT Libraries Government Documents Department

Final report on initial samples supplied by LLNL for task 3.3 binder burnout and sintering schedule optimisation

Description: Sixteen of the twenty-one samples have been investigated using the scanning laser dilatometer. This includes all three types of samples with different preparation routes and organic content. Cracks were observed in all samples, even those only heated to 300 C. It was concluded that the cracking was occurring in the early part of the heat treatment before the samples reached 300 C. Increase in the rate of dilation of the samples occurred above 170 C which coincided with the decomposition of the binder/wax additives as determined by differential thermal analysis. A comparison was made with SYNROC C material (Powder Run 143), samples of which had been CIPed and green machined to a similar diameter and thickness as the 089 mm SRTC pucks. These samples contained neither binder nor other organic processing aids and had been kept in the same desiccator as the SRTC samples. The CIPed Synroc C samples sintered to high density with zero cracks. As the cracks made up only a small contribution to the change in diameter of the sample compared to the sintering shrinkage, useful information could still be gained from the runs. The sintering curves showed that there was much greater shrinkage of the Type III samples containing only the 5% PEG binder compared to the Type I which contained polyolefin wax as processing aid. Slight changes in gradient of the sintering curve were observed, however, due to the masking effect of the cracking, full analysis of the sintering kinetics cannot be conducted. Even heating the samples to 300 C at 1.0 or 0.5 C/min could not prevent crack formation. This indicated that heating rate was not the critical parameter causing cracking of the samples. Sectioning of green bodies revealed the inhomogeneous nature of the binder/lubricant distribution in the samples. Increased homogeneity would reduce the ...
Date: January 4, 1999
Creator: Walls, P
Partner: UNT Libraries Government Documents Department

IMPACT OF COMPOSITION AND HEAT TREATMENT ON PORE SIZE IN POROUS WALLED HOLLOW GLASS MICROSPHERES

Description: The Savannah River National Laboratory (SRNL) developed a new geometric form: hollow glass microspheres (HGMs), with unique porous walls. The new geometric form combines the existing technology of HGMs with basic glass science knowledge in the realm of glass-in-glass phase separation. Conceptually, the development of a HGM with porous walls (referred to as a PWHGM) provides a unique system in which various media or filling agents can be incorporated into the PWHGM (via transport through the porous walls) and ultimately has the capacity to serve as a functional delivery system in various industrial applications. Applications of these types of systems could range from hydrogen storage, molecular sieves, drug and bioactive delivery systems, to environmental, chemical and biological indicators, relevant to Energy, Environmental Processing and Homeland Security fields. As a specific example, previous studies at SRNL have introduced materials capable of hydrogen storage (as well as other materials) into the interior of the PWHGMs. The goal of this project was to determine if the microstructure (i.e., pore size and pore size distribution) of a PWHGM could be altered or tailored by varying composition and/or heat treatment (time and/or temperature) conditions. The ability to tailor the microstructure through composition or heat treatments could provide the opportunity to design the PWHGM system to accommodate different additives or fill agents. To meet this objective, HGMs of various alkali borosilicate compositions were fabricated using a flame forming apparatus installed at the Aiken County Technical Laboratory (ACTL). HGMs were treated under various heat treatment conditions to induce and/or enhance glass in glass phase separation. Heat treatment temperatures ranged from 580 C to 620 C, while heat treatment times were either 8 or 24 hours. Of the two primary variables assessed in this study, heat treatment temperature was determined to be most effective in changing the porosity ...
Date: December 4, 2007
Creator: Raszewski, F; Erich Hansen, E; Ray Schumacher, R & David Peeler, D
Partner: UNT Libraries Government Documents Department

Remediation of Uranium in the Hanford Vadose Zone Using Gas-Transported Reactants: Laboratory Scale Experiments in Support of the Deep Vadose Zone Treatability Test Plan for the Hanford Central Plateau

Description: This laboratory-scale investigation is focused on decreasing mobility of uranium in subsurface contaminated sediments in the vadose zone by in situ geochemical manipulation at low water content. This geochemical manipulation of the sediment surface phases included reduction, pH change (acidic and alkaline), and additions of chemicals (phosphate, ferric iron) to form specific precipitates. Reactants were advected into 1-D columns packed with Hanford 200 area U-contaminated sediment as a reactive gas (for CO2, NH3, H2S, SO2), with a 0.1% water content mist (for NaOH, Fe(III), HCl, PO4) and with a 1% water content foam (for PO4). Uranium is present in the sediment in multiple phases that include (in decreasing mobility): aqueous U(VI) complexes, adsorbed U, reduced U(IV) precipitates, rind-carbonates, total carbonates, oxides, silicates, phosphates, and in vanadate minerals. Geochemical changes were evaluated in the ability to change the mixture of surface U phases to less mobile forms, as defined by a series of liquid extractions that dissolve progressively less soluble phases. Although liquid extractions provide some useful information as to the generalized uranium surface phases (and are considered operational definitions of extracted phases), positive identification (by x-ray diffraction, electron microprobe, other techniques) was also used to positively identify U phases and effects of treatment. Some of the changes in U mobility directly involve U phases, whereas other changes result in precipitate coatings on U surface phases. The long-term implication of the U surface phase changes to alter U mass mobility in the vadose zone was then investigated using simulations of 1-D infiltration and downward migration of six U phases to the water table. In terms of the short-term decrease in U mobility (in decreasing order), NH3, NaOH mist, CO2, HCl mist, and Fe(III) mist showed 20% to 35% change in U surface phases. Phosphate addition (mist or foam advected) showed inconsistent ...
Date: January 4, 2010
Creator: Szecsody, James E.; Truex, Michael J.; Zhong, Lirong; Williams, Mark D.; Resch, Charles T. & McKinley, James P.
Partner: UNT Libraries Government Documents Department

Final Report on Initial Samples Supplied by LLNL for Task 3.3 Binder Burnout and Sintering Schedule Optimisation

Description: Sixteen of the twenty-one samples have been investigated using the scanning laser dilatometer. This includes all three types of samples with different preparation routes and organic content. Cracks were observed in all samples, even those only heated to 300 C. It was concluded that the cracking was occurring in the early part of the heat treatment before the samples reached 300 C. Increase in the rate of dilation of the samples occurred above 170 C which coincided with the decomposition of the binder/wax additives as determined by differential thermal analysis. A comparison was made with SYNROC C material (Powder Run 143), samples of which had been CIPed and green machined to a similar diameter and thickness as the 089mm SRTC pucks. These samples contained neither binder nor other organic processing aids and had been kept in the same desiccator as the SRTC samples. The CIPed Synroc C samples sintered to high density with zero cracks. As the cracks made up only a small contribution to the change in diameter of the sample compared to the sintering shrinkage, useful information could still be gained from the runs. The sintering curves showed that there was much greater shrinkage of the Type III samples containing only the 5% PEG binder compared to the Type I which contained polyolefin wax as processing aid. Slight changes in gradient of the sintering curve were observed, however, due to the masking effect of the cracking, full analysis of the sintering kinetics cannot be conducted. Even heating the samples to 300 C at 1.0 or 0.5 C/min could not prevent crack formation. This indicated that heating rate was not the critical parameter causing cracking of the samples. Sectioning of green bodies revealed the inhomogeneous nature of the binder/lubricant distribution in the samples. Increased homogeneity would reduce the amount ...
Date: January 4, 1999
Creator: Walls, P
Partner: UNT Libraries Government Documents Department

The effect of chemical additives on the synthesis of ethanol

Description: The objective of this research is to elucidate the role of various chemical additives on ethanol synthesis over Rh- and Ni-based catalysts. Chemical additives used will include S, P, Ag, Cu, Mn, and Na. The effect of additives on the surface state of the catalysts, heat of adsorption of reactant molecules, reaction intermediates, reaction pathways, reaction kinetics, and product distributions is/will be investigated by a series of studies including temperature programmed desorption, infrared study of NO adsorption, reactive probing, steady state rate measurement, and transient kinetic study. A better understanding of the role of additive may allow us to use chemical additives to manipulate the catalytic properties of Rh- and Ni-based catalysts for producing high yields of ethanol from syngas. CO insertion is known to be a key step to the formation of acetaldehyde and ethanol from CO hydrogenation over Rh catalysts. Ethylene hydroformylation has often served as a probe to determine CO insertion capabilities of Rh catalysts. The mechanism of CO insertion in ethylene hydroformylation over Rh/SiO{sub 2} was investigated.
Date: February 4, 1989
Creator: Chuang, S.S.C.
Partner: UNT Libraries Government Documents Department

The effect of chemical additives on the synthesis of ethanol. Technical progress report 5, September 16, 1988--December 15, 1988

Description: The objective of this research is to elucidate the role of various chemical additives on ethanol synthesis over Rh- and Ni-based catalysts. Chemical additives used will include S, P, Ag, Cu, Mn, and Na. The effect of additives on the surface state of the catalysts, heat of adsorption of reactant molecules, reaction intermediates, reaction pathways, reaction kinetics, and product distributions is/will be investigated by a series of studies including temperature programmed desorption, infrared study of NO adsorption, reactive probing, steady state rate measurement, and transient kinetic study. A better understanding of the role of additive may allow us to use chemical additives to manipulate the catalytic properties of Rh- and Ni-based catalysts for producing high yields of ethanol from syngas. CO insertion is known to be a key step to the formation of acetaldehyde and ethanol from CO hydrogenation over Rh catalysts. Ethylene hydroformylation has often served as a probe to determine CO insertion capabilities of Rh catalysts. The mechanism of CO insertion in ethylene hydroformylation over Rh/SiO{sub 2} was investigated.
Date: February 4, 1989
Creator: Chuang, S. S. C.
Partner: UNT Libraries Government Documents Department