Andrew M. Casella

Deposition Velocities of Newtonian and Non-Newtonian Slurries in Pipelines

The WTP pipe plugging issue, as stated by the External Flowsheet Review Team (EFRT) Executive Summary, is as follows: “Piping that transports slurries will plug unless it is properly designed to minimize this risk. This design approach has not been followed consistently, which will lead to frequent shutdowns due to line plugging.” A strategy was employed to perform critical-velocity tests on several physical simulants. Critical velocity is defined as the point where a stationary bed of particles deposits on the bottom of a straight horizontal pipe during slurry transport operations. Results from the critical velocity testing provide an indication of slurry stability as a function of fluid rheological properties and transport conditions. The experimental results are compared to the WTP design guide on slurry transport velocity in an effort to confirm minimum waste velocity and flushing velocity requirements as established by calculations and critical line velocity correlations in the design guide. The major findings of this testing is discussed below. Experimental results indicate that the use of the Oroskar and Turian (1980) correlation in the design guide is conservative—Slurry viscosity has a greater affect on particles with a large surface area to mass ratio. The increased viscous forces on these particles result in a decrease in predicted critical velocities from this traditional industry derived equations that focus on particles large than 100 m in size. Since the Hanford slurry particles generally have large surface area to mass ratios, the reliance on such equations in the Hall (2006) design guide is conservative. Additionally, the use of the 95% percentile particle size as an input to this equation is conservative. However, test results indicate that the use of an average particle density as an input to the equation is not conservative. Particle density has a large influence on the overall result returned by the correlation. Lastly, the viscosity correlation used in the WTP design guide has been shown to be inaccurate for Hanford waste feed materials. The use of the Thomas (1979) correlation in the design guide is not conservative—In cases where 100% of the particles are smaller than 74 m or particles are considered to be homogeneous due to yield stress forces suspending the particles the homogeneous fraction of the slurry can be set to 100%. In such cases, the predicted critical velocity based on the conservative Oroskar and Turian (1980) correlation is reduced to zero and the design guide returns a value from the Thomas (1979) correlation. The measured data in this report show that the Thomas (1979) correlation predictions often fall below that measured experimental values. A non-Newtonian deposition velocity design guide should be developed for the WTP— Since the WTP design guide is limited to Newtonian fluids and the WTP expects to process large quantities of such materials, the existing design guide should be modified address such systems. A central experimental finding of this testing is that the flow velocity required to reach turbulent flow increases with slurry rheological properties due to viscous forces dampening the formation of turbulent eddies. The flow becomes dominated by viscous forces rather than turbulent eddies. Since the turbulent eddies necessary for particle transport are not present, the particles will settle when crossing this boundary called the transitional deposition boundary. This deposition mechanism should be expected and designed for in the WTP.

Nitrogen Trifluoride-Based Fluoride- Volatility Separations Process: Initial Studies

This document describes the results of our investigations on the potential use of nitrogen trifluoride as the fluorinating and oxidizing agent in fluoride volatility-based used nuclear fuel reprocessing. The conceptual process uses differences in reaction temperatures between nitrogen trifluoride and fuel constituents that produce volatile fluorides to achieve separations and recover valuable constituents. We provide results from our thermodynamic evaluations, thermo-analytical experiments, kinetic models, and provide a preliminary process flowsheet. The evaluations found that nitrogen trifluoride can effectively produce volatile fluorides at different temperatures dependent on the fuel constituent.

Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than the approximately 10% typical of todays confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of approximately the same accuracy as the pure empirical approach. In addition, total Pu with much better accuracy with the hybrid approach than the pure analytical approach. In FY2012, PNNL will continue efforts to optimize its empirical model and minimize its reliance on calibration data. In addition, PNNL will continue to develop an analytical model, considering effects such as neutron-scattering in the fuel and cladding, as well as neutrons streaming through gaps between fuel pins in the fuel assembly.

Fuel Thermo-physical Characterization Project: Evaluation of Models to Calculate Thermal Diffusivity of Layered Composites

The Office of Material Management and Minimization Fuel Thermo-physical Characterization Project at Pacific Northwest National Laboratory (PNNL) is tasked with using PNNL facilities and processes to receive irradiated low enriched uranium-molybdenum fuel plate samples and perform analyses in support of the Office of Material Management and Minimization Reactor Conversion Program. This work is in support of the Fuel Development Pillar that is managed by Idaho National Laboratory. A key portion of the scope associated with this project was to measure the thermal properties of fuel segments harvested from plates that were irradiated in the Advanced Test Reactor. Thermal diffusivity of samples prepared from the fuel segments was measured using laser flash analysis. Two models, one developed by PNNL and the other developed by the Technische Universitat Munchen (TUM), were evaluated to extract the thermal diffusivity of the uranium-molybdenum alloy from measurements made on the irradiated, layered composites. The experimental data of the “TC” irradiated fuel segment was evaluated using both models considering a three-layer and five-layer system. Both models are in acceptable agreement with one another and indicate that the zirconium diffusion barrier has a minimal impact on the overall thermal diffusivity of the monolithic U-Mo fuel.

Modeling of Particulate Behavior in Pinhole Breaches

Abstract A model is presented for calculating depressurization time for and particulate release from used nuclear fuel dry storage containers that have developed a pinhole breach. Particular attention is given to particulate deposition and transmission within the breach pathway. The model is modular in nature and is developed in a way that allows for more advanced treatments of internal temperature, internal component geometry, or aerosol flow to be readily incorporated. The model can be treated as a basis for addressing concerns associated with monitoring and verification efforts during long-term dry cask storage.

Assaying Used Nuclear Fuel Assemblies Using Lead Slowing-Down Spectroscopy and Singular Value Decomposition

This study investigates the use of a Lead Slowing-Down Spectrometer (LSDS) for the direct and independent measurement of fissile isotopes in light-water nuclear reactor fuel assemblies. The current study applies MCNPX, a Monte Carlo radiation transport code, to simulate the measurement of the assay of the used nuclear fuel assemblies in the LSDS. An empirical model has been developed based on the calibration of the LSDS to responses generated from the simulated assay of six well-characterized fuel assemblies. The effects of self-shielding are taken into account by using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the self-shielding functions from the assay of assemblies in the calibration set. The performance of the empirical algorithm was tested on version 1 of the Next-Generation Safeguards Initiative (NGSI) used fuel library consisting of 64 assemblies, as well as a set of 27 diversion assemblies, both of which were developed by Los Alamos National Laboratory. The potential for direct and independent assay of the sum of the masses of Pu-239 and Pu-241 to within 2%, on average, has been demonstrated.

Assessment of the Use of Nitrogen Trifluoride for Purifying Coolant and Heat Transfer Salts in the Fluoride Salt-Cooled High-Temperature Reactor

This report provides an assessment of the use of nitrogen trifluoride for removing oxide and water-caused contaminants in the fluoride salts that will be used as coolants in a molten salt cooled reactor.

Characterization of the kinetics of NF3-fluorination of NpO2

Solid NpO2 has been contacted by gaseous NF3 under isothermal conditions at 450°C, 475°C, and 500°C; and the resulting reactions have been monitored using thermogravimetric analysis. In each case, at least two sequential reactions are clearly observed. The first reaction is fluorination of NpO2 to NpF4 and the second is oxidation and fluorination of NpF4 to NpF6. Careful observation of the experimental reaction curves reveals evidence of several physical and chemical mechanisms occurring sequentially and at times simultaneously. As such, a mathematical modeling approach utilizing a combination of sequential and parallel fundamental gas-solid reaction mechanisms (chemical reaction, diffusion, and phase boundary) is, in general, found to provide representative reaction curves that are in good agreement with experimental reaction curves. The correspondence of fundamental reaction mechanisms with distinctive characteristics of the experimental reaction curves (maximums and inflection points) provides insight ...

Uniform deposition of uranium hexafluoride (UF6): Standardized mass deposits and controlled isotopic ratios using a thermal fluorination method

We report a convenient method for the generation of volatile uranium hexafluoride (UF6) from solid uranium oxides and other U compounds, followed by uniform deposition of low levels of UF6 onto sampling coupons. Under laminar flow conditions, UF6 is shown to interact with surfaces within a fixed reactor geometry to a highly predictable degree. We demonstrate the preparation of U deposits that range between approximately 0.01 and 500ngcm(-2). The data suggest the method can be extended to creating depositions at the sub-picogramcm(-2) level. The isotopic composition of the deposits can be customized by selection of the U source materials and we demonstrate a layering technique whereby two U solids, each with a different isotopic composition, are employed to form successive layers of UF6 on a surface. The result is an ultra-thin deposit that bears an isotopic signature that is a composite of the two U sources. The reported deposition method has direct application to the development of unique analytical standards for nuclear safeguards and forensics. Further, the method allows access to very low atomic or molecular coverages of surfaces.

Monte Carlo N-particle tracking of ultrafine particle flow in bent microtubes

ABSTRACT The problem of large pressure-differential-driven laminar convective–diffusive ultrafine aerosol flow through bent microtubes is of interest in several contemporary research areas including; release of contents from pressurized containment vessels, aerosol sampling equipment, advanced scientific instruments, gas-phase microheat exchangers, and microfluidic devices. In each of these areas, the predominant problem is the determination of the fraction of particles entering the microtube that is deposited within the tube and the fraction that is transmitted through. Due to the extensive parameter restrictions of this class of problems, a Lagrangian particle tracking method making use of the coupling of the analytical stream line solutions of Dean for convective motion and a sampling of a Gaussian distribution for diffusive motion is a useful tool in problem characterization. This method is a direct analog to the Monte Carlo N-Particle method of particle transport extensively used in nuclear physics and engineering. In this work, 10-nm-diameter particles with a density of 1 g/cm3 are tracked within microtubes with toroidal bends with pressure differentials ranging between 0.2175 and 0.87 atmospheres. The tubes have radii of 25 microns or 50 microns and the radius of curvature is either 1 m or 0.3183 cm. The carrier gas is helium, and temperatures of 298 K and 558 K are considered. Numerical convergence is considered as a function of time step size and of the number of particles per simulation. Particle transmission rates and deposition patterns within the bent microtubes are calculated. Copyright