Physical Sciences and Mathematics Commons^™

Theoretical Modeling Of Protective Oxide Layer Growth In Non-Isothermal Lead-Alloys Coolant Systems: Quarterly Progress Report (01/01/05- 03/31/05), Yitung Chen

Transmutation Sciences Materials (TRP)

The goal of the proposed research project is to provide basic understanding of the protective oxide layer behaviors and to develop oxide layer growth models of steels in non-isothermal lead-alloys (lead or lead-bismuth eutectic) coolant systems. It is widely recognized that the corrosiveness of the lead-alloys is a critical obstacle and challenge for which it can be safely used or applied in the nuclear coolant systems. Active oxygen control technique can promote the formation of the “self-healing” oxide films on the structural material surface, drastically reducing steel corrosion and coolant contamination. Many experiments of steels exposed to flowing lead-alloys have …

Fundamental Chemistry Of U And Pu In The Tbp-Dodecane-Nitric Acid System: Quaterly Report January - March, 2005, Kenneth Czerwinski, Cynthia-May Gong, Amber Wright

Separations Campaign (TRP)

The speciation of hexavalent U and tetravalent Pu will be examined in the TBP-dodecane-nitric acid systems. This topic is chosen based on data needs for separation modeling identified by the AFCI. Emphasis will be placed on studying the influence of nitrate and acetohydroxamic acid on U and Pu speciation as well as conditions where a third phase forms in the organic phase. The organic phase will be 30% TBP in dodecane. Equal volumes of aqueous and organic phase will be used. The speciation of the actinides in the aqueous and organic phase will be determined by a number of different …

Fundamental Chemistry Of U And Pu In The Tbp-Dodecane-Nitric Acid System: Quarterly Report January - March, 2006, Amber Wright, Frederic Poineau, Kenneth Czerwinski

Separations Campaign (TRP)

The speciation of hexavalent U and tetravalent Pu will be examined in the Tributylphosphate (TBP)-dodecane-nitric acid systems. This topic is chosen based on data needs for separation modeling identified by the AFCI. Emphasis will be placed on studying the influence of nitrate and acetohydroxamic acid on U and Pu speciation as well as conditions where a third phase forms in the organic phase. The organic phase will be 30% TBP in dodecane. Equal volumes of aqueous and organic phase will be used. The speciation of the actinides in the aqueous and organic phase will be determined by a number of …

Neutron Multiplicity Measurements For The Afci Program Quarterly Progress Report January-March 2005, Denis Beller

Transmutation Sciences Physics (TRP)

The U.S. Advanced Fuel Cycle Initiative (AFCI) is a program to develop economic and environmental methods to reduce the impact of waste from commercial nuclear fuel cycles. One concept for near-complete destruction of waste isotopes from used nuclear fuel is accelerator driven transmutation. High-power accelerators would be used to produce high-energy charged particles, which then collide with heavy metal targets to create a cascade of neutrons. These neutrons then cause a nuclear chain reaction in subcritical systems. Fission neutrons then transmute fissile waste isotopes as well as other problematic isotopes such as technetium-99 and iodine-129. To design these systems, complex …

Dissolution, Reactor, And Environmental Behavior Of Zro2-Mgo Inert Fuel Matrix: Quarterly Report, January 2005 To March 2005, Earl Wolfram, Thomas Hartmann, Kenneth Czerwinski

Fuels Campaign (TRP)

This project will examine inert matrix fuels containing ZrO₂ and MgO as the inert matrix, with the relative amount of MgO varied from 30% to 70% in ZrO₂. Reactor physics calculations will be used to examine suitable quantities of burnable poisons from the candidate elements Gd, Er, or Hf with reactor grade Pu providing the fissile component, with up to 10% of ²³⁹Pu. Ceramics will be synthesized and characterized based on the reactor physics results. The solubility the fuel ceramics, in reactor conditions, reprocessing conditions, and repository conditions, will be investigated in a manner to provide …

Impact Of The Synthesis Process On Structure Properties For Afci Fuel Candidates, Thomas Hartmann, Kenneth Czerwinski

Fuels Campaign (TRP)

Transmutation work at Los Alamos National Laboratory is currently focused on mono-nitride ceramic fuel forms, and consists of closely coordinated “hot” actinide and “cold” inert and surrogate fuels work. Matrix and surrogate materials work involves three major components: (1) fuel matrix synthesis and fabrication, (2) fuel performance, and (3) fuel materials modeling. The synthesis and fabrication component supports basic material studies, as well as actinide fuel fabrication work through fuel fabrication process development. Fuel performance studies are examining the tolerance of nitride-type fuel to heavy irradiation damage. The fuel materials simulation work involves both atomistic and continuum scale modeling employing …

Dissolution, Reactor, And Environmental Behavior Of Zro2-Mgo Inert Fuel Matrix: Neutronic Evaluation Of Zro2-Mgo Inert Fuels, E. Fridman, S. Kolesnikov, E. Shwageraus, A. Galperin

Fuels Campaign (TRP)

This report presents the results of the Task 3, defined in working program as: evaluation of burnable poison designs. Adopting the basic design of a standard PWR and Pu loadings required for 18-month cycle (results of Task 2), this part of the program is aimed to estimate performance of each BP design and BP material to address challenges of Fertile-Free Fuel (FFF) Concept. Finally, an optimal BP design will be developed and an overall feasibility of FFF concept will be determined. Basically, the main challenge encountered in neutronic design for a FFF core is to develop reactivity control system which …

Immobilization Of Fission Iodine By Reaction With A Fullerene Containing Carbon Compound And Insoluble Natural Organic Matrix: Quaterly Report October-December 2004, Spencer M. Steinberg

Separations Campaign (TRP)

We have conducted a large number of experiments to determine the possible reaction of iodate with sphagnum peat moss. These experiments indicate that the natural organic material reacts with iodate resulting in the formation of organically bound iodine and/or iodide in solution.

In the last quarter, we have conducted a number of experiments at various pHs and several temperatures (70oC, 60oC and 40oC). The reaction of iodate with peat follows pseudo first-order kinetics, although the reaction rate does appear to decrease significantly with reaction time. As noted in a previous report organically bound iodine appears to go through a maximum …

Design Concepts And Process Analysis For Transmuter Fuel Manufacturing: Quarterly Progress Report #1, Jamil M. Renno, Georg F. Mauer

Fuels Campaign (TRP)

A Hot Cell robotic assembly: Pick and place dynamic simulation, including feedback control with Matlab, was developed for dispersion fuel manufacture.

The deployment of remote manufacturing of transmuter fuel is a necessity for the transmutation applications. In the reporting period, a virtual hot cell for the manufacturing of dispersion fuel was designed using MSC.visualNastran^©, ProEngineer^© and MATLAB^©. Atypical events were successfully simulated. Relevant physical quantities arising during such events were monitored as well.

Effect Of Silicon Content On The Corrosion Resistance And Radiation-Induced Embrittlement Of Materials For Advanced Heavy Liquid Metal Nuclear Systems: Quarterly Progress Report (August 2004 – October 2004), Ajit K. Roy

Transmutation Sciences Materials (TRP)

The purpose of this collaborative research project involving the University of Nevada Las Vegas (UNLV), Los Alamos National Laboratory (LANL) and Idaho State University (ISU) is to evaluate the effect of silicon (Si) content on the corrosion behavior and radiation-induced embrittlement of martensitic stainless steels having chemical compositions similar to that of the modified 9Cr-1Mo steel. Recent studies at LANL involving Alloy EP-823 of different Si content have demonstrated that increased Si content in this alloy may enhance the corrosion resistance in molten lead-bismutheutectic (LBE). Since very little data exists in the open literature on the beneficial effect of Si …

Use Of Positron Annihilation Spectroscopy For Stress-Strain Measurements: Quarterly Progress Report (September 01 – November 30, 2004), Ajit K. Roy

Transmutation Sciences Materials (TRP)

Accomplishments:

● A technical paper titled “Residual Stress Characterization in Structural Materials by Destructive and Nondestructive Techniques” has been accepted for publication in the Journal of Materials Engineering and Performance, ASM International, Ohio.

● The PAS method has been applied to develop calibration curves for line shape parameters (S and T) using unstressed and stressed (different magnitude) tensile specimens of martensitic stainless steels. These curves will enable the determination of residual stresses in plastically-deformed materials once the magnitude of S or T parameter is determined by the PAS technique.

● The tensile and welded specimens have been irradiated by low …

An Examination Of Avoided Costs In Utah, Mark Bolinger, Ryan Wiser

All U.S. Government Documents (Utah Regional Depository)

The Utah Wind Working Group (UWWG) believes there are currently opportunities to encourage wind power development in the state by seeking changes to the avoided cost tariff paid to qualifying facilities (QFs). These opportunities have arisen as a result of a recent re-negotiation of Pacificorp’s Schedule 37 tariff for wind QFs under 3 MW, as well as an ongoing examination of Pacificorp’s Schedule 38 tariff for wind QFs larger than 3 MW. It is expected that decisions made regarding Schedule 38 will also impact Schedule 37. Through the Laboratory Technical Assistance Program (Lab TAP), the UWWG has requested (through the …

Development Of A Systems Engineering Model Of The Chemical Separations Process, Yitung Chen, Darrell Pepper, Sean Hsieh

Separations Campaign (TRP)

The chemical processing of used nuclear fuel is an integral component of any strategy for the transmutation of nuclear waste. Due to the large volume of material that must be handled in this first step of the transmutation process, the efficiency of the separations process is a key factor in the potential economic viability of transmutation strategies. The ability to optimize the chemical separation systems is vital to ensure the feasibility of the transmutation program.

Systems analysis, or total systems modeling, is one of the strongest tools available to researchers for understanding and optimizing complex systems such as chemical separations …

Nuclear Criticality, Shielding, And Thermal Analyses Of Separations Processes For The Transmutation Fuel Cycle, William Culbreth, Denis Beller

Separations Campaign (TRP)

The first step in any transmutation strategy is the separation of radionuclides in used nuclear fuel. The current separation strategy supporting the Advanced Fuel Cycle Initiative (AFCI) program is based on the use of a solvent extraction separation process to separate the actinides, fission products, and uranium from used commercial nuclear fuel, and on the use of pyrochemical separation technologies to process used transmuter fuels. To separate the fission products and transuranic elements from the uranium in used fuel, the national program is developing a new solvent extraction process, the Uranium Extraction Plus, or UREX+, process based on the traditional …

Immobilization Of Fission Iodine By Reaction With A Fullerene Containing Carbon Compound And Insoluble Natural Matrix, Spencer M. Steinberg, Gary Cerefice, David W. Emerson

Separations Campaign (TRP)

The recovery of iodine released during the processing of used nuclear fuel poses a significant challenge to the transmutation of nuclear waste. Iodine-129, a long-lived fission product formed by both commercial nuclear power generation and nuclear weapons production, is released when reprocessing nuclear fuel. Since iodine can be concentrated in the human thyroid, any uncontrolled release of iodine may result in an increased rate of thyroid cancer in the exposed population. For this reason, recovery of iodine is important for implementing any nuclear transmutation strategy.

The stability of the association of iodine with FCC and NOM products are studied. Product …

Development, Fabrication And Study Of Fullerene-Containing Carbon Material (Fcc) For Immobilization Of Iodine: Progress Report #1-4, Michael Savopulo, Boris E. Burakov

Separations Campaign (TRP)

During current reporting period the experiments on synthesis of ceramic-like material by conversion of iodine-doped FCC and activated carbon to Si_xC_y have been completed. Cold pressed granules of FCC and activated carbon were rinsed in water-ethanol solution of tetraethoxysilane (TEOS), Si(OC₂H₅)₄, and then used for further synthesis. All new samples obtained have been studied using precise powder XRD analysis.

Development, Fabrication And Study Of Fullerene-Containing Carbon Material (Fcc) For Immobilization Of Iodine: Final Report 2005, Michael Savopulo, Boris E. Burakov

Separations Campaign (TRP)

Immobilization of highly radioactive and long-lived isotope of ¹²⁹I, which is a fission product in spent nuclear fuel, requires development of new durable host-materials.

Iodine is a very volatile chemical element, and even its chemically strong compounds such as AgI and CuI are not stable under ultraviolet irradiation or oxidizing conditions. Therefore, development of host materials for iodine immobilization is based on unusual approach – the search and testing of new compounds which were not studied before in respect of iodine sorption and strong fixation.

Although FCC material demonstrated high loading capacity to iodine sorption it is necessary to …

Evaluation Of Fluorapatite As A Waste-Form Material, Dennis W. Lindle, Oliver Hemmers, Dale L. Perry

Separations Campaign (TRP)

Argonne National Laboratory has proposed a new extraction procedure to handle TRISO-coated fuels, the Fluoride Extraction Process, or FLEX. The FLEX process is designed to separate the uranium in the fuel from the actinides and most fission products by taking advantage of the unique properties of uranium hexafluoride (UF₆). In the FLEX process, the used TRISO fuel is reacted with zirconium fluoride salt, forming UF₆ and the fluoride salts of the actinides and fission products. At process temperatures, the UF₆ volatizes into a gas, and is released from the molten salt mixture. This leaves behind the …

Development Of Fluorapatite As A Waste Form: Final Report #280204-1, Boris E. Burakov

Separations Campaign (TRP)

In the framework of Agreement #280204 (first year) it was necessary to review methods of apatite synthesis; identify optimal procedure of precursor preparation; obtain and study first fluorapatite samples. Although, some apatite-based ceramics were successfully synthesized using co-precipitated precursors and sintering method, there are still a lot of uncertainties related to optimal apatite doping with different radionuclides and non-radioactive elements. It is necessary to provide complete incorporation of waste elements into apatite crystalline structure avoiding formation of separate phases of radionuclides. Also, it is important to note that real waste streams might contain radionuclides with essentially different chemical features such …

Development Of Integrated Process Simulation System Model For Spent Fuel Treatment Facility (Sftf) Design, Yitung Chen, Sean Hsieh

Separations Campaign (TRP)

The major objective is to create a framework that combines all the strengths of AMUSE’s complicated calculations, well established commercial system process package such as ASPENPLUS, HYSYS and PRO/II and TRPSEMPro’s flexible parameter optimization modules. Development of the process simulation code can be done using the solvent extraction process experience at Argonne National Laboratory and in collaboration with the NCACM.

The major activities of the task are the following:

• Develop a framework for simulating the SFTF process using AMUSE code, commercial process package, such as ASPEN- PLUS, and system engineering model.
• Develop a middleware package that can communicate between the …

Electrochemical Separation Of Curium And Americium, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

The objective of this project is to use electrochemical techniques to develop a thermodynamic understanding of actinide and lanthanide species in aqueous solution and use this data to effectively separate species with very similar chemical properties. In consultation with our DOE collaborator, electrochemical methods and materials will be evaluated and used to exploit the thermodynamic differences between similar chemical species enhancing our ability to selectively target and sequester individual species from mixtures.

The following were specific goals for this year:

• To develop a fundamental understanding of the thermodynamic properties of actinide and lanthanide species such as Cm, Am, Ce, Nd, …

Fundamental Chemistry Of U And Pu In The Tbp-Dodecane-Nitric Acid System: Quarterly Report, Kenneth Czerwinski, Cynthia-May Gong, Amber Wright

Separations Campaign (TRP)

The speciation of hexavalent U and tetravalent Pu will be examined in the TBPdodecane- nitric acid systems. This topic is chosen based on data needs for separation modeling identified by the AFCI. Emphasis will be placed on studying the influence of nitrate and acetohydroxamic acid on U and Pu speciation as well as conditions where a third phase forms in the organic phase. The organic phase will be 30 % TBP in dodecane. Equal volumes of aqueous and organic phase will be used. The speciation of the actinides in the aqueous and organic phase will be determined by a number …

Fundamental Chemistry Of U And Pu In The Tbp-Dodecane-Nitric Acid System, Kenneth Czerwinski, Byron Bennett

Separations Campaign (TRP)

The research objectives of this project are as follows:

• To determine the influence of nitrate on the speciation of U and Pu in the TBP-dodecane-nitric acid system. The aqueous and organic speciation of U and Pu are examined as a function of the nitric acid concentration, nitrate concentration (by the addition of NaNO₃), actinide ion concentration, temperature, and time.
• To determine the speciation of U and Pu with AHA in the presence and absence of TBP-dodecane organic phase. The aqueous and organic speciation of U and Pu are evaluated as a function of AHA concentration, metal ion concentration, …

Neutron Multiplicity Measurements Of Target/Blanket Materials, Denis Beller

Transmutation Sciences Physics (TRP)

To optimize the performance of accelerator-driven sub-critical (ADS) transmutation systems, engineers will need to design the system to operate with a neutron multiplication factor just less than that of a critical, or self-sustaining, system. This design criterion requires particle transport codes that instill the highest level of confidence with minimal uncertainty, because larger uncertainties in the codes require larger safety margins in the design and result in a lower efficiency of the ADS transmuter. For current design efforts in the U.S., a Monte Carlo particle transport code MCNPX is used to model neutron production and transport for spallation neutron systems. …

Corrosion Of Steel By Lead Bismuth Eutectic, John Farley, Allen L. Johnson, Dale L. Perry

Transmutation Sciences Materials (TRP)

There is an active international interest in lead-bismuth eutectic and similar liquid lead systems because of the relevance to the transmutation of nuclear waste, fast reactors, and spallation neutron sources.

Materials in these systems must be able to tolerate high neutron fluxes, high temperatures, and chemical corrosion. For lead bismuth eutectic (LBE) systems, there is an additional challenge because the corrosive behaviors of materials in LBE are not well understood. Most of the available information on LBE systems has come from the Russians, who have over 80 reactor-years experience with LBE coolant in their Alpha-class submarine reactors. The Russians found …

Environment-Induced Degradation And Crack-Growth Studies Of Candidate Target Materials, Ajit K. Roy

Transmutation Sciences Materials (TRP)

The primary objective of this task was to evaluate the effects of environmental and mechanical parameters on environment induced degradations of candidate target structural materials for applications in spallation-neutron-target systems. The materials selected for evaluation and characterization were martensitic stainless steels including Alloys HT-9, EP-823, and 422.

Accelerator-driven transmutation systems involve bombarding a target material such as molten lead-bismuth-eutectic (LBE) by a proton beam, thereby producing neutrons. The molten LBE target will be contained in a subsystem structural container made of a suitable material such as Alloys HT-9, EP-823, and 422. During the transmutation process, the target structural material may …

Modeling Corrosion In Oxygen Controlled Lbe Systems With Coupling Of Chemical Kinetics And Hydrodynamics, Samir Moujaes, Yitung Chen

Transmutation Sciences Materials (TRP)

The corrosion of structural materials is a major concern for the use of lead-bismuth eutectic (LBE) systems for nuclear applications such as in transmuter targets or fast reactors. Corrosion in liquid metal systems can occur through various processes, including, for example, dissolution, formation of inter-metallic compounds at the interface, and penetration of liquid metal along grain boundaries. Predicting the rate of these processes depends on numerous system operational factors: temperature, system geometry, thermal gradients, solid and liquid compositions, and velocity of the liquid metal, to name a few. Corrosion, along with mechanical and/or hydraulic factors, often contributes to component failure. …

Development Of A Mechanistic Understanding Of High-Temperature Deformation Of Alloy Ep-823, Ajit K. Roy, Brendan O'Toole

Transmutation Sciences Materials (TRP)

During the transmutation process, a significant amount of heat can be generated in a molten lead-bismuth-eutectic (LBE) target, which will be contained in a subsystem structural container made of a suitable martensitic iron-chromium-molbdenum (Fe-Cr-Mo) stainless steel such as Alloys EP-823, HT-9 and 422. These materials will be subjected to high tensile stresses while they are in contact with the molten LBE at temperatures ranging between 400 and 600^oC. Therefore, a research program was conducted to evaluate the deformation characteristics of all three alloys in properly heat-treated conditions at temperatures relevant to the operating conditions.

Developing A Sensing System For The Measurement Of Oxygen Concentration In Liquid Pb-Bi Eutectic, Yingtao Jiang, Bingmei Fu

Transmutation Sciences Materials (TRP)

Although liquid lead-bismuth eutectic (LBE) is a good candidate for the coolant that can be employed in a subcritical transmutation blanket, it is known to be very corrosive to stainless steel, the material used in the containment structure. To mitigate this problem, trace levels of oxygen can be introduced into the system, causing the formation of a protective oxide layer at the interface between the LBE and steel. The proper formation of this oxide layer largely depends on the accurate measurement and subsequent control of the oxygen concentration in liquid LBE.

Yttria Stabilized Zirconia (YSZ) oxygen sensors, using molten bismuth …

Use Of Positron Annihilation Spectroscopy For Stress-Strain Measurements, Ajit K. Roy

Transmutation Sciences Materials (TRP)

Engineering metals and alloys, when subjected to tensile loading beyond a limiting value, undergo plastic deformation resulting in lattice defects such as voids and dislocations. These imperfections interact with the crystal lattice, producing a higher state of internal stress, also known as residual stress, which can be associated with reduced ductility. Residual stresses are also generated in welded structures due to rapid solidification and resultant dissimilar metallurgical microstructures between the weld and the base metals. Development of these internal stresses is often influenced by incompatible permanent strain resulting from thermal and mechanical operations associated with welding and plastic deformation. These …