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At least 793 records · Page 44

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DOE OSTI2013

Management of salt waste from electrochemical processing of used nuclear fuel

Electrochemical processing of used nuclear fuel involves operation of one or more cells containing molten salt electrolyte. Processing of the fuel results in contamination of the salt via accumulation of fission products and transuranic (TRU) actinides. Upon reaching contamination limits, the salt must be removed and either disposed or treated to remove the contaminants and recycled back to the process. During development of the Experimental Breeder Reactor-II spent fuel treatment process, waste salt from the electro-refiner was to be stabilized in a ceramic waste form and disposed of in a high-level waste repository. With the cancellation of the Yucca Mountain high-level waste repository, other options are now being considered. One approach that involves direct disposal of the salt in a geologic salt formation has been evaluated. While waste forms such as the ceramic provide near-term resistance to corrosion, they may not be necessary to ensure adequate performance of the repository. To improve the feasibility of direct disposal, recycling a substantial fraction of the useful salt back to the process equipment could minimize the volume of the waste. Experiments have been run in which a cold finger is used for this purpose to crystallize LiCl from LiCl/CsCl. If it is found to be unsuitable for transportation, the salt waste could also be immobilized in zeolite without conversion to the ceramic waste form. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS2003

Carbon Fiber Reinforced Ceramic Composites for Propulsion Applications

This report presents a critical review of the processing techniques for fabricating continuous fiber-reinforced CMCs for possible applications at elevated temperatures. Some of the issues affecting durability of the composite materials such as fiber coatings and cracking of the matrix because of shrinkage in PIP-process are also examined. An assessment of the potential inexpensive processes is also provided. Finally three potential routes of manufacturing C/SiC composites using a technology that NC A&T developed for carbon/carbon composites are outlined. Challenges that will be encountered are also listed.

Shivakumar, Kunigal↗

DOE OSTI2025

Development of direct ink write radially graded alumina/zirconia

Functionally graded materials (FGMs) are of interest in multiple fields, yet many materials combinations are limited by coefficient of thermal expansion (CTE) mismatch. Here, a radially graded alumina/yttria-doped zirconia (Al 2 O 3 /8YZ) FGM is used to demonstrate processing strategies to mitigate CTE and sintering behavior differences between these oxides. FGM materials are especially sensitive to ink stability during printing, as all components (in this case, Al 2 O 3 and 8YZ) must be stabilized in the same dispersant or additive solution. Thus, this system is also ideal to demonstrate ink optimization best practices. Materials were characterized throughout processing to correlate the effects of common additives on both the ceramic particle suspensions and final sintered components. Aggregation observed in the initial additive-containing suspensions were present in the sintered component. The differences in sintering onset temperature and shrinkage rate resulted in internal stresses within the sintered component, which ultimately caused mechanical failure of the component under low stress. In conclusion, a processing strategy was recommended to mitigate the sintering behavior mismatch of alumina and 8 wt% yttria-stabilized zirconia.

Lamm, Benjamin W. [Oak Ridge National Laboratory (↗

DOE OSTI2016

High charge-discharge performance of Pb{sub 0.98}La{sub 0.02}(Zr{sub 0.35}Sn{sub 0.55}Ti{sub 0.10}){sub 0.995}O{sub 3} antiferroelectric ceramics

The energy storage performance and charge-discharge properties of Pb{sub 0.98}La{sub 0.02}(Zr{sub 0.35}Sn{sub 0.55}Ti{sub 0.10}){sub 0.995}O{sub 3} (PLZST) antiferroelectric ceramics were investigated through directly measuring the hysteresis loops and pulse discharge current-time curves. The energy density only varies 0.2% per degree from 25 °C to 85 °C, and the energy efficiency maintains at about 90%. Furthermore, an approximate calculating model of maximum power density p{sub max} was established for the discharge process. Under a relatively high working electric field (8.2 kV/mm), this ceramics possess a greatly enhanced power density of 18 MW/cm{sup 3}. Moreover, the pulse power properties did not show degradation until 1500 times of charge-discharge cycling. The large released energy density, high energy efficiency, good temperature stability, greatly enhanced power density, and excellent fatigue endurance combined together make this PLZST ceramics an ideal candidate for pulse power applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Computational Fluid Dynamics Modeling of Bubbling in a Viscous Fluid for Validation of Waste Glass Melter Modeling

At the Hanford site, radioactive waste stored in underground tanks is slated for vitrification for final disposal. A comprehensive knowledge of the glass batch melting process will be useful in optimizing the process, which could potentially reduce the cost and duration of this multi-billion dollar cleanup effort. We are developing a high-fidelity heat transfer model of a Joule-heated ceramic lined melter to improve the understanding of the complex, inter-related processes occurring with the melter. The glass conversion rates in the cold cap layer are dependent on promoting efficient heat transfer. In practice, heat transfer is augmented by inserting air bubblers into the molten glass. However, the computational simulations must be validated to provide confidence in the solutions. As part of a larger validation procedure, it is beneficial to split the physics of the melter into smaller systems to validate individually. The substitution of molten glass for a simulant liquid with similar density and viscosity at room temperature provides a way to study mixing through bubbling as an isolated effect without considering the heat transfer dynamics. The simulation results are compared to experimental data obtained by the Vitreous State Laboratory at the Catholic University of America using bubblers placed within a large acrylic tank that is similar in scale to a pilot glass waste melter. Comparisons are made for surface area of the rising air bubbles between experiments and CFD simulations for a variety of air flow rates and bubble injection depths. Also, computed bubble rise velocity is compared to a well-accepted expression for bubble terminal velocity (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2018

Advanced Reaction System Program: Materials for ARS Reaction Chambers (FY18 Milestone, Subtask 3.3)

The objective of this effort is to identify materials and manufacturing technology that will allow the rapid construction and evaluation of computer modeled advanced reactor system designs to process specific carbon feedstock materials. Before full scale reaction systems can be built, prototypes need to be constructed and operated to validate the proposed new system performance against target criteria. The first steps, however, are to understand what type of materials are needed that can withstand the targeted process environments and determine how structures using those materials can be built. A wide range of reaction vessel conditions may exist in the processes being considered that could involve temperatures up to 1200°C, abrasive materials (high velocity coal and coal ash), different carbon feedstock materials (coal, biomass, and process wastes such as petcoke), corrosive and oxidizing/reducing gases, different material phases (solid, liquid, and gas), cyclic temperatures, microwave energy, customized vessel construction material needs (process stability, cost, weight, and compatibility with other materials), along with other known/unknown variables – all of which must be considered in selecting materials and considering manufacturing processes. The current focus of the research is to develop a reaction vessel sidewall structure consisting of a metal outer support and an inner ceramic (or cermet) protective surface. Ceramic coatings are desired because of their good corrosion and wear resistance, and because they are the material of choice to reduce metal shell temperature in high temperature processes. However significant property mismatches between metals and ceramics have been a roadblock to the joining of metals and ceramics.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

NASA NTRS2004

Durability and Design Issues of Thermal/environmental Barrier Coatings on Sic/sic Ceramic Matrix Composites Under 1650 C Test Conditions

Ceramic thermal/environmental barrier coatings for SiC-based ceramics will play an increasingly important role in future gas turbine engines because of their ability to effectively protect the engine components and further raise engine temperatures. However, the coating durability remains a major concern with the ever-increasing temperature requirements. Currently, advanced T/EBC systems, which typically include a high temperature capable zirconia- (or hahia-) based oxide top coat (thermal barrier) on a less temperature capable mullite/barium-strontium-aluminosilicate (BSAS)/Si inner coat (environmental barrier), are being developed and tested for higher temperature capability Sic combustor applications. In this paper, durability of several thermal/environmental barrier coating systems on SiC/SiC ceramic matrix composites was investigated under laser simulated engine thermal gradient cyclic, and 1650 C (3000 F) test conditions. The coating cracking and delamination processes were monitored and evaluated. The effects of temperature gradients and coating configurations on the ceramic coating crack initiation and propagation were analyzed using finite element analysis (FEA) models based on the observed failure mechanisms, in conjunction with mechanical testing results. The environmental effects on the coating durability will be discussed. The coating design approach will also be presented.

Zhu, Dong-Ming↗

DOE OSTI2020

Optimization of Lithium Content and Sintering Additives in Tape Cast Lithium Garnet Electrolyte Sheets

The lithium garnet (LLZO) remains one of the most promising electrolyte materials for producing solid state batteries. Tape casting is one method for producing the thin ceramic electrolyte layer required for a high-performance solid state battery. Processing of LLZO is complicated by several factors including lithium volatilization, abnormal grain growth and phase instability. Many of these issues are exacerbated in tape cast sheets by the sheets' higher surface area to volume ratio, when compared to pellet processing methods. Here, we report on an environmentally friendly aqueous tape casting process for LLZO using methylcellulose as a binder and compare final sheet properties to other, solvent-based, options. Solids loading, binder content, dispersant composition, and wetting agent type are varied to improve ease of casting and enhance properties of the as-cast tape. Lithium content in sintered LLZO sheets is controlled by the inclusion of excess Li 2 CO 3 as lithium source in the ceramic tape itself and by a novel method of producing a lithium-saturated furnace atmosphere. Sintering time and temperature are optimized, and rapid thermal processing is investigated as a method of reducing lithium loss. Al 2 O 3 and MgO are examined for use as sintering additives. Characterization of LLZO sheets is performed with XRD, EIS and SEM. Li 2 CO 3 and sintering additive levels are optimized for ionic conductivity and density. The optimization effort improved the conductivity and density of 100µm thick sintered sheets to greater than 3x10 -4 S/cm conductivity and 90% density.

36 MATERIALS SCIENCE↗

NASA NTRS2002

Environment-Conscious Ceramics (Ecoceramics) Technology Received 2001 R&D 100 Award

Since the dawn of human civilization, there has been a delicate balance between the use of resources as human frontiers expanded and the need to have a minimum influence on the ecosystem. The first 200 years of the industrial revolution essentially solved the problem of production. However, the massive production of goods also generated tremendous amounts of byproducts and wastes. In the new millennium, to sustain a healthy life in harmony with nature, it will be extremely important for us to develop various materials, products, and processes that minimize any harmful influence on the environment. Environment-conscious ceramics (ecoceramics) are a new class of materials that can be fabricated with renewable resources (wood) and wood waste material (wood sawdust). Wood is a "lignocellulosic" material formed by the photosynthetic reaction within the needles or leaves of trees. The photosynthesis process uses sunlight to take carbon dioxide from air and convert it into oxygen and organic materials. Wood has been known to be one of the best and most intricate engineering materials created by nature and known to mankind. In addition, natural woods of various types are available throughout the world. On the other hand, wood sawdusts are generated in abundant quantities by sawmills. Environment-conscious ceramic materials, fabricated via the pyrolysis and infiltration of natural wood-derived preforms, have tailorable properties with numerous potential applications. The experimental studies conducted to date on the development of materials based on biologically derived structures indicate that these materials behave like ceramic materials manufactured by conventional approaches. These structures have been shown to be quite useful in producing porous or dense materials having various microstructures and compositions.

Singh, Mrityunjay↗

DOE OSTI2023

Thermodynamic and Kinetic Barriers Limiting Solid-State Reactions Resolved through In Situ Synchrotron Studies of Lithium Halide Salts

Although halide salts such as LiCl and LiBr are routinely used as a source of Li ions during ion exchange reactions, a detailed understanding of the processes controlling the rates of these reactions is presently lacking. Recently, it has been discovered that the rate limiting barriers for ion exchange are commonly associated with these salts rather than the ceramic target of ion exchange, making it important to quantitatively understand of salt processes. Here it is demonstrated that in situ synchrotron studies of ion exchange reactions can be used to precisely quantify the thermodynamic activation energies associated with these solid state reactions in a manner that can be directly compared with predictions from density functional theory (DFT). While the temperature dependence of the LiCl reaction rate is found to be set by a barrier associated with ion hopping, it was discovered that for LiBr it is also affected by the defect formation energy – an energy found to be substantially lower than predicted by DFT. Furthermore, it is shown that when reaction rates for different relative amounts of reactants are varied, it is possible to identify the rate-limiting reagent and to elucidate an overall scaling relationship that controls the concentration-dependence of the reaction rate. Also, it is demonstrated that global fits across doped and undoped salts can be used to probe both intrinsic and extrinsic vacancy concentrations. This improved understanding of ion exchange mechanisms can be used to accelerate ion exchange reaction rates by orders of magnitude. In conclusion, the techniques demonstrated here can be broadly applied to probe the kinetics and thermodynamics of solid state reactions.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Computational Fluid Dynamics Modeling of Bubbling in a Viscous Fluid for Validation of Waste Glass Melter Modeling

bubbling↗

DOE OSTI2022

Novel Ultrafast Lu2O3:Yb Ceramics for Future HEP Applications

Inorganic scintillators activated by charge transfer luminescence Yb3+ are considered promising ultrafast material to break the ps timing barrier for future high energy physics applications. Inorganic scintillators in ceramic form are potentially more cost-effective than crystals because of their lower fabrication temperature and no need for aftergrowth mechanical processing. This paper reports an investigation on Lu2O3:Yb and Lu2xY2(1−x)O3:Yb scintillating ceramic samples fabricated by Radiation Monitoring Devices Inc. All samples show X-ray excited luminescence peaked at 370 nm. Ultrafast decay time of 1.1 ns was observed by using a microchannel plate-photomultiplier tube-based test bench at Caltech. Considering its intrinsic high density (9.4 g/cm3), Lu2O3:Yb ceramics are promising for future time of fight application for high energy physics experiments.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Laser-Induced Thermal Decomposition of Uranium Coordination Compounds with Non-oxidic Ligands to Produce Nitride and Carbide Materials

The production of ceramics from uranium coordination compounds can be achieved through thermal processing if an excess amount of the desired atoms (i.e., C or N), or reactive gaseous products (e.g., methane or nitrogen oxide) is made available to the reactive uranium metal core via decomposition/fragmentation of the surrounding ligand groups. Here, computational thermodynamic approaches were utilized to identify the temperatures necessary to produce uranium metal from some starting compounds—UI 4 (TMEDA) 2 , UCl 4 (TMEDA) 2 , UCl 3 (pyridine) x , and UI 3 (pyridine) 4 . Experimentally, precursors were irradiated by a laser under various gaseous environments (argon, nitrogen, and methane) creating extreme reaction conditions (i.e., fast heating, high temperature profile >2000 °C, and rapid cooling). Despite the fast dynamics associated with laser irradiation, the central uranium atom reacted with the thermal decomposition products of the ligands yielding uranium ceramics. Residual gas analysis identified vaporized products from the laser irradiation, and the final ceramic products were characterized by powder X-ray diffraction. The composition of the uranium precursor as well as the gaseous environment had a direct impact on the production of the final phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2004

Combining Hard with Soft Materials in Nanoscale Under High-Pressure High-Temperature Conditions

Nano-composites with a primary nanocrystalline ceramic matrix and a secondary nanocrystalline material (metal or semiconductor) were synthesized by infiltration of an appropriate liquid into ceramic compacts under pressures of up to 8 GPa and temperatures of up to 2000 K. The purpose of our work is to obtain nanocomposites which constitute homoger?ous mixtures of two phases, both forming nano- grains of about 10 nm in size. The high pressure is used to bring the porosity of the compacted powders down to the nano-scale and force a given liquid into the nano-sized pores. The advantage of the infiltration technique is that, in a single, continuous process, we start with a nanocrystalline powder, compress it to form the matrix of the composite, and crystallize and/or synthesize a second nanomaterial in the matrix pores. The key limitation of this technology is, that the pores in the matrix need to stay open during the entire process of infiltration. Thus the initial powder should form a rigid skeleton, otherwise the so-called self-stop process can limit cr block a further flow of the liquid phase and hinder the process of the composite formation. Therefore powders of only very hard ceramic materials like diamond, Sic, or Alz03, which can withstand a substantial external load without undesired deformation, can be used as the primary phase. With this technique, using diamond and S i c ceramic powders infiltrated by liquid metals (AI, Zn, Sn, Ag, Au) and semiconductors (Si, Ge, GaAs, CdTe), we obtained nano-composites with the grain size in the range of 10 - 30 nm. Our work addresses the key problem in manufacturing bulk nanocrystalline materials, i.e. preservation of nano-scale during the fabrication process. In this paper we discuss basic technical and methodological problems associated with nano-infiltration based on the results obtained for Zn-Sic composites.

Palosz, B.↗

NASA NTRS2008

Current Computational Challenges for CMC Processes, Properties, and Structures

In comparison to current state-of-the-art metallic alloys, ceramic matrix composites (CMC) offer a variety of performance advantages, such as higher temperature capability (greater than the approx.2100 F capability for best metallic alloys), lower density (approx.30-50% metal density), and lower thermal expansion. In comparison to other competing high-temperature materials, CMC are also capable of providing significantly better static and dynamic toughness than un-reinforced monolithic ceramics and significantly better environmental resistance than carbon-fiber reinforced composites. Because of these advantages, NASA, the Air Force, and other U.S. government agencies and industries are currently seeking to implement these advanced materials into hot-section components of gas turbine engines for both propulsion and power generation. For applications such as these, CMC are expected to result in many important performance benefits, such as reduced component cooling air requirements, simpler component design, reduced weight, improved fuel efficiency, reduced emissions, higher blade frequencies, reduced blade clearances, and higher thrust. Although much progress has been made recently in the development of CMC constituent materials and fabrication processes, major challenges still remain for implementation of these advanced composite materials into viable engine components. The objective of this presentation is to briefly review some of those challenges that are generally related to the need to develop physics-based computational approaches to allow CMC fabricators and designers to model (1) CMC processes for fiber architecture formation and matrix infiltration, (2) CMC properties of high technical interest such as multidirectional creep, thermal conductivity, matrix cracking stress, damage accumulation, and degradation effects in aggressive environments, and (3) CMC component life times when all of these effects are interacting in a complex stress and service environment. To put these computational issues in perspective, the various modeling needs within these three areas are briefly discussed in terms of their technical importance and their key controlling mechanistic factors as we know them today. Emphasis is placed primarily on the SiC/SiC ceramic composite system because of its higher temperature capability and enhanced development within the CMC industry. A brief summary is then presented concerning on-going property studies aimed at addressing these CMC modeling needs within NASA in terms of their computational approaches and recent important results. Finally an overview perspective is presented on those key areas where further CMC computational studies are needed today to enhance the viability of CMC structural components for high-temperature applications.

DiCarlo, James↗

DOE OSTI2015

Proton conducting ceramics in membrane separations

Perovskite materials of the general formula SrCeO.sub.3 and BaCeO.sub.3 are provided having improved conductivity while maintaining an original ratio of chemical constituents, by altering the microstructure of the material. A process of making Pervoskite materials is also provided in which wet chemical techniques are used to fabricate nanocrystalline ceramic materials which have improved grain size and allow lower temperature densification than is obtainable with conventional solid-state reaction processing.

36 MATERIALS SCIENCE↗

DOE OSTI2013

High energy storage density performance of Ba, Sr-modified lead lanthanum zirconate titanate stannate antiferroelectric ceramics

Graphical abstract: Polarization hysteresis (P–E) loops of the (Pb{sub 0.85}Ba{sub 0.08}Sr{sub 0.03}La{sub 0.03}) (Zr{sub 0.74}Sn{sub 0.22}Ti{sub 0.04}) samples: (a) measured at different applied electric-field and (b) measured at different temperatures is shown. It is typical antiferroelectrics whose remnant polarization is zero. As the remnant polarization of AFE is small and the ceramics are accompanied by the formation of the anti-parallel domain structure, energy stored in PLZST can be effectively released. Thus we calculated the energy density from the P–E loop and obtained the power density was up to 1.2 J/cm{sup 3} at 55 °C, and at 45 °C the energy density was ∼1.24 J/cm{sup 3}. As usual, for bulk ceramics, the switching between the AFE and FE states occurs at lower field. This value is much higher than that reported previously for the PLZT bulk ceramic (0.4 J/cm{sup 3}). - Highlights: • Ba{sup 2+}, Sr{sup 2+} co-doping caused the T{sub c} of PLZST moved to the lower temperature (T{sub c} ≈ 40 °C). • The ΔE was so smaller, E{sub AF} ≈ 90 kV/cm and E{sub FA} ≈ 85 kV/cm. • Ba, Sr co-doped PLZST ceramic exhibited slanted P–E loops with a large breakdown field (100 kV/cm). • A high energy density was up to 1.2 J/cm{sup 3}. - Abstract: (Pb{sub 0.85}Ba{sub 0.08}Sr{sub 0.03}La{sub 0.03})(Zr{sub 0.74}Sn{sub 0.22}Ti{sub 0.04}) (Ba, Sr co-doped PLZST) co-doping antiferroelectric (AFE) ceramics with orthorhombic perovskite structure were prepared by the traditional solid state reaction process. It was observed that the doping of barium and strontium caused the Curie temperature of PLZST move to the lower temperature (T{sub c} ≈ 40 °C). Ba, Sr co-doped PLZST AFE ceramics exhibited excellent electrical properties, the AFE to ferroelectric (FE) transition occurred at field E{sub AF} ≈ 90 kV/cm, and the transition from FE to AFE occurred at E{sub FA} ≈ 85 kV/cm. The maximum relative permittivity was about 4800, occurring at a field near the AFE to FE transition point, with a dielectric loss of 0.006. The samples exhibited small ΔE and slanted hysteresis loops with a large breakdown field of 100 kV/cm due to Ba, Sr co-doping ceramics, and a high energy density of 1.2 J/cm{sup 3}.

36 MATERIALS SCIENCE↗

NASA NTRS1978

Advanced ceramic material for high temperature turbine tip seals

Ceramic material systems are being considered for potential use as turbine blade tip gas path seals at temperatures up to 1370 1/4 C. Silicon carbide and silicon nitride structures were selected for study since an initial analysis of the problem gave these materials the greatest potential for development into a successful materials system. Segments of silicon nitride and silicon carbide materials over a range of densities, processed by various methods, a honeycomb structure of silicon nitride and ceramic blade tip inserts fabricated from both materials by hot pressing were tested singly and in combination. The evaluations included wear under simulated engine blade tip rub conditions, thermal stability, impact resistance, machinability, hot gas erosion and feasibility of fabrication into engine components. The silicon nitride honeycomb and low-density silicon carbide using a selected grain size distribution gave the most promising results as rub-tolerant shroud liners. Ceramic blade tip inserts made from hot-pressed silicon nitride gave excellent test results. Their behavior closely simulated metal tips. Wear was similar to that of metals but reduced by a factor of six.

Solomon, N. G.↗