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This is a NEAMS milestone report for the subcontract to PennState U on modeling hydride formation and evolution in Zr based cladding.
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The U.S. Department of Energy Office of Nuclear Energy, Office of Fuel Cycle Technology established the Used Fuel Disposition Campaign (UFDC) to conduct research and development activities related to storage, transportation, and disposal of used nuclear fuel (UNF) and high-level radioactive waste. Within the UFDC, the storage and transportation task has been created to address issues of extended storage and transportation. One gap in knowledge identified as high priority by UFDC includes hydrogen effects in zirconium alloy cladding and reorientation of cladding hydrides. During reactor operations, hydrogen is generated from the oxidation of the surface of zirconium alloy materials in the coolant of light water reactors can be absorbed into the cladding and form zirconium hydrides. At high temperatures and hoop stresses, these normally circumferential oriented hydrides in high burnup UNF (HB-UNF) may reorient in the radial direction and affect the mechanical properties of the cladding. Understanding these changes in mechanical properties will aid in analyzing how UNF will perform during storage and transportation. Separate effects testing to measure the mechanical properties of un-hydrided, pre-hydrided, and irradiated HB-UNF is currently underway at Pacific Northwest National Laboratory (PNNL). In order to measure these mechanical properties, staff at PNNL are employing tensile, compression, and burst testing. Systems have been developed to pre-hydride cladding and reorient cladding hydrides. The development of these systems and the testing methods are described herein.
The motivation for transitioning away from zirconium-based fuel cladding in light water reactors to significantly more oxidation-resistant materials, thereby enhancing safety margins during severe accidents, is laid out. A review of the development status for three accident tolerant fuel cladding technologies, namely coated zirconium-based cladding, ferritic alumina-forming alloy cladding, and silicon carbide fiber–reinforced silicon carbide matrix composite cladding, is offered. Technical challenges and data gaps for each of these cladding technologies are highlighted. Full development towards commercial deployment of these technologies is identified as a high priority for the nuclear industry.
The Consortium for the Advanced Simulation of Light Water Reactors (CASL), the first Energy Innovation Hub of the Department of Energy, was established in 2010 with the goal of providing modeling and simulation (M&S) capabilities that support and accelerate the improvement of nuclear energy's economic competitiveness and the reduction of spent nuclear fuel volume per unit energy, and all while assuring nuclear safety. To accomplish this requires advances in M&S capabilities in radiation transport, thermal-hydraulics, fuel performance and corrosion chemistry. To focus CASL's R&D, industry challenge problems have been defined, which equate with long standing issues of the nuclear power industry that M&S can assist in addressing. To date CASL has developed a multi-physics “core simulator” based upon pin-resolved radiation transport and subchannel (within fuel assembly) thermal-hydraulics, capitalizing on the capabilities of high performance computing. CASL's fuel performance M&S capability can also be optionally integrated into the core simulator, yielding a coupled multi-physics capability with untapped predictive potential. Material models have been developed to enhance predictive capabilities of fuel clad creep and growth, along with deeper understanding of zirconium alloy clad oxidation and hydrogen pickup. Understanding of corrosion chemistry (e.g., CRUD formation) has evolved at all scales: micro, meso and macro. CFD R&D has focused on improvement in closure models for subcooled boiling and bubbly flow, and the formulation of robust numerical solution algorithms. For multiphysics integration, several iterative acceleration methods have been assessed, illuminating areas where further research is needed. Finally, uncertainty quantification and data assimilation techniques, based upon sampling approaches, have been made more feasible for practicing nuclear engineers via R&D on dimensional reduction and biased sampling. Industry adoption of CASL's evolving M&S capabilities, which is in progress, will assist in addressing long-standing and future operational and safety challenges of the nuclear industry. - Highlights: • Complexity of physics based modeling of light water reactor cores being addressed. • Capability developed to help address problems that have challenged the nuclear power industry. • Simulation capabilities that take advantage of high performance computing developed.
An engineering effort is underway to re-establish capability to produce 238Pu oxide at the kilogram scale in the United States. A multi-step batch process is being developed to produce this important material. Recently, a portion of this process was studied using discrete-event simulation tools to determine whether the conceptual process might achieve its yearly production goal. The study showed the conceptual process can meet the yearly production goal under some circumstances, but process improvements would be needed to ensure greater likelihood of success. This study extends the work performed previously by examining the effects of changing the reactor target design on the yearly process output. Two new reactor target configurations are considered an aluminum-clad reactor target containing 50% greater 237Np oxide content than the original target, and a zirconium alloy-clad target using no aluminum. The results indicate that use of the new aluminum-clad target configuration may allow the process to achieve the same yearly production goal in less time using fewer targets. If the zirconium alloy-clad target is used, then even fewer targets would be needed to reach the production goal, but some process changes would be required to handle the zirconium cladding. The number of days needed to process a target batch to completion, and the steady state 238Pu oxide production rate, for each configuration are compared to the results from the initial simulation study.
Zirconium-based cladding materials that surround used nuclear fuel (UNF) rods represent a significant fraction of the total amount of high level waste that must be disposed of in long term geological repositories. The decontamination, recovery and reuse of these materials would significantly reduce the high level waste associated with light water reactors and could provide a new source of hafnium free zirconium for the fabrication of new nuclear components. One part in the strategy to recycle zirconium from used cladding materials involves developing a computational modeling (DFT) protocol to understand the reactions between ZrCl{sub 4} and metal chloride impurities that may occur in the gas phase during sublimation. Several of the metal chloride species present are known to form Lewis acid/base adducts in the gas phase and development of purification protocols require investigation into the properties of these ZrCl{sub 4} contaminates.
In this paper, accident-tolerant fuel (ATF) cladding materials aim to improve fuel reliability and safety during accident scenarios in water-cooled reactors. These ATF cladding should also perform comparable or better than the current zirconium alloy cladding under reactor normal operating conditions. Surface-modified Zircaloy-4 was produced by depositing a protective coating of chromium by two different coating techniques, Physical Vapor Deposition (PVD) and Cold Spray (CS). The coating thickness, structure, composition, and mechanical properties of the coated Zircaloy were assessed with advanced materials characterization techniques. Results showed a strengthening effect of the Cr-coating, along with ~83% higher hardness compared to that of the Zircaloy-4 substrate. Surface topography and surface chemistry of the Cr-coated Zircaloy-4 were assessed with contact profilometry, atomic force microscopy, contact angle goniometry, and X-ray photoelectron spectroscopy. Deposited Cr-coating significantly improved surface wettability compared to the substrate Zircaloy-4. The formation of surface oxides on the coatings by prolonged exposure to ambient air showed a further increase in the hydrophobic behavior. Surface parameters and surface chemistry after flow boiling critical heat flux tests, conducted at atmospheric pressure, evidenced a slight increase in surface roughness with notable changes in wettability associated with the formation of surface oxides.
This report highlights accident-tolerant fuel (ATF) code assessment activities performed under Project NRCHQ- 60-17-T-0017, Lattice Physics Enhancements and Assessment. ATF covers a broad range of advanced fuel and clad designs for light water reactors (LWRs) to enhance performance under several accident conditions. Several ATF concepts are anticipated to be deployed as lead test rods (LTRs) or lead test assemblies (LTAs) within the next five years. The purpose of this work is to assess the predictive capabilities of NRC neutronics codes that underpin various licensing calculations. ATF designs use different fuel and clad materials compared to standard UO 2 fuel and zirconium-alloy claddings (hereafter UO 2 -Zry). These new materials and geometrical designs need to be assessed to quantify the impact of nuclear data uncertainties on quantities of interest (QOIs) in licensing calculations and the impact of modeling approximations which may be valid for UO 2 -Zry but not for ATF. This report outlines a systematic approach for ATF neutronics code assessment which includes sensitivity and uncertainty (S/U) analysis of nuclear data, identification of experimental benchmark and gaps for code validation, investigation of modeling approximations, and code-to-code comparisons of calculated QOIs against high-fidelity reference continuous energy (CE) Monte Carlo (MC) calculations. This report focuses on the assessment of the SCALE/Polaris lattice physics code for reactor safety analysis. Polaris lattice physics calculations generate few group (FG) cross sections for PARCS full-core calculations. (Full-core analysis, spent fuel analysis, and severe accident analysis will be performed in future work.) The selected ATF concepts for this report include Cr 2 O 3 and Al 2 O 3 -Cr 2 O 3 -doped UO 2 fuel, U 3 Si 2 fuel, FeCrAl cladding, SiC cladding, and Cr-coated cladding.
New sulfur chloride compounds—sulfur monochloride (S 2 Cl 2 ) and thionyl chloride (SOCl 2 )—have been proposed as alternative chlorinating agents for the chemical decladding of zirconium-based used nuclear fuel cladding materials. However, the radiation stability of these compounds has not been thoroughly evaluated, despite envisioned process conditions involving intense, multi-component radiation fields. Knowledge of the radiation chemistry of these sulfur chlorides is essential for the development and optimization of alternative chlorination technologies. To this end, we present preliminary findings on the gamma radiolysis of neat S 2 Cl 2 and SOCl 2 at ambient temperature up to ~ 34 MGy. In this study, Raman spectroscopy and density functional theory calculations were used to identify the Raman-active degradation products from S 2 Cl 2 and SOCl 2 radiolysis. Both sulfur chloride compounds exhibited significant radiation resistance, with respect to changes in the Raman signatures of the parent compounds and the ingrowth of Raman-active degradation products. For S 2 Cl 2 , molecular chlorine (Cl 2 ) was directly identified as the predominant degradation product, which was completely consumed at higher absorbed doses (> 9 MGy). Similarly, the main degradation product from SOCl 2 radiolysis was also Cl 2 , although in this system it continued to grow in with dose over the entire dose range. Further, an “S=O” containing degradation product(s) was also identified as a compliment to Cl 2 . Overall, the perceived radiation resistance of these sulfur chloride compounds makes them suitable for inclusion in a used nuclear fuel chemical decladding process, especially as radiolytically formed Cl 2 can be used to reform the parent compounds, thereby increasing the longevity of the solvents used.
It is expected that tritium pretreatment will be required in future reprocessing plants to prevent the release of tritium to the environment (except for long-cooled fuels; >30 yrs). To design and operate future reprocessing plants in a safe and environmentally compliant manner, the amount and form of tritium in the used nuclear fuel (UNF) must be understood and quantified. Tritium in light water reactor (LWR) fuel is dispersed between the fuel matrix and the fuel cladding, and some tritium may be in the plenum, probably as tritiated water (THO or T{sub 2}O). In a standard processing flowsheet, tritium management would be accomplished by treatment of liquid streams within the plant. Pretreating the fuel prior to dissolution to release the tritium into a single off-gas stream could simplify tritium management, so the removal of tritium in the liquid streams throughout the plant may not be required. The fraction of tritium remaining in the cladding may be reduced as a result of tritium pretreatment. Since Zircaloy'R cladding makes up roughly 25% by mass of UNF in the United States, processes are being considered to reduce the volume of reprocessing waste attributed to Zircaloy'R clad fuel by recovering the zirconium from the cladding for reuse. Treatment options for Zircaloy cladding include recycling to recover the significant value of the zirconium and eliminate costs associated with the disposal of transuranic-contaminated Zircaloy. If LWR fuel is reprocessed and the fuel is dissolved without tritium pretreatment, the tritium in the cladding will remain bound to the cladding. If tritium pretreatment is included in the flow sheet, some portion of the tritium in the cladding may be released along with the tritium from the fuel matrix. To design and operate reprocessing plants in a safe and environmentally compliant manner, the amount and form of tritium in the UNF must be understood and quantified. For Zircaloy-clad fuels from light water reactors, the tritium produced from ternary fission and other sources is expected to be divided between the fuel, where it is generated, and the cladding. It has been previously documented that a fraction of the tritium produced in uranium oxide fuel from LWRs can migrate and become trapped in the cladding. Estimates of the percentage of tritium in the cladding typically range from 0-96%. There is relatively limited data on how the tritium content of the cladding varies with burnup and fuel history (temperature, power, etc.) and how pretreatment impacts its release. The present study was undertaken to understand how tritium pretreatment at standard tritium pretreatment conditions (oxidation in air at 480 to 600 deg. C) affects the tritium content in the Zircaloy cladding and the extent to which the tritium content could be reduced with modest increases in the tritium pretreatment temperature. The data indicate that <20% of the tritium in PWR cladding will be removed by pretreatment at 500-700 deg. C for 24 h. Essentially 100% of the tritium will likely be released if the heating time at 700 deg. C is extended to 96 h. Small amounts of tritium are expected to be released if the cladding is heated at ≤ 600 deg. C for up to 96 h. The results of this study indicate that the amount of tritium released from tritium pretreatment systems will be dependent on both the operating temperature and length of time in the pretreatment system. Under certain conditions, a significant fraction of the tritium could remain bound in the cladding and would need to be considered in any subsequent processing of the cladding to recover/recycle the zirconium. (authors)
A continuum model for calculating the time-dependent hydrogen pickup fractions in various Zirconium alloys under steam and pressured water oxidation has been developed in this paper. Using only one fitting parameter, the effective hydrogen gas partial pressure at the oxide surface, a qualitative agreement is obtained between the predicted and previously measured hydrogen pickup fractions. The calculation results therefore demonstrate that H diffusion through the dense oxide layer plays an important role in the hydrogen pickup process. Finally, the limitations and possible improvement of the model are also discussed.
The adsorption of atomic and gaseous chlorine on Zr (0001) surface has been investigated using state-of-the-art density functional theory calculations as part of an effort to gain fundamental understanding of chlorination processes occurring in fuel cladding materials. Zirconium alloys, including Zircaloy-4, Zircaloy-2 and Zr-Nb alloys (Zirlo{sup TM} and Zr-2.5Nb) are the most common fuel cladding materials in nuclear light water reactors (LWRs) due to their favorable mechanical properties, corrosion resistance, low thermal-neutron capture cross section and criticality. The United States produces a large amount of cladding material from used nuclear fuel, which could approach 1,000 MT/year in the next 50 years. In nuclear fuel recycling, spent nuclear fuel assemblies are disassembled and the cladding hulls are separated from the U oxide spent fuel. Zr can be recovered from Zr cladding using the chlorination method. However the presence of impurities in the recovered ZrCl{sub 4} was reported, including Sn, Cr and Fe. Thus, further efforts are necessary to improve the purification process significantly. This requires fundamental understanding of chlorination processes in cladding materials. Most of the material properties are expected to be similar between the pure zirconium and its alloys due to the fact that the alloy composition consists of more than 95 weight-percent zirconium and less than 2% of tin, niobium, iron, chromium, nickel and other metals. Therefore, while the overarching goal is to understand the chlorination process occurring in complex fuel cladding materials, chlorination of pure zirconium was used as an initial system for the modeling and simulation efforts in this study.
During the initial feasibility test using actual used nuclear fuel (UNF) cladding in FY 2012, an incubation period of 30–45 minutes was observed in the initial dry chlorination. The cladding hull used in the test had been previously oxidized in a dry air oxidation pretreatment prior to removal of the fuel. The cause of this incubation period was attributed to the resistance to chlorination of an oxide layer imparted by the dry oxidation pretreatment on the cladding. Subsequently in 2013, researchers at the Korea Atomic Energy Institute (KAERI) reported on their chlorination study [R1] on ~9-gram samples of unirradiated ZirloTM cladding tubes that had been previously oxidized in air at 500oC for various time periods to impart oxide layers of varying thickness. In early 2014, discussions with Indefinite Delivery, Indefinite Quantity (IDIQ) contracted technical consultants from Westinghouse described their previous development (and patents) [R2] on methods of chemical washing to remove some or all of the hydrous oxide layer imparted on UNF cladding during irradiation in light water reactors (LWRs) . Thus, the Oak Ridge National Laboratory (ORNL) study, described herein, was planned to extend the KAERI study on the effects of anhydrous oxide layers, but on larger ~100-gram samples of unirradiated zirconium alloy cladding tubes, and to investigate the effects of various methods of chemical pretreatment prior to chlorination with 100% chlorine on the average reaction rates and Cl2 usage efficiencies.
Short communication on the completion and testing of a new high-temperature cell holder to support high dose rate electron beam irradiations of select sulfur chlorides (S2Cl2 and SOCl2) for advanced low temperature chlorination of zirconium-based used nuclear fuel cladding.
Secondary hydriding can take place during a loss-of-coolant accident event after the ballooning and burst of the zirconium alloy cladding. The oxidation and hydrogen uptake in the ballooned section can produce the weakest segment of the rod. This phenomenon was investigated in the past mainly for Zircaloy-4 cladding. We investigated the effect of secondary hydriding in VVER reactors with E110 and E110G alloys. A high-temperature facility was built to carry out high-temperature treatment of fuel cladding samples. The burst of tubes was reached with inner pressurization at 750 and 800 C. After burst the samples were oxidized in the same furnace for different periods and at different temperatures. The oxidized samples were tested in a tensile test machine with four-point bending tests. The microstructure of the samples was analyzed by optical and scanning electron microscopy. The hydrogen content of the cladding was measured by heat extraction, prompt gamma activation analyses, and neutron radiography methods. The experiments indicated that the ballooned section after oxidation became the weakest segment of the VVER fuel. According to the mechanical testing, the cladding samples were brittle even after a short oxidation time (200 s at 1,000 C) without any sign of ductile behavior. The comparison of E110 and E110G samples showed that the E110 tubes lost their load-bearing capability or even integrity much earlier than the E110G samples treated under similar conditions. (authors)
Accident tolerant materials are defined as those that provide significantly increased response time in the event of an accident while providing similar or improved performance as the conventional UO2/Zircaloy-4 fuel rods during normal operation. One avenue for materials to demonstrate enhanced accident tolerance is to have improved reaction (e.g., oxidation) kinetics with steam, resulting in slower hydrogen (or other combustible gases) generation rate, while maintaining acceptable thermo-mechanical properties, fuel-clad interactions, and fission product behavior. Due to their improved reaction kinetics with steam compared to Zircaloy-4, iron-chromium-aluminum (FeCrAl) alloys are being considered as an accident tolerant cladding material. In order to determine whether FeCrAl alloys are indeed accident tolerant materials, comparisons between conventional zirconium-based claddings under accident conditions is required. To this end, we have developed a burst (failure) criterion for FeCrAl using existing experimental data for first-generation alloys. This model was incorporated into the BISON fuel performance code to perform comparative studies with Zircaloy-4 cladding tubes under non-oxidizing and oxidizing LOCA conditions. The separate effects LOCA conditions considered were adopted from the PUZRY and REBEKA test series. Due to the fact that FeCrAl alloys have a larger thermal absorption cross-section and higher stiffness than Zircaloy-4, cladding thickness will be smaller for FeCrAl than for Zircaloy-4. Three different cladding thicknesses were analyzed in this work. The results indicate that for both non-oxidizing (PUZRY) and oxidizing (REBEKA) LOCA conditions, FeCrAl has similar burst behavior (i.e., time to burst and pressure at burst) as Zircaloy-4. It should be noticed that this study used data for first-generation FeCrAl alloys to develop the burst criterion. Although no burst data?currently exists for C35M (a second-generation FeCrAl alloy under development at Oak Ridge National Laboratory), improved burst behavior is anticipated. As burst data for C35M becomes available the burst criterion will be updated and the simulations revisited to determine the accident tolerance of second-generation FeCrAl alloys.
Accident tolerant materials are defined as those that provide significantly increased response time in the event of an accident while providing similar or improved performance as the conventional UO2/Zircaloy-4 fuel rods during normal operation. One avenue for materials to demonstrate enhanced accident tolerance is to have improved reaction (e.g., oxidation) kinetics with steam, resulting in slower hydrogen (or other combustible gases) generation rate, while maintaining acceptable thermo-mechanical properties, fuel-clad interactions, and fission product behavior. Due to their improved reaction kinetics with steam compared to Zircaloy-4, iron-chromium-aluminum (FeCrAl) alloys are being considered as an accident tolerant cladding material. In order to determine whether FeCrAl alloys are indeed accident tolerant materials, comparisons between conventional zirconium-based claddings under accident conditions is required. To this end, we have developed a burst (failure) criterion for FeCrAl using existing experimental data for first-generation alloys. This model was incorporated into the BISON fuel performance code to perform comparative studies with Zircaloy-4 cladding tubes under non-oxidizing and oxidizing LOCA conditions. The separate effects LOCA conditions considered were adopted from the PUZRY and REBEKA test series. Due to the fact that FeCrAl alloys have a larger thermal absorption cross-section and higher stiffness than Zircaloy-4, cladding thickness will be smaller for FeCrAl than for Zircaloy-4. Three different cladding thicknesses were analyzed in this work. The results indicate that for both non-oxidizing (PUZRY) and oxidizing (REBEKA) LOCA conditions, FeCrAl has similar burst behavior (i.e., time to burst and pressure at burst) as Zircaloy-4. It should be noticed that this study used data for first-generation FeCrAl alloys to develop the burst criterion. Although no burst data?currently exists for C35M (a second-generation FeCrAl alloy under development at Oak Ridge National Laboratory), improved burst behavior is anticipated. As burst data for C35M becomes available the burst criterion will be updated and the simulations revisited to determine the accident tolerance of second-generation FeCrAl alloys.