High Temperature Particle Filtration Technology

High temperature filtration can serve to improve the economic, environmental, and energy performance of chemical processes. This project was designed to evaluate the stability of filtration materials in the environments of the production of dimethyldichlorosilane (DDS). In cooperation with Dow Corning, chemical environments for the fluidized bed reactor where silicon is converted to DDS and the incinerator where vents are cornbusted were characterized. At Oak Ridge National Laboratory (ORNL) an exposure system was developed that could simulate these two environments. Filter samples obtained from third parties were exposed to the environments for periods up to 1000 hours. Mechanical properties before and after exposure were determined by burst-testing rings of filter material. The results indicated that several types of filter materials would likely perform well in the fluid bed environment, and two materials would be good candidates for the incinerator environment

Deep Burn Develpment of Transuranic Fuel for High-Temperature Helium-Cooled Reactors - July 2010

The DB Program Quarterly Progress Report for April - June 2010, ORNL/TM/2010/140, was distributed to program participants on August 4. This report discusses the following: (1) TRU (transuranic elements) HTR (high temperature helium-cooled reactor) Fuel Modeling - (a) Thermochemical Modeling, (b) 5.3 Radiation Damage and Properties; (2) TRU HTR Fuel Qualification - (a) TRU Kernel Development, (b) Coating Development, (c) ZrC Properties and Handbook; and (3) HTR Fuel Recycle - (a) Recycle Processes, (b) Graphite Recycle, (c) Pyrochemical Reprocessing - METROX (metal recovery from oxide fuel) Process Development

The environmental dependence of redox energetics of PuO2 and \alpha-Pu2O3: A quantitative solution from DFT+U calculations

We report a comprehensive density functional theory (DFT) + $U$ study of the energetics of charged and neutral oxygen defects in both PuO$_{2}$ and $\alpha$-Pu$_{2}$O$_{3}$, and present a quantitative determination of the equilibrium compositions of reduced PuO$_{2}$ (PuO$_{2-x}$) as functions of environmental temperature and partial pressure of oxygen, which shows fairly agreement with corresponding high-temperature experiments. Under ambient conditions, the endothermic reduction of PuO$_{2}$ to $\alpha$-Pu$_{2}$O$_{3}$ is found to be facilitated by accompanying volume expansion of PuO$_{2-x}$ and the possible migration of O-vacancy, whereas further reduction of $\alpha$-Pu$_{2}$O$_{3}$ is predicted to be much more difficult. In contrast to the endothermic oxidation of PuO$_{2}$,\ the oxidation of $\alpha$-Pu$_{2}$O$_{3}$ is a stable exothermic process.Comment: 5 PLA pages, 4 figure

Chemical Vapor Infiltration Process Modeling and Optimization

Chemical vapor infiltration is a unique method for preparing continuous fiber ceramic composites that spares the strong but relatively fragile fibers from damaging thermal, mechanical, and chemical degradation. The process is relatively complex and modeling requires detailed phenomenological knowledge of the chemical kinetics and mass and heat transport. An overview of some of the current understanding and modeling of CVI and examples of efforts to optimize the processes is given. Finally, recent efforts to scale-up the process to produce tubular forms are described

Stability of High-Level Waste Forms

The objective of the proposed effort is to use a new approach to develop solution models of complex waste glass systems and spent fuel that are predictive with regard to composition, phase separation, and volatility. The effort will also yield thermodynamic values for waste components that are fundamentally required for corrosion models used to predict the leaching/corrosion behavior for waste glass and spent fuel material. This basic information and understanding of chemical behavior can subsequently be used directly in computational models of leaching and transport in geologic media, in designing and engineering waste forms and barrier systems, and in prediction of chemical interactions

Phase equilibria of advanced technology uranium silicide-based nuclear fuel

The phases in uranium-silicide binary system were evaluated in regards to their stabilities, phase boundaries, crystal structures, and phase transitions. The results from this study were used in combination with a well assessed literature to optimize the U-Si phase diagram using the CALPHAD method. A thermodynamic database was developed, which could be used to guide nuclear fuel fabrication, could be incorporated into other nuclear fuel thermodynamic databases, or could be used to generate data required by fuel performance codes to model fuel behavior in normal or off-normal reactor operations. The U3Si2 and U3Si5 phases were modeled using the Compound Energy Formalism model with 3 sublattices to account for the variation in composition. The crystal structure used for the USi phase was the tetragonal with an I4/mmm space. Above 450°C, the U3Si5 phase was modeled. The composition of the USi2 phase was adjusted to USi1.84. The calculated invariant reactions and the enthalpy of formation for the stoichiometric phases were in agreement with experimental data

Chemical vapor infiltration process modeling and optimization

Chemical vapor infiltration is a unique method for preparing continuous fiber ceramic composites that spares the strong but relatively fragile fibers from damaging thermal, mechanical, and chemical degradation. The process is relatively complex and modeling requires detailed phenomenological knowledge of the chemical kinetics and mass and heat transport. An overview of some of the current understanding and modeling of CVI and examples of efforts to optimize the processes is given. Finally, recent efforts to scale-up the process to produce tubular forms are described

Compatibility/Stability Issues in the Use of Nitride Kernels in LWR TRISO Fuel

The stability of the SiC layer in the presence of free nitrogen will be dependent upon the operating temperatures and resulting nitrogen pressures whether it is at High Temperature Gas-Cooled Reactor (HTGR) temperatures of 1000-1400 C (coolant design dependent) or LWR temperatures that range from 500-700 C. Although nitrogen released in fissioning will form fission product nitrides, there will remain an overpressure of nitrogen of some magnitude. The nitrogen can be speculated to transport through the inner pyrolytic carbon layer and contact the SiC layer. The SiC layer may be envisioned to fail due to resulting nitridation at the elevated temperatures. However, it is believed that these issues are particularly avoided in the LWR application. Lower temperatures will result in significantly lower nitrogen pressures. Lower temperatures will also substantially reduce nitrogen diffusion rates through the layers and nitriding kinetics. Kinetics calculations were performed using an expression for nitriding silicon. In order to further address these concerns, experiments were run with surrogate fuel particles under simulated operating conditions to determine the resulting phase formation at 700 and 1400 C

Forced Chemical Vapor Infiltration of Tubular Geometries: Modeling, Design, and Scale-Up

In advanced indirectly fired coal combustion systems and externally fired combined cycle concepts, ceramic heat exchangers are required to transfer heat from the hot combustion gases to the clean air that drives the gas turbines. For high efficiencies, the temperature of the turbine inlet needs to exceed 1,100 C and preferably be about 1,260 C. The heat exchangers will operate under pressure and experience thermal and mechanical stresses during heating and cooling, and some transients will be severe under upset conditions. Silicon carbide-matrix composites appear promising for such applications because of their high strength at elevated temperature, light weight, thermal and mechanical shock resistance, damage tolerance, and oxidation and corrosion resistance. The development of thick-walled, tubular ceramic composites has involved investigations of different fiber architectures and fixturing to obtain optimal densification and mechanical properties. The current efforts entail modeling of the densification process in order to increase densification uniformity and decrease processing time. In addition, the process is being scaled to produce components with a 10 cm outer diameter

Deep Burn: Development of Transuranic Fuel for High-Temperature Helium-Cooled Reactors- Monthly Highlights November 2010

During FY 2011 the DB Program will report Highlights on a monthly basis, but will no longer produce Quarterly Progress Reports. Technical details that were previously included in the quarterly reports will be included in the appropriate Milestone Reports that are submitted to FCRD Program Management. These reports will also be uploaded to the Deep Burn website. The Monthly Highlights report for October 2010, ORNL/TM-2010/300, was distributed to program participants on November 29, 2010. This report discusses the following: (1) Thermochemical Data and Model Development; (2) TRU (transuranic elements) TRISO (tri-structural isotropic) Development - (a) TRU Kernel Development, (b) Coating Development; (3) LWR Fully Ceramic Fuel - (a) FCM Fabrication Development, (b) FCM Irradiation Testing