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The Influence of Calcium Carbonate Grain Coatings on Contaminant Reactivity in Vadose Zone Sediments

Description: The primary objective of this project is to investigate the role of calcium carbonate grain coatings on adsorption and heterogeneous reduction reactions of key chemical and radioactive contaminants in sediments on the Hanford Site. Research will ascertain whether these coatings promote or discourage contaminant reaction with sediment mineral particles, and whether calcium carbonate phases resulting from waste-sediment reaction sequester contaminants through coprecipitation. The research will provide new conceptual models of contaminant reaction/retardation processes in Hanford sediments (for 90Sr2+ and Cr(VI)O4 2- primarily) and improved geochemical models to forecast the future behavior of in-ground contaminants.
Date: June 1, 2002
Creator: Zachar, John M.; Chambers, Scott; Brown Jr, Gordon E. & Eggleston, Carrick M.
Partner: UNT Libraries Government Documents Department

Calcium Carbonate Storage in Amorphous Form and Its Template-Induced Crystallization

Description: Calcium carbonate crystallization in organisms often occurs through the transformation from the amorphous precursor. It is believed that the amorphous phase could be temporarily stabilized and stored, until its templated transition to the crystalline form is induced. Here we develop a bio-inspired crystallization strategy that is based on the above mechanism. Amorphous calcium carbonate (ACC) spherulitic particles are formed and stabilized on a self-assembled monolayer (SAM) of hydroxy-terminated alkanethiols on Au surface. The ACC is stored as a reservoir for ions and is induced to crystallize on command by introducing a secondary surface that is functionalized with carboxylic acid-terminated SAM. This secondary surface acts as a template for oriented and patterned nucleation. Various oriented crystalline arrays and micropatterned films are formed. We also show that the ACC phase can be doped with foreign ions (e.g. Mg) and organic molecules (e.g. dyes) and that these dopants later function as growth modifiers of calcite crystals and become incorporated into the crystals during the transformation process of ACC to calcite. We believe that our strategy opens the way of using a stabilized amorphous phase as a versatile reservoir system that can be converted in a highly controlled fashion to a crystalline form upon contacting the nucleating template.
Date: August 31, 2007
Creator: Han, T Y & Aizenberg, J
Partner: UNT Libraries Government Documents Department

New Acid Stimulation Treatment to Sustain Production - Los Angeles Downtown Oil Field

Description: Hydrochloric acid stimulation was successfully used on several wells in the Los Angeles Downtown Field, in the past. The decline rates after stimulation were relatively high and generally within six months to a year, production rates have returned to their prestimulation rates. The wells in Los Angeles Downtown Field have strong scale producing tendencies and many wells are treated for scale control. Four wells were carefully selected that are representative of wells that had a tendency to form calcium carbonate scale and had shown substantial decline over the last few years.
Date: March 10, 2003
Creator: Russell, Richard C.
Partner: UNT Libraries Government Documents Department

Calorimetric Studies of the Energetics of Order-Disorder in the System Mg(1-x)Fe(x)Ca(CO(3))(2)

Description: Calorimetric studies by Chai and Navrotsky (1996) on dolomite-ankerite energetic have been extended by including two additional types of samples: a very disordered stoichiometric MgCa(CO{sub 3}){sub 2} prepared from low temperature aqueous solution and three largely ordered natural samples of intermediate iron content. Combining these data with previous work, three distinct trends of energetic can be seen: those for samples with nearly complete order, nearly complete disorder, and intermediate order. From these trends, the enthalpy of complete disordering is estimated to be 33 {+-} 6 kJ/mol for MgCa(CO{sub 3}){sub 2} and 18 {+-} 5 kJ/mol for FeCa(CO{sub 3}){sub 2}.
Date: February 10, 1999
Creator: Brady, P.; Dooley, D.; Navrotsky, A. & Reeder, R.
Partner: UNT Libraries Government Documents Department

Test of a chemical dispersant for the control of scale formation at treatment facility D

Description: At the Lawrence Livermore National Laboratory (LLNL), ground water is being treated to remove contaminants such as volatile organic compounds and chromium by several types of processes. At Treatment Facility D, remediation of volatile organics is accomplished by sparging the water with air, and the chromium is removed by an ion- exchange process. The air stripping has the effect of raising the pH of the water from -7 to -8, probably as result of removing carbon dioxide from the water. In the absence of further water treatment, calcium carbonate (CaCO{sub 3}), or calcite, deposits on the downstream equipment as a scale, which causes operational problems. At present, this scale deposition is being controlled by the addition of a polyphosphate formulation (JP-7, Jaeger Products, Inc, Houston, TX), but the use of this chemical is not completely satisfactory because of stringent phosphate discharge limits for the treated water A more benign method of scale control would be highly desirable. Therefore, we evaluated an organic chemical dispersant as a possible alternative.
Date: May 1, 1998
Creator: Krauter, P., LLNL
Partner: UNT Libraries Government Documents Department

U1h Superstructure

Description: The U1H Shaft Project is a design build subcontract to supply the U. S. Department of Energy (DOE) a 1,045 ft. deep, 20 ft. diameter, concrete lined shaft for unspecified purposes. The subcontract awarded to Atkinson Construction by Bechtel Nevada to design and construct the shaft for the DOE has been split into phases with portions of the work being released as dictated by available funding. The first portion released included the design for the shaft, permanent hoist, headframe, and collar arrangement. The second release consisted of constructing the shaft collar to a depth of 110 ft., the service entry, utility trenches, and installation of the temporary sinking plant. The temporary sinking plant included the installation of the sinking headframe, the sinking hoist, two deck winches, the shaft form, the sinking work deck, and temporary utilities required to sink the shaft. Both the design and collar construction were completed on schedule. The third release consisted of excavating and lining the shaft to the station depth of approximately 950 feet. Work is currently proceeding on this production sinking phase. At a depth of approximately 600 feet, Atkinson has surpassed production expectation and is more than 3 months ahead of schedule. Atkinson has employed the use of a Bobcat 331 excavator as the primary means of excavation. the shaft is being excavated entirely in an alluvial deposit with varying degrees of calcium carbonate cementation. Several more work packages are expected to be released in the near future. The remaining work packages include, construction of the shaft station a depth of 975 ft. and construction of the shaft sump to a depth of 1,045 ft., installation of the loading pocket and station steel and equipment, installation of the shaft steel and guides, installation of the shaft utilities, and installation of the permanent headframe, ...
Date: November 2000
Creator: Sykes, Glen
Partner: UNT Libraries Government Documents Department

Effect of CO{sub 2} air mixtures on the pH of air-stripped water at Treatment Facility D

Description: A small-scale model of the air stripping tanks at TFD was constructed and tested to determine the effect of carbon dioxide additions, to the stripper air, on system water pH. The objective was to determine whether this technique could be used to control and minimize CaCO{sub 3} scale formation. It was found that a concentration of 0.7 vol. % CO{sub 2} is required to maintain the water at its original, influent pH value of 7.4, but lower concentrations may be effective in controlling scale. There is also a possibility of reducing CO{sub 2} consumption by recycling the CO{sub 2}-rich air. The use of CO{sub 2} injection at Site 300 water treatment is reviewed.
Date: January 1, 1998
Creator: Krauter, P.W.; Harrar, J.E. & Orloff, S.P.
Partner: UNT Libraries Government Documents Department

Solvent mediated self-assembly of solids

Description: Solvent-mediated crystallization represents a robust approach to self-assembly of nanostructures and microstructures. In organic systems, the relative ease with which the structure of hydrogen- bonded molecules can be manipulated allows for generation of a wide variety of nanoscale crystal structures. In living organisms, control over the micron-to-millimeter form of inorganic crystals is achieved through introduction of bio-organic molecules. The purpose of this proposal is to understand the interplay between solution chemistry, molecular structure, surface chemistry, and the processes of nucleation and crystal growth in solvent-mediated systems, with the goal of developing the atomic and molecular basis of a solvent-mediated self-assembly technology. We will achieve this purpose by: (1) utilizing an atomic force microscopy (AFM) approach that provides in situ, real time imaging during growth from solutions, (2) by modifying kinetic Monte Carlo (KMC) models to include solution-surface kinetics, (3) by introducing quantum chemistry (QC) calculations of the potentials of the relevant chemical species and the near-surface structure of the solution, and (4) by utilizing molecular dynamics (MD) simulations to identify the minimum energy pathways to the solid state. Our work will focus on two systems chosen to address both the manometer and micron-to-millimeter length scales of assembly, the family of 2,5- diketopiperazines (X-DKPs) and the system of CaCO{sub 3} with amino acids. Using AFM, we will record the evolution of surface morphology, critical lengths, step speeds, and step-step interactions as a function of supersaturation and temperature. In the case of the X-DKPs, these measurements will be repeated as the molecular structure of the growth unit is varied. In the case of CaCO{sub 3}, they will be performed as a function of solution chemistry including pH, ionic strength, and amino acid content. In addition, we will measure nucleation rates and orientations of CaCO{sub 3} on polyamino acid templates. From these measurements, ...
Date: December 12, 1997
Creator: De Yoreo, J.; Wilson, W.D. & Palmore, T.
Partner: UNT Libraries Government Documents Department

''The Influence of Calcium Carbonate Grain Coatings on Contaminant Reactivity in Vadose Zone Sediments''

Description: Our component of this project focuses on the reaction of contaminant-containing fluids with carbonate mineral surfaces in order to better understand the dissolution-growth and related solid-solution processes that ultimately affect contaminant mobility in settings containing carbonates or carbonate grain coatings. Our collaborators (Stanford, PNNL) have focused on other aspects of carbonate and carbonate mineral surfaces as part of the overall project. Because some of the sediments through which contaminants leaking from the Hanford waste have carbonate grain coatings; better understanding the chemistry of carbonate-contaminant interaction constitutes fundamental chemistry needed in order to construct better models of contaminant transport through carbonate-containing sediments.
Date: June 11, 2003
Creator: Eggleston, Carrick M.
Partner: UNT Libraries Government Documents Department

The Influence of Calcium Carbonate Grain Coatings on Contaminant Reactivity in Vadose Zone Sediments

Description: Calcium carbonate (CaCO3) is widely distributed through the Hanford vadose zone as a minor phase. As a result of current and past geochemical processes, CaCO3 exists as grain coatings, intergrain fill, and distinct caliche layers in select locations. Calcium carbonate may also precipitate when high-level wastes react with naturally Ca- and Mg-saturated Hanford sediments. Calcium carbonate is a very reactive mineral phase. Sorption reactions on its surface may slow the migration of certain contaminants (Co, Sr), but its surface coatings on other mineral phases may diminish contaminant retardation (for example, Cr) by blocking surface reaction sites of the substrate. This project explores the behavior of calcium carbonate grain coatings, including how they form and dissolve, their reactivity toward key Hanford contaminants, their impact (as surface coatings) on the reactivity of other mineral substrates, and on their in-ground composition and minor element enrichment. The importance of CaCO3 as a contaminant sorbent will be defined in all of its different manifestations in Hanford sediments: dispersed minor lithic fragments, pedogenic carbonate coatings on gravel and stringers in silt, and nodules in clay and paleosols. Mass action models will be developed that allow understanding and prediction of the geochemical effects of CaCO3 on contaminant retardation in Hanford sediments.
Date: June 1, 2001
Creator: Zachara, John M.; Chambers, Scott; Brown Jr., Gordon E. & Eggleston, Carrick M.
Partner: UNT Libraries Government Documents Department

Direct Measurement of CO2 Fluxes in Marine Whitings

Description: Clean, affordable energy is a requisite for the United States in the 21st Century Scientists continue to debate over whether increases in CO{sub 2} emissions to the atmosphere from anthropogenic sources, including electricity generation, transportation and building systems may be altering the Earth's climate. While global climate change continues to be debated, it is likely that significant cuts in net CO{sub 2} emissions will be mandated over the next 50-100 years. To this end, a number of viable means of CO{sub 2} sequestration need to be identified and implemented. One potential mechanism for CO{sub 2} sequestration is the use of naturally-occurring biological processes. Biosequestration of CO{sub 2} remains one of the most poorly understood processes, yet environmentally safe means for trapping and storing CO{sub 2}. Our investigation focused on the biogeochemical cycling of carbon in microbial precipitations of CaCO{sub 3}. Specifically, we investigated modern whitings (microbially-induced precipitates of the stable mineral calcium carbonate) as a potential, natural mechanism for CO{sub 2} abatement. This process is driven by photosynthetic metabolism of cyanobacteria and microalgae. We analyzed net air: sea CO{sub 2} fluxes, net calcification and photosynthetic rates in whitings. Both field and laboratory investigations have demonstrated that atmospheric CO{sub 2}decreases during the process of microbial calcification.
Date: July 5, 2001
Creator: Robbins, Lisa L. & Yates, Kimberly K.
Partner: UNT Libraries Government Documents Department

A Novel Treatment for Acid Mine Drainage Utilizing Reclaimed Limestone Residual

Description: The viability of utilizing Reclaimed Limestone Residual (RLR) to remediate Acid Mine Drainage (AMD) was investigated. Physical and chemical characterization of RLR showed that it is composed of various minerals that contain significant quantities of limestone or calcium bearing compounds that can be exploited for acid neutralization. Acid Neutralization Potential (ANP) test results showed that RLR has a neutralization potential of approximately 83% as calcium carbonate (CaCO{sub 3}). Neutralization tests with most of the heavy metals associated with AMD showed removal efficiencies of over 99%. An unexpected benefit of utilizing RLR was the removal of hexavalent chromium Cr (VI) from the aqueous phase. Due to an elevation in pH by RLR most AMD heavy metals are removed from solution by precipitation as their metal hydroxides. Cr (VI) however is not removed by pH elevation and therefore subsequent ongoing tests to elucidate the mechanism responsible for this reaction were conducted.
Date: August 31, 2004
Creator: Moo-Young, Horace K. & Ochola, Charles E.
Partner: UNT Libraries Government Documents Department

Mechanism of Calcite Co-Orientation in the Sea Urchin Tooth

Description: Sea urchin teeth are remarkable and complex calcite structures, continuously growing at the forming end and self-sharpening at the mature grinding tip. The calcite (CaCO{sub 3}) crystals of tooth components, plates, fibers, and a high-Mg polycrystalline matrix, have highly co-oriented crystallographic axes. This ability to co-orient calcite in a mineralized structure is shared by all echinoderms. However, the physico-chemical mechanism by which calcite crystals become co-oriented in echinoderms remains enigmatic. Here, we show differences in calcite c-axis orientations in the tooth of the purple sea urchin (Strongylocentrotus purpuratus), using high-resolution X-ray photoelectron emission spectromicroscopy (X-PEEM) and microbeam X-ray diffraction ({mu}XRD). All plates share one crystal orientation, propagated through pillar bridges, while fibers and polycrystalline matrix share another orientation. Furthermore, in the forming end of the tooth, we observe that CaCO{sub 3} is present as amorphous calcium carbonate (ACC). We demonstrate that co-orientation of the nanoparticles in the polycrystalline matrix occurs via solid-state secondary nucleation, propagating out from the previously formed fibers and plates, into the amorphous precursor nanoparticles. Because amorphous precursors were observed in diverse biominerals, solid-state secondary nucleation is likely to be a general mechanism for the co-orientation of biomineral components in organisms from different phyla.
Date: December 1, 2009
Creator: Killian, Christopher; Metzler, Rebecca; Gong, Y. U. T.; Olson, Ian; Aizenberg, Joanna; Politi, Yael et al.
Partner: UNT Libraries Government Documents Department

Corrosion resistance of inconel 690 to sodium carbonate, calcium carbonate, and sodium meta silicate at 900 and 1100{degrees}C

Description: Corrosive attack of Inconel 690 coupons was not observed following 3 day exposure tests to calcium carbonate, sodium carbonate, and sodium meta silicate at 900 {degrees}C. However, melt line attack was evident on coupons exposed to sodium meta silicate and sodium carbonate tested for 3 days at 1100 {degrees}C. In addition, intergranular attack (IGA), approximately 0.67 mils/day, was observed on the Inconel 690 coupon exposed to calcium carbonate at 1100 {degrees}C. Calcium carbonate did not completely remove the glass coating at 950 {degrees}C. In fact, it was comparable to the results obtained by exposing a glass coated coupon at 950 {degrees}C in air. Therefore, calcium carbonate is not recommended for cleaning the DWPF melter pour spout. Both sodium carbonate and sodium meta silicate appear to remove most of the glass. However, these cleaning agents will remain on the metal surface following exposure at 950 {degrees}C resulting in very rough surface and a potential for corrosive attack when heated to 1100 {degrees}C.
Date: January 29, 1997
Creator: Imrich, K. J.
Partner: UNT Libraries Government Documents Department

REMOVAL OF H2S AND SO2 BY CaCO3-BASED SORBENTS AT HIGH PRESSURES

Description: The mechanism of the removal of SO{sub 2} and H{sub 2}S by CaCO{sub 3}-based sorbents in pressurized fluidized-bed coal combustors (PFBC) and high pressure gasifiers was investigated in this project. Reactivity evolution experiments were carried out in thermogravimetric apparatuses both under simulated high pressure conditions and at high pressures. Experiments at high pressure were conducted in a high pressure thermogravimetric arrangement that was set up and developed under this project. Two calcitic solids of high calcium carbonate content (over 97%) were employed in the experiments: a fine-grained distributed by Greer Limestone Co. (Greer Limestone) and a solid supplied in the form of large calcitic crystals (Iceland Spar). The decision to work with these solids was mainly based on the fact that they have been employed in several past studies of sulfation, sulfidation, and calcination in our laboratory, and therefore, a large volume of data on their performance under different conditions was available for comparison purposes. In addition to the experimental studies, work was also done on the development of rigorous mathematical models for the description of the occurrence of simultaneous processes (e.g., calcination and sulfation and carbonation and sulfation) in the interior of porous solids and for the simulation of the evolution of the pore structure of porous solids that undergo chemical transformation in their interior.
Date: September 1, 2000
Creator: Sotirchos, Prof. Stratis V.
Partner: UNT Libraries Government Documents Department

Preferential recycling/rejection in CFBC/FBC systems using triboelectrostatic separation

Description: Circulating Fluidized Bed Combustion (CFBC) and Fluidized Bed Combustion (FBC) with recirculation are widely used technologies in the US for power generation. They have the advantage of fuel flexibility, and low NO{sub x} and SO{sub x} emissions. Typically, as partially combusted fuel is circulated in the system, only a split stream of this circulating stream is rejected, with remainder recycled to the combustor. As a consequence, there is unburned carbon and partially used, valuable, calcium hydroxide in the reject stream. If these useful materials in the reject stream can be recovered and sent back to the combustor, the efficiency of the system will be increased significantly and the equivalent emissions will be lower. This project studies an innovative concept to incorporate triboelectric separation into CFBC/FBC systems in order to preferentially split its recycle/reject streams based on material compositions of the particles. The objective is to answer whether useful constituents, like carbon, calcium carbonate and calcium hydroxide or oxide, can be selectively separated from combustion ash at elevated temperatures. Laboratory experimental studies are performed at temperatures from 25 C to 210 C, the data from which are presented in the form of recovery curves. These curves present quality-versus-quantity information useful for predicting the efficacy of triboelectric separation as applied to CFBC/FBC byproduct recycling and/or rejection.
Date: May 25, 2000
Creator: Ban, Heng & Stencel, J.M.
Partner: UNT Libraries Government Documents Department

DEVELOPMENT OF A CALCIUM-BASED SORBENT FOR HOT GAS CLEANUP

Description: The development and testing of potential calcium-based sorbents for hot gas cleanup continued. One of the most promising materials combines powdered limestone and a calcium aluminate cement by two step pelletization followed by steam curing. Reasonably strong pellets are produced with good adsorption characteristics by incorporating 20 wt.% cement in the core and 40 wt.% cement in the shell. The resulting 4.76 mm diameter pellets are capable of withstanding a crushing force approaching 11.5 N/mm before breaking and are also capable of removing H{sub 2}S from dilute, hot gas streams. The pellets are also regenerable and reusable. Another promising material combines calcium carbonate powder and finely ground calcined alumina in tablet form. The small tablets are prepared by mixing the materials with water to form a thick paste which is then molded and dried. The tablets are hardened by calcining at either 1000 to 1100 C. The resulting tablets are strong and capable of removing H{sub 2}S from a dilute, hot gas stream.
Date: October 1, 1999
Creator: Wheelock, T.D.; Doraiswamy, L.K. & Constant, K.
Partner: UNT Libraries Government Documents Department

DEVELOPMENT OF A CALCIUM-BASED SORBENT FOR HOT GAS CLEANUP

Description: The preparation and testing of potential sorbents for removing H{sub 2}S and COS from hot coal gas continued. Two preparation methods received the most consideration. Both methods involve pelletizing powders in a revolving drum under moist conditions followed either by heat treatment or steam curing to harden the pellets, depending on the particle bonding mechanism. One method was used to pelletize mixtures of calcium carbonate and either alumina or a calcium aluminate cement in a single step. Another method was used to pelletize powdered limestone in an initial step followed by the application of a coating consisting of both limestone and a hydraulic cement in a second step. By employing this method, an especially promising material was produced consisting of a limestone core surrounded by a shell consisting initially of 80 wt.% limestone and 20% wt.% calcium aluminate cement. The best material exhibited both an acceptable crushing strength and adsorption capacity for H{sub 2}S.
Date: March 31, 1999
Creator: Wheelock, T.D.; Doraiswamy, L.K. & Constant, K.
Partner: UNT Libraries Government Documents Department

Preferential recycling/rejection in CFBC/FBC systems using triboelectrostatic separation

Description: Circulating Fluidized Bed Combustion (CFBC) and Fluidized Bed Combustion (FBC) with recirculation are widely used technologies in the US for power generation. They have the advantage of fuel flexibility, and low NO{sub x} and SO{sub x} emissions. Typically, as partially combusted fuel is circulated in the system, only a split stream of this circulating stream is rejected, with remainder recycled to the combustor. As a consequence, there is unburned carbon and partially used, valuable, calcium hydroxide in the reject stream. If these useful materials in the reject stream can be recovered and sent back to the combustor, the efficiency of the system will be increased significantly and the equivalent emissions will be lower. This project studies an innovative concept to incorporate triboelectric separation into CFBC/FBC systems in order to preferentially split its recycle/reject streams based on material compositions of the particles. The objective is to answer whether useful constituents, like carbon, calcium carbonate and calcium hydroxide or oxide, can be selectively separated from combustion ash at elevated temperatures. Laboratory experimental studies are performed at temperatures from 25 C to 210 C, the data from which are presented in the form of recovery curves. These curves present quality-versus-quantity information useful for predicting the efficacy of triboelectric separation as applied to CFBC/FBC byproduct recycling and/or rejection.
Date: May 25, 2000
Creator: Ban, Heng & Stencel, J.M.
Partner: UNT Libraries Government Documents Department

MARKET ASSESSMENT AND TECHNICAL FEASIBILITY STUDY OF PRESSURIZED FLUIDIZED BED COMBUSTION ASH USE

Description: Western Research Institute, in conjunction with the Electric Power Research Institute, Foster Wheeler International, Inc. and the US Department of Energy, has undertaken a research and demonstration program designed to examine the market potential and the technical feasibility of ash use options for PFBC ashes. Ashes from the Foster Wheeler Energia Oy pilot-scale circulating PFBC tests in Karhula, Finland, combusting (1) low-sulfur subbituminous and (2) high-sulfur bituminous coal, and ash from the AEP's high-sulfur bituminous coal-fired bubbling PFBC in Brilliant, Ohio, were evaluated in laboratory and pilot-scale ash use testing at WR1. The technical feasibility study examined the use of PFBC ash in construction-related applications, including its use as a cementing material in concrete and use in cement manufacturing, fill and embankment materials, soil stabilization agent, and use in synthetic aggregate production. Testing was also conducted to determine the technical feasibility of PFBC ash as a soil amendment for acidic and sodic problem soils and spoils encountered in agricultural and reclamation applications. The results of the technical feasibility testing indicated the following conclusions. PFBC ash does not meet the chemical requirements as a pozzolan for cement replacement. However, it does appear that potential may exist for its use in cement production as a pozzolan and/or as a set retardant. PFBC ash shows relatively high strength development, low expansion, and low permeability properties that make its use in fills and embankments promising. Testing has also indicated that PFBC ash, when mixed with low amounts of lime, develops high strengths, suitable for soil stabilization applications and synthetic aggregate production. Synthetic aggregate produced from PFBC ash is capable of meeting ASTM/AASHTO specifications for many construction applications. The residual calcium carbonate and calcium sulfate in the PFE3C ash has been shown to be of value in making PFBC ash a suitable soil amendment for ...
Date: April 1, 1997
Creator: Bland, A.E. & Brown, T.H.
Partner: UNT Libraries Government Documents Department