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High Specific Surface area Aerogel Cryoadsorber for Vacuum Pumping Applications

Description: A cryogenic pumping system is provided, comprising a vacuum environment, an aerogel sorbent formed from a carbon aerogel disposed within the vacuum environment, and cooling means for cooling the aerogel sorbent sufficiently to adsorb molecules from the vacuum environment onto the aerogel sorbent. Embodiments of the invention include a liquid refrigerant cryosorption pump, a compressed helium cryogenic pump, a cryopanel and a Meissner coil, each of which uses carbon aerogel as a sorbent material.
Date: December 22, 1998
Creator: Hill, Randal M.; Fought, Eric R. & Biltoft, Peter J.
Partner: UNT Libraries Government Documents Department

LITERATURE REVIEW OF PUO2 CALCINATION TIME AND TEMPERATURE DATA FOR SPECIFIC SURFACE AREA

Description: The literature has been reviewed in December 2011 for calcination data of plutonium oxide (PuO{sub 2}) from plutonium oxalate Pu(C{sub 2}O{sub 4}){sub 2} precipitation with respect to the PuO{sub 2} specific surface area (SSA). A summary of the literature is presented for what are believed to be the dominant factors influencing SSA, the calcination temperature and time. The PuO{sub 2} from Pu(C{sub 2}O{sub 4}){sub 2} calcination data from this review has been regressed to better understand the influence of calcination temperature and time on SSA. Based on this literature review data set, calcination temperature has a bigger impact on SSA versus time. However, there is still some variance in this data set that may be reflecting differences in the plutonium oxalate preparation or different calcination techniques. It is evident from this review that additional calcination temperature and time data for PuO{sub 2} from Pu(C{sub 2}O{sub 4}){sub 2} needs to be collected and evaluated to better define the relationship. The existing data set has a lot of calcination times that are about 2 hours and therefore may be underestimating the impact of heating time on SSA. SRNL recommends that more calcination temperature and time data for PuO{sub 2} from Pu(C{sub 2}O{sub 4}){sub 2} be collected and this literature review data set be augmented to better refine the relationship between PuO{sub 2} SSA and its calcination parameters.
Date: March 6, 2012
Creator: Daniel, G.
Partner: UNT Libraries Government Documents Department

Gas Generation Testing of Neptunium Oxide Generated Using the HB-Line Phase IIFlowsheet

Description: The hydrogen (H{sub 2}) gas generation rate for neptunium dioxide (NpO{sub 2}) samples produced on a laboratory scale using the HB-Line Phase II flowsheet has been measured following exposure to 75% relative humidity (RH). As expected, the observed H{sub 2} generation rates for these samples increase with increasing moisture content. A maximum H{sub 2} generation rate of 1.8 x 10{sup -6} moles per day per kilogram (mol {center_dot} day{sup -1} kg{sup -1}) was observed for NpO{sub 2} samples with approximately one and one-half times (1 1/2 X) the expected specific surface area (SSA) for the HB-Line Phase II product. The SSA of NpO{sub 2} samples calcined at 650 C is similar to plutonium dioxide (PuO{sub 2}) calcined at 950 C according to the Department of Energy (DOE) standard for packaging and storage of PuO{sub 2}. This low SSA of the HB-Line Phase II product limits moisture uptake to less than 0.2 weight percent (wt %) even with extended exposure to 75% RH.
Date: August 29, 2003
Creator: Duffey, J
Partner: UNT Libraries Government Documents Department

Dynamic response of physisorbed hydrogen molecules on lanthanide-modified zirconia nanoparticles

Description: Ultrafine lanthanide (Ln = Ce and Nd)-modified zirconia powders synthesized by a coprecipitation method exhibit high surface areas and adsorption sites that are essential for catalytic applications. We report a study of the surface chemistry of Ce{sub 0.1}Zr{sub 0.9}O{sub 2} and Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95} powders. First, the specific surface area and porosity are characterized by nitrogen isotherm-adsorption measurements. Second, the motion of hydrogen molecules physisorbed on Ce- and Nd-doped zirconias is studied by inelastic neutron scattering. Nitrogen adsorption-desorption isotherm measurements yield a BET surface area (26.1 m{sup 2}/g) and mesopore size ({approximately}5 nm radius) in Ce{sub 0.1}Zr{sub 0.9}O{sub 2} as compared to those (72.3 m{sup 2}/g and {approximately}3 nm) in Nd{sub 0.1}Zr{sub 0.9} O{sub 1.95}. The vibrational densities of states of H{sub 2} on Ce{sub 0.1}Zr{sub 0.9}O{sub 2} and Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95} were measured at 20 K over the 0-200 meV energy range for three hydrogen coverage. The spectra for both samples consist of two parts: a sharp peak at {approximately}14.5 meV and a broad component extending beyond 200 meV. The sharp peak corresponds to transitions from the J=0 to J=1 rotational states of bulk hydrogen molecules, and its intensity decreases with decreasing H{sub 2} coverage. The broad component corresponds to overdamped motion of surface adsorbed hydrogen molecules. The major difference in the latter component between the Ce- and Nd-doped samples is an excess of intensities in the 5-14 meV region in Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95}. The confined motion of adsorbed H{sub 2} on the different micropore and mesopore surfaces of Ce{sub 0.1}Zr{sub 0.9}O{sub 2} and Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95} is discussed.
Date: October 1, 1997
Creator: Loong, C.K.; Trouw, F.; Ozawa, Masakuni & Suzuki, Suguru
Partner: UNT Libraries Government Documents Department

MOISTURE AND SURFACE AREA MEASUREMENTS OF PLUTONIUM-BEARING OXIDES

Description: To ensure safe storage, plutonium-bearing oxides are stabilized at 950 C for at least two hours in an oxidizing atmosphere. Stabilization conditions are expected to decompose organic impurities, convert metals to oxides, and result in moisture content below 0.5 wt%. During stabilization, the specific surface area is reduced, which minimizes readsorption of water onto the oxide surface. Plutonium oxides stabilized according to these criteria were sampled and analyzed to determine moisture content and surface area. In addition, samples were leached in water to identify water-soluble chloride impurity content. Results of these analyses for seven samples showed that the stabilization process produced low moisture materials (< 0.2 wt %) with low surface area ({le} 1 m{sup 2}/g). For relatively pure materials, the amount of water per unit surface area corresponded to 1.5 to 3.5 molecular layers of water. For materials with chloride content > 360 ppm, the calculated amount of water per unit surface area increased with chloride content, indicating hydration of hygroscopic salts present in the impure PuO{sub 2}-containing materials. The low moisture, low surface area materials in this study did not generate detectable hydrogen during storage of four or more years.
Date: September 28, 2009
Creator: Crowder, M.; Duffey, J.; Livingston, R.; Scogin, J.; Kessinger, G. & Almond, P.
Partner: UNT Libraries Government Documents Department

DEVELOPMENT OF MESOPOROUS MEMBRANE MATERIALS FOR CO2 SEPARATION

Description: Mesoporous and precipitated alumina were synthesized as the base material for CO{sub 2} adsorbent. The porous alumina is doped with Ba to enhance it CO{sub 2} affinity due to the basicity of Ba. it is shown by gas chromatograph (GC) that the addition of Ba enhances the separation CO{sub 2} from N{sub 2}. It was found that mesoporous alumina has larger specific surface area and better selectivity of CO{sub 2} than precipitated alumina. Ba improves the affinity of mesoporous alumina with CO{sub 2}. Phase may play an important role in selective adsorption of CO{sub 2}. It is speculated that mesoporous alumina is more reactive than precipitated alumina creating the xBaO {center_dot} Al{sub 2}O{sub 3} phase that may be more affinity to CO{sub 2} than N{sub 2}. On the other hand, the barium aluminate phase (Ba{sub 3}Al{sub 2}O{sub 6}) in the mesoporous sample does not help the adsorption of CO{sub 2}.
Date: May 1, 2002
Creator: Shih, Wei-Heng; Zhao, Qiang & Wang, Nanlin
Partner: UNT Libraries Government Documents Department

Permanganate Treatment of DNAPLs in Reactive Barriers and Source Zone Flooding Schemes

Description: This research involves a combined experimental modeling study that builds on our previous DOE-sponsored work in understanding how KMnO4 can be used with in situ cleanups of contaminated sites. The specific objectives of this study are (1) to describe how solid forms of KMnO4 behave in saturated media, (2) to undertake flow tank studies that examine the hydraulic impact of reaction products (especially MnO2) on the flux of water through the zone of contamination, and (3) to represent process understanding in flow and transport models. We have made excellent progress in addressing these issues through a variety of different laboratory and theoretical investigations, as well as work that summarizes the state of the science. In the space available for this report, we can only summarize the key findings of the study. Readers interested in additional details can refer to the papers that are listed at end of this report. There has been significant industrial interest in the use of KMnO4 schemes for the in situ destruction of various chlorinated solvents. Given our previous work that emphasized some of the problems associated with field applications of the method, we were invited to contribute to a special edition of Environmental & Engineering Geoscience that examined the effects of heterogeneity on in situ remediation schemes. Our review targeted the most common implementation namely the use of an injection/withdrawal system to circulate oxidants (e.g., potassium permanganate, hydrogen peroxide, and Fenton's Reagent) through a source zone containing a dense nonaqueous phase liquid (DNAPL). The review demonstrated with various examples (1) how the efficiency of chemical oxidation is highly dependent on physical and chemical heterogeneities, and (2) how effective delivery is essential for successful remediation. A summary of this work is provided here in Section 1 of the Chapter Methods and Results. We investigated the mineralogy ...
Date: September 14, 2003
Creator: Schwartz, Franklin W.
Partner: UNT Libraries Government Documents Department

Effect of Precipitation Conditions on the Specific Surface Area of Neptunium Oxide

Description: Neptunium oxalate was precipitated under nominal and bounding HB-Line flowsheet conditions. The nominal case represents expected normal HB-Line operation. The bounding case represents process flowsheet extremes that could occur which are anticipated to decrease particle size and increase surface area. The neptunium oxalate produced under bounding conditions was used to validate the effectiveness of HB-Line calcination conditions. The maximum specific surface area of the neptunium oxide (NpO2) used in gas generation testing was 5.34 m2/g. Experiments were conducted to verify that even under bounding precipitation conditions the SSA of NpO2 produced would remain within the range evaluated during gas generation testing. The neptunium oxalate from nominal and bounding precipitation conditions was calcined at 600 degrees Celsius and 625 degrees Celsius, respectively, to form NpO2. Samples from each batch of neptunium oxalate were calcined for one, two, or four hours. Results indicate that the SSA of NpO2 continues to decrease between one and four hours. After two hours of calcination at 625 degrees Celsius, the SSA of NpO2 from the bounding case meets the surface area requirements for limiting moisture uptake.
Date: June 1, 2004
Creator: HILL, BENJAMINC.
Partner: UNT Libraries Government Documents Department

Kinetics and mechanisms of NOx - char reduction. Quarterly technical progress report, August 1, 1995--October 31, 1995

Description: The emission of nitrogen oxides from combustion of coal remains a problem of considerable interest, whether the concern is with acid rain, stratospheric ozone chemistry, or {open_quotes}greenhouse{close_quotes} gases. Whereas earlier the concern was focused mainly on NO (as a primary combustion product) and to a lesser extent NO{sub 2} (since it is mainly a secondary product of combustion), in recent years the emissions of N{sub 2}O have also captured considerable attention, particularly in the context of fluidized bed combustion, in which the problem appears to be most acute. The research community has only recently begun to take solid hold on the N{sub 2}O problem. This is in part because earlier estimates of the importance of N{sub 2}O in combustion processes were clouded by artifacts in sampling which have now been resolved. This project is concerned with the mechanism of reduction of both NO and N{sub 2}O by carbons. It was recognized some years ago that NO formed during fluidized bed coal combustion can be heterogeneously reduced in-situ by the carbonaceous solid intermediates of combustions. This has been recently supplemented by the knowledge that heterogeneous reaction with carbon can also play an important role in reducing emissions of N{sub 2}O, but that the NO-carbon reactions might also contribute to formation of N{sub 2}O. The precise role of carbon in N{sub 2}O reduction and formation has yet to be established, since in one case the authors of a recent study were compelled to comment that the basic knowledge of N{sub 2}O formation and reduction still has to be improved. The same can be said of the NO-carbon system.
Date: May 1, 1996
Creator: Suuberg, E.M.; Lilly, W.D. & Aarna, I.
Partner: UNT Libraries Government Documents Department

Innovative Fresh Water Production Process for Fossil Fuel Plants

Description: This project concerns a diffusion driven desalination (DDD) process where warm water is evaporated into a low humidity air stream, and the vapor is condensed out to produce distilled water. Although the process has a low fresh water to feed water conversion efficiency, it has been demonstrated that this process can potentially produce low cost distilled water when driven by low grade waste heat. This report summarizes the progress made in the development and analysis of a Diffusion Driven Desalination (DDD) system. Detailed heat and mass transfer analyses required to size and analyze the diffusion tower using a heated water input are described. The analyses agree quite well with the current data and the information available in the literature. The direct contact condenser has also been thoroughly analyzed and the system performance at optimal operating conditions has been considered using a heated water/ambient air input to the diffusion tower. The diffusion tower has also been analyzed using a heated air input. The DDD laboratory facility has successfully been modified to include an air heating section. Experiments have been conducted over a range of parameters for two different cases: heated air/heated water and heated air/ambient water. A theoretical heat and mass transfer model has been examined for both of these cases and agreement between the experimental and theoretical data is good. A parametric study reveals that for every liquid mass flux there is an air mass flux value where the diffusion tower energy consumption is minimal and an air mass flux where the fresh water production flux is maximized. A study was also performed to compare the DDD process with different inlet operating conditions as well as different packing. It is shown that the heated air/heated water case is more capable of greater fresh water production with the same energy consumption ...
Date: September 29, 2006
Creator: Klausner, James F.; Mei, Renwei; Li, Yi & Knight, Jessica
Partner: UNT Libraries Government Documents Department

Scalar properties of transversely isotropic tuff from images of orthogonal cross sections

Description: Image processing methods have been used very effectively to estimate physical properties of isotropic porous earth materials such as sandstones. Anisotropic materials can also be analyzed in order to estimate their physical properties, but additional care and a larger number of well-chosen images of cross sections are required to obtain correct results. Although low-symmetry anisotropic media present difficulties for two-dimensional image processing methods, geologic materials are often transversely isotropic. Scalar properties of porous materials such as porosity and specific surface area can be determined with only minor changes in the analysis when the medium is transversely isotropic rather than isotropic. For example, in a rock that is transitively isotropic due to thin layers or beds, the overall porosity may be obtained by analyzing images of cross sections taken orthogonal to the bedding planes, whereas cross sections lying within the bedding planes will determine only the local porosity of the bed itself. It is known for translationally invariant anisotropic media that the overall specific surface area can be obtained from radial averages of the two-point correlation function in the full three-dimensional volume. Layered materials are not translationally invariant in the direction of the layering, but we show nevertheless how averages of cross sections may be used to obtain the specific surface area for a transversely isotropic rock. We report values of specific surface area obtained for thin sections of Topopah Spring Tuff from Yucca Mountain, Nevada. This formation is being evaluated as a potential host rock for geologic disposal of nuclear waste. Although the present work has made use of thin sections of tuff for the images, the same methods of analysis could also be used to simplify quantitative analysis of three-dimensional volumes of pore structure data obtained by means of x-ray microtomography or other methods, using only a few representative ...
Date: January 1, 1997
Creator: Berge, P.A.; Berryman, J.G.; Blair, S.C. & Pena, C.
Partner: UNT Libraries Government Documents Department

Surface area and chemical reactivity characteristics of uranium metal corrosion products.

Description: The results of an initial characterization of hydride-containing corrosion products from uranium metal Zero Power Physics Reactor (ZPPR) fuel plates are presented. Sorption analyses using the BET method with a Kr adsorbate were performed to measure the specific areas of corrosion product samples. The specific surface areas of the corrosion products varied from 0.66 to 1.01 m{sup 2}/g. The reactivity of the products in Ar-9%O{sub 2} and Ar-20%O{sub 2} were measured at temperatures between 35 C and 150 C using a thermo-gravimetric analyzer. Ignition of the products occurred at temperatures of 150 C and above. The oxidation rates below ignition were comparable to rates observed for uranium metal.
Date: February 17, 1998
Creator: Totemeier, T. C.
Partner: UNT Libraries Government Documents Department

Progress towards a PETN Lifetime Prediction Model

Description: Dinegar (1) showed that decreases in PETN surface area causes EBW detonator function times to increase. Thermal aging causes PETN to agglomerate, shrink, and densify indicating a ''sintering'' process. It has long been a concern that the formation of a gap between the PETN and the bridgewire may lead to EBW detonator failure. These concerns have led us to develop a model to predict the rate of coarsening that occurs with age for thermally driven PETN powder (50% TMD). To understand PETN contributions to detonator aging we need three things: (1) Curves describing function time dependence on specific surface area, density, and gap. (2) A measurement of the critical gap distance for no fire as a function of density and surface area for various wire configurations. (3) A model describing how specific surface area, density and gap change with time and temperature. We've had good success modeling high temperature surface area reduction and function time increase using a phenomenological deceleratory kinetic model based on a distribution of parallel nth-order reactions having evenly spaced activation energies where weighing factors of the reactions follows a Gaussian distribution about the reaction with the mean activation energy (Figure 1). Unfortunately, the mean activation energy derived from this approach is high (typically {approx}75 kcal/mol) so that negligible sintering is predicted for temperatures below 40 C. To make more reliable predictions, we've established a three-part effort to understand PETN mobility. First, we've measured the rates of step movement and pit nucleation as a function of temperature from 30 to 50 C for single crystals. Second, we've measured the evaporation rate from single crystals and powders from 105 to 135 C to obtain an activation energy for evaporation. Third, we've pursued mechanistic kinetic modeling of surface mobility, evaporation, and ripening.
Date: September 11, 2006
Creator: Burnham, A K; Overturf III, G E; Gee, R; Lewis, P; Qiu, R; Phillips, D et al.
Partner: UNT Libraries Government Documents Department

Development of a Catalyst/Sorbent for Methane Reforming

Description: This project led to the further development of a combined catalyst and sorbent for improving the process technology required for converting CH{sub 4} and/or CO into H{sub 2} while simultaneously separating the CO{sub 2} byproduct all in a single step. The new material is in the form of core-in-shell pellets such that each pellet consists of a CaO core surrounded by an alumina-based shell capable of supporting a Ni catalyst. The Ni is capable of catalyzing the reactions of steam with CH{sub 4} or CO to produce H{sub 2} and CO{sub 2}, whereas the CaO is capable of absorbing the CO{sub 2} as it is produced. The absorption of CO{sub 2} eliminates the reaction inhibiting effects of CO{sub 2} and provides a means for recovering the CO{sub 2} in a useful form. The present work showed that the lifecycle performance of the sorbent can be improved either by incorporating a specific amount of MgO in the material or by calcining CaO derived from limestone at 1100 C for an extended period. It also showed how to prepare a strong shell material with a large surface area required for supporting an active Ni catalyst. The method combines graded particles of {alpha}-alumina with noncrystalline alumina having a large specific surface area together with a strength promoting additive followed by controlled calcination. Two different additives produced good results: 3 {micro}m limestone and lanthanum nitrate which were converted to their respective oxides upon calcination. The oxides partially reacted with the alumina to form aluminates which probably accounted for the strength enhancing properties of the additives. The use of lanthanum made it possible to calcine the shell material at a lower temperature, which was less detrimental to the surface area, but still capable of producing a strong shell. Core-in-shell pellets made with the improved shell ...
Date: December 31, 2008
Creator: Shans, B.H.; Wheelock, T.D.; Satrio, Justinus; Albrecht, Karl; Keeley, Tanya Harris Janine; Silva, Ben et al.
Partner: UNT Libraries Government Documents Department

TECHNICAL BASIS FOR DOE STANDARD 3013 EQUIVALENCY SUPPORTING REDUCED TEMPERATURE STABILIZATION OF OXALATE-DERIVED PLUTONIUM OXIDE PRODUCED BY THE HB-LINE FACILITY AT SAVANNAH RIVER SITE

Description: The HB-Line (HBL) facility at the Savannah River Site (SRS) is designed to produce high-purity plutonium dioxide (PuO{sub 2}) which is suitable for future use in production of Mixed Oxide (MOX) fuel. The MOX Fuel Fabrication Facility (MFFF) requires PuO{sub 2} feed to be packaged per the U.S. Department of Energy (DOE) Standard 3013 (DOE-STD-3013) to comply with the facility's safety basis. The stabilization conditions imposed by DOE-STD-3013 for PuO{sub 2} (i.e., 950 C for 2 hours) preclude use of the HBL PuO{sub 2} in direct fuel fabrication and reduce the value of the HBL product as MFFF feedstock. Consequently, HBL initiated a technical evaluation to define acceptable operating conditions for production of high-purity PuO{sub 2} that fulfills the DOE-STD-3013 criteria for safe storage. The purpose of this document is to demonstrate that within the defined operating conditions, the HBL process will be equivalent for meeting the requirements of the DOE-STD-3013 stabilization process for plutonium-bearing materials from the DOE complex. The proposed 3013 equivalency reduces the prescribed stabilization temperature for high-purity PuO{sub 2} from oxalate precipitation processes from 950 C to 640 C and places a limit of 60% on the relative humidity (RH) at the lowest material temperature. The equivalency is limited to material produced using the HBL established flow sheet, for example, nitric acid anion exchange and Pu(IV) direct strike oxalate precipitation with stabilization at a minimum temperature of 640 C for four hours (h). The product purity must meet the MFFF acceptance criteria of 23,600 {micro}g/g Pu (i.e., 2.1 wt %) total impurities and chloride content less than 250 {micro}g/g of Pu. All other stabilization and packaging criteria identified by DOE-STD-3013-2012 or earlier revisions of the standard apply. Based on the evaluation of test data discussed in this document, the expert judgment of the authors supports packaging ...
Date: July 2, 2012
Creator: Duffey, J.; Livingston, R.; Berg, J. & Veirs, D.
Partner: UNT Libraries Government Documents Department

DEVELOPMENT OF MESOPOROUS MEMBRANE MATERIALS FOR CO2 SEPARATION

Description: The huge emissions of carbon dioxide from fossil fuel fired power plants and industrial plants over the last century have resulted in an increase of the atmospheric carbon dioxide concentration. Climatological modeling work has predicted severe climate disruption as a result of the trapping of heat due to CO{sub 2}. As an attempt to address this global warming effect, DOE has initiated the Vision 21 concept for future power plants. We first synthesized mesoporous aluminosilicates that have high surface area and parallel pore channels for membrane support materials. Later we synthesized microporous aluminosilicates as the potential thin membrane materials for selective CO{sub 2} adsorption. The pore size is controlled to be less that 1 nm so that the adsorption of CO{sub 2} on the pore wall will block the passage of N{sub 2}. Mesoporous and precipitated alumina were synthesized as the base material for CO{sub 2} adsorbent. The porous alumina is doped with Ba to enhance its CO{sub 2} affinity due to the basicity of Ba. It is shown by gas chromatograph (GC) that the addition of Ba enhances the separation CO{sub 2} from N{sub 2}. It was found that mesoporous alumina has larger specific surface area and better selectivity of CO{sub 2} than precipitated alumina. Ba improves the affinity of mesoporous alumina with CO{sub 2}. Phase may play an important role in selective adsorption of CO{sub 2}. It is speculated that mesoporous alumina is more reactive than precipitated alumina creating the xBaO {center_dot}Al{sub 2}O{sub 3} phase that may be more affinitive to CO{sub 2} than N{sub 2}. On the other hand, the barium aluminates phase (Ba{sub 3}Al{sub 2}O{sub 6}) in the mesoporous sample does not help the adsorption of CO{sub 2}. Microporous aluminosilicate was chosen as a suitable candidate for CO{sub 2}/N{sub 2} separation because the pore size is ...
Date: March 25, 2003
Creator: Shih, Wei-Heng; Patil, Tejas & Zhao, Qiang
Partner: UNT Libraries Government Documents Department

Closeout of Advanced Boron and Metal Loaded High Porosity Carbons.

Description: The Penn State effort explored the development of new high-surface-area materials for hydrogen storage, materials that could offer enhancement in the hydrogen binding energy through a direct chemical modification of the framework in high specific-surface-area platforms. The team chemically substituted boron into the hexagonal sp2 carbon framework, dispersed metal atoms bound to the boro-carbon structure, and generated the theory of novel nanoscale geometries that can enhance storage through chemical frustration, sheet curvature, electron deficiency, large local fields and mixed hybridization states. New boro-carbon materials were synthesized by high temperature plasma, pyrolysis of boron-carbon precursor molecules, and post-synthesis modification of carbons. Hydrogen uptake has been assessed, and several promising leads have been identified, with the requirement to simultaneously optimize total surface area while maintaining the enhanced hydrogen binding energies already demonstrated.
Date: May 1, 2011
Creator: Eklund, Peter C.; Chung, T. C. Mike; Foley, Henry C. & Crespi, Vincent H.
Partner: UNT Libraries Government Documents Department

Effect of Grinding on the Stucture of Glassy Carbon

Description: An earlier suggestion that various allotropic forms of carbon preexist as micron size crystallites in glassy carbon was investigated. Samples previously heated only to 1000 C and thinned by crushing (grinding) or by ion melting and observed using transmission electron diffraction and microscopy gave single crystal or spotty ring patterns for the former but only diffuse rings for the latter. Wide range X-ray diffraction, small angle X-ray scattering, density and surface area measurements of as received plate and ground material show that grinding flattens the internal pore structure of the material, decreasing the specific surface area by 25 percent and increasing the radius of gyration by about 8 percent, It is concluded that the spot patterns indicating crystalline forms result from strain relief during grinding.
Date: December 1, 1979
Creator: Baker, D. F.; Bragg, R. H. & Rao, A. S.
Partner: UNT Libraries Government Documents Department

Corrosion tests to determine temperature and pH dependencies of the dissolution rates of sodalite, binder glass, and ceramic waste form.

Description: A glass bonded-sodalite ceramic waste form (CWF) has been developed to immobilize salt wastes from electrometallurgical treatment of sodium-bonded spent nuclear fuel. The CWF is a composite of salt-loaded sodalite and a binder glass formed at high temperature (850-950 C) by hot isostatic pressing (HIP) or pressureless-consolidation (PC) processes. A waste form degradation and radionuclide release model has been developed to support qualification of the CWF for disposal in the proposed repository at Yucca Mountain. Six series of tests were conducted in conjunction with the development of that model. (1) Static tests were conducted to measure the dissolution rate of sodalite, HIP binder glass, and HIP CWF at 40, 70, and 90 C in pH range 4.8-9.8 buffer solution. The parameter values in the degradation model were calculated from the dissolution rates measured by the static tests. (2) Static tests were conducted at 70 C in noncomplexing tertiary amine pH buffers to confirm that the dissolution rate measured with traditional buffers was not affected by the complexation of metal ions. The results showed that the difference between dissolution rate determined with noncomplexing buffer and that determined with traditional buffers was negligible. (3) Static tests were conducted in five buffer solutions in the pH range 4.8-9.8 at 20 C with HIP sodalite, HIP glass, and HIP CWF. The results showed that the model adequately predicts the dissolution rate of these materials at 20 C. (4) Static tests at 20 and 70 C with CWF made by the PC process indicated that the model parameters extracted from the results of tests with HIP CWF could be applied to PC CWF. (5) The dissolution rates of a modified glass made with a composition corresponding to 80 wt% glass and 20 wt% sodalite were measured at 70 C to evaluate the sensitivity of the ...
Date: February 12, 2003
Creator: Jeong, S.-Y.; Fanning, T. H.; Morss, L. R. & Ebert, W. L.
Partner: UNT Libraries Government Documents Department

Induced Polarization with Electromagnetic Coupling: 3D Spectral Imaging Theory, EMSP Project No. 73836

Description: This project was designed as a broad foundational study of spectral induced polarization (SIP) for characterization of contaminated sites. It encompassed laboratory studies of the effects of chemistry on induced polarization, development of 3D forward modeling and inversion codes, and investigations of inductive and capacitive coupling problems. In the laboratory part of the project a physico-chemical model developed in this project was used to invert laboratory IP spectra for the grain size and the effective grain size distribution of the sedimentary rocks as well as the formation factor, porosity, specific surface area, and the apparent fractal dimension. Furthermore, it was established that the IP response changed with the solution chemistry, the concentration of a given solution chemistry, valence of the constituent ions, and ionic radius. In the field part of the project, a 3D complex forward and inverse model was developed. It was used to process data acquired at two frequencies (1/16 Hz and 1/ 4Hz) in a cross-borehole configuration at the A-14 outfall area of the Savannah River Site (SRS) during March 2003 and June 2004. The chosen SRS site was contaminated with Tetrachloroethylene (TCE) and Trichloroethylene (PCE) that were disposed in this area for several decades till the 1980s. The imaginary conductivity produced from the inverted 2003 data correlated very well with the log10 (PCE) concentration derived from point sampling at 1 ft spacing in five ground-truth boreholes drilled after the data acquisition. The equivalent result for the 2004 data revealed that there were significant contaminant movements during the period March 2003 and June 2004, probably related to ground-truth activities and nearby remediation activities. Therefore SIP was successfully used to develop conceptual models of volume distributions of PCE/TCE contamination. In addition, the project developed non-polarizing electrodes that can be deployed in boreholes for years. A total of 28 ...
Date: December 14, 2004
Creator: Morgan, F. Dale & Sogade, John
Partner: UNT Libraries Government Documents Department

DEVELOPMENT OF A KINETIC MODEL OF BOEHMITE DISSOLUTION IN CAUSTIC SOLUTIONS APPLIED TO OPTIMIZE HANFORD WASTE PROCESSING

Description: Boehmite (e.g., aluminum oxyhydroxide) is a major non-radioactive component in Hanford and Savannah River nuclear tank waste sludge. Boehmite dissolution from sludge using caustic at elevated temperatures is being planned at Hanford to minimize the mass of material disposed of as high-level waste (HLW) during operation of the Waste Treatment Plant (WTP). To more thoroughly understand the chemistry of this dissolution process, we have developed an empirical kinetic model for aluminate production due to boehmite dissolution. Application of this model to Hanford tank wastes would allow predictability and optimization of the caustic leaching of aluminum solids, potentially yielding significant improvements to overall processing time, disposal cost, and schedule. This report presents an empirical kinetic model that can be used to estimate the aluminate production from the leaching of boehmite in Hanford waste as a function of the following parameters: (1) hydroxide concentration; (2) temperature; (3) specific surface area of boehmite; (4) initial soluble aluminate plus gibbsite present in waste; (5) concentration of boehmite in the waste; and (6) (pre-fit) Arrhenius kinetic parameters. The model was fit to laboratory, non-radioactive (e.g. 'simulant boehmite') leaching results, providing best-fit values of the Arrhenius A-factor, A, and apparent activation energy, E{sub A}, of A = 5.0 x 10{sup 12} hour{sup -1} and E{sub A} = 90 kJ/mole. These parameters were then used to predict boehmite leaching behavior observed in previously reported actual waste leaching studies. Acceptable aluminate versus leaching time profiles were predicted for waste leaching data from both Hanford and Savannah River site studies.
Date: January 6, 2011
Creator: RS, DISSELKAMP
Partner: UNT Libraries Government Documents Department

Optimizing the Binding Energy of Hydrogen on Nanostructured Carbon Materials through Structure Control and Chemical Doping

Description: The DOE Hydrogen Sorption Center of Excellence (HSCoE) was formed in 2005 to develop materials for hydrogen storage systems to be used in light-duty vehicles. The HSCoE and two related centers of excellence were created as follow-on activities to the DOE Office of Energy Efficiency and Renewable Energy’s (EERE’s) Hydrogen Storage Grand Challenge Solicitation issued in FY 2003. The Hydrogen Sorption Center of Excellence (HSCoE) focuses on developing high-capacity sorbents with the goal to operate at temperatures and pressures approaching ambient and be efficiently and quickly charged in the tank with minimal energy requirements and penalties to the hydrogen fuel infrastructure. The work was directed at overcoming barriers to achieving DOE system goals and identifying pathways to meet the hydrogen storage system targets. To ensure that the development activities were performed as efficiently as possible, the HSCoE formed complementary, focused development clusters based on the following four sorption-based hydrogen storage mechanisms: 1. Physisorption on high specific surface area and nominally single element materials 2. Enhanced H2 binding in Substituted/heterogeneous materials 3. Strong and/or multiple H2 binding from coordinated but electronically unsatruated metal centers 4. Weak Chemisorption/Spillover. As a member of the team, our group at Duke studied the synthesis of various carbon-based materials, including carbon nanotubes and microporous carbon materials with controlled porosity. We worked closely with other team members to study the effect of pore size on the binding energy of hydrogen to the carbon –based materials. Our initial project focus was on the synthesis and purification of small diameter, single-walled carbon nanotubes (SWNTs) with well-controlled diameters for the study of their hydrogen storage properties as a function of diameters. We developed a chemical vapor deposition method that synthesized gram quantities of carbon nanotubes with average diameter size at less than 1 nm. However, initial tests performed at our ...
Date: February 1, 2011
Creator: Liu, Jie
Partner: UNT Libraries Government Documents Department

Superior catalysts for selective catalytic reduction of nitric oxide. Quarterly technical progress report, January 1, 1995--March 31, 1995

Description: During this quarter, progress was made on the following tasks: TPD techniques were employed to study the reaction mechanism of the selective catalytic reduction of nitrogen oxide with ammonia over iron oxide pillared clay catalyst; and a sulfur dioxide resistant iron oxide/titanium oxide catalyst was developed.
Date: December 1, 1995
Creator: Li, W.B. & Yang, R.T.
Partner: UNT Libraries Government Documents Department

Sorption and chemical transformation of PAHs on coal fly ash. Final technical report

Description: The objectives of this work were to characterize the interactions of coal fly ash with polycyclic aromatic hydrocarbons (PAH`s) and their derivatives, and to attempt to understand the influence of surface properties of coal ash in the chemical transformations of PAH`s.
Date: February 1, 1995
Creator: Mamantov, G. & Wehry, E.L.
Partner: UNT Libraries Government Documents Department