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At least 361 records · Page 20

Feasibility of an on-line fission-gas-leak detection system

Calculations were made to determine if a cladding failure could be detected in a 100-kW zirconium hydride reactor primary system by monitoring the highly radioactive NaK coolant for the presence of I-131. The system is to be completely sealed. A leak of 0.01 percent from a single fuel pin was postulated. The 0.364-MeV gamma of I-131 could be monitored on an almost continuous basis, while its presence could be varified by using a longer counting time for the 0.638-MeV gamma. A lithium-drifted germanium detector would eliminate radioactive corrosion product interference that could occur with a sodium iodide scintillation detector.

Lustig, P. H.↗

Computer Modeling of Transport of Oxidizing Species in Grain Boundaries during Zirconium Corrosion

Zirconium (Zr) based alloys are widely used as the cladding materials in light-water reactors. The water-side corrosion of these alloys degrades their structural integrity and poses serious safety concerns. During the Zr corrosion process, a thin Zr oxide (ZrO2) layer forms on the alloy surface and serves as a barrier layer for further corrosion. The majority of the oxide has the monoclinic phase. At the transition region between the oxide and the metal, the oxide contains a thin layer of stabilized tetragonal phase. It is found that the texture of the tetragonal layer determines the protectiveness of the oxide for corrosion. The transport of oxidizing species, such as anion defects, cation defects, and electron through the tetragonal oxide layer could be the rate limiting step of the corrosion. The defect diffusion can be affected by the growing stresses and microstructures such as grain boundaries and dislocations. In this work molecular dynamics simulations are used to investigate the anion and cation diffusion in bulk and at grain boundaries in tetragonal ZrO2. The results show that defect diffusion at grain boundaries is complex and the behavior strongly depends on the grain boundary type. For most of the grain boundaries studied the defect diffusion are much slower than in the bulk, implying that grain boundaries may not be fast defect transport paths during corrosion. The connection between the modeling results and published experimental work will also be discussed. This work is funded by the Laboratory Directed Research and Development (LDRD) program at Idaho National Laboratory.

36 MATERIALS SCIENCE↗

Biaxial Creep Behavior of Nb-Modified Zircaloys

Zirconium-niobium (Zr-Nb) alloys are used as cladding materials to encapsulate radioactive fuel in nuclear reactors. They possess excellent corrosion resistance at high temperatures making it possible to achieve high fuel burnup, directly increasing the thermal efficiency of the reactor. While they are commonly used in recrystallized (Rx) form in boiling water reactors, there is a need to understand the effect of cold work and stress relief (CWSR) on the biaxial creep characteristics of these materials due to their use in pressurized water reactors. In this study, the biaxial creep behaviors of as-received Zr-Nb alloys, HANA and Zirlo®, have been investigated at 500°C and 400°C, respectively, using internally pressurized tubing superimposed with axial load under varied hoop σθ to axial σz stress ratios of 0 to 2 while monitoring both the axial and hoop strains using a linear variable displacement transformer and a laser telemetric extensometer, respectively. The crystallographic textures and creep loci of these as-received Zr-Nb alloys have been evaluated to correlate with the previous studies on recrystallized HANA4 and CWSR Zircaloy-4. The creep locus of HANA4 was found to be unaffected by initial state (CWSR or Rx) and showed close correspondence to planar isotropy while the creep locus of CWSR Zirlo exhibited more resistance to axial deformation than diametrical as per CWSR Zircaloy-4 reported earlier. These differences are shown to arise from grain-shape anisotropy of the CWSR Zirlo and Zircaloy-4. The simulated creep loci using crystallite-orientation distribution functions in conjunction with prism slip models showed excellent agreement with experimental results.

Tillman, Micah↗

Raman spectroscopy of zirconium hydride

The characterization of zirconium hydride is important in the nuclear industry because of the hydrogen-induced embrittlement of Zircaloy cladding and its use as a neutron moderator. This paper introduces the use of Raman spectroscopy for the characterization of zirconium hydride. First-principles density functional theory (DFT) calculations were used to predict the Raman spectra of ζ-ZrH 0.5 , γ-ZrH, δ-ZrH 1.5 , δ-ZrH 1.66 , and ε-ZrH 2 with all their predicted symmetries; ζ-ZrH 0.5 (P3m1, R$\overline{3}$m, C2/m, Cm, Cmmm, and Pn$\overline{3}$m); γ-ZrH (P222, Ccce, and P4 2 /mmc); δ-ZrH 1.5 (P$\overline{4}$m2, P4 2 /mcm, Fmmm, Pn$\overline{3}$m, Ibam, P2/c, PI, and P4 2 /nnm); δ-ZrH 1.66 (Fm$\overline{3}$m); and ε-ZrH 2 (Fm$\overline{3}$m, R$\overline{3}$m, and I 4 /mmm). Two samples of Zircaloy-4 containing 133 wt ppm and 360 wt ppm hydrogen were characterized by Raman spectroscopy, showing two signal lines at 215 cm -1 and 1,187 cm -1 , which were assigned to the presence of δ-ZrH 1.66 . These signals had a good spatial correlation with visible hydride precipitates in Raman spectroscopy images. In conclusion, this work provides the basis for the characterization of all possible zirconium hydride compositions and structures using Raman spectroscopy.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Zirconium-based alloys, nuclear fuel rods and nuclear reactors including such alloys, and related methods

Zirconium-based metal alloy compositions comprise zirconium, a first additive in which the permeability of hydrogen decreases with increasing temperatures at least over a temperature range extending from 350.degree. C. to 750.degree. C., and a second additive having a solubility in zirconium over the temperature range extending from 350.degree. C. to 750.degree. C. At least one of a solubility of the first additive in the second additive over the temperature range extending from 350.degree. C. to 750.degree. C. and a solubility of the second additive in the first additive over the temperature range extending from 350.degree. C. to 750.degree. C. is higher than the solubility of the second additive in zirconium over the temperature range extending from 350.degree. C. to 750.degree. C. Nuclear fuel rods include a cladding material comprising such metal alloy compositions, and nuclear reactors include such fuel rods. Methods are used to fabricate such zirconium-based metal alloy compositions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Transmission Electron Microscopy Characterization of Fuel Cladding Chemical Interaction between Minor Actinides bearing U-Pu-Zr Fuel and AIM1 Cladding

Minor actinides (MA) significantly contribute to the long-term radiotoxicity of spent nuclear fuel (SNF). Separating MA from SNF and incorporating it into metallic fuels for fast reactor transmutation is a potential method to reduce this radiotoxicity. Here, this study focuses on transmission electron microscopy characterization of two samples from the fuel cladding chemical interaction (FCCI) region of an americium (Am) and neptunium (Np)-bearing (MA-bearing) uranium-plutonium-zirconium (U-Pu-Zr) fuel irradiated in the Phenix fast reactor to 9.5 % FIMA burnup at approximately 550 °C cladding temperature. The results show that despite the complex chemical interactions between MA and AIM1 cladding elements, excessive FCCI was not induced, and Am penetration depth in the cladding limited to less than 4 µm. Np remained mostly inside fuel. The Zr-rich compounds layer effectively limited the accumulation of lanthanide on the inner cladding surface. Overall, the FCCI behavior between investigated MA-bearing U-Pu-Zr fuel and AIM1 cladding is benign.

Chemical interaction↗

Interfacing VPSC with finite element codes. Demonstration of irradiation growth simulation in a cladding tube

This Milestone report shows good progress in interfacing VPSC with the FE codes ABAQUS and MOOSE, to perform component-level simulations of irradiation-induced deformation in Zirconium alloys. In this preliminary application, we have performed an irradiation growth simulation in the quarter geometry of a cladding tube. We have benchmarked VPSC-ABAQUS and VPSC-MOOSE predictions with VPSC-SA predictions to verify the accuracy of the VPSCFE interface. Predictions from the FE simulations are in general agreement with VPSC-SA simulations and also with experimental trends.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Advanced Low-Temperature Chlorination of Zirconium

Recovery of Zr from nuclear fuel is of high interest because the Zr cladding material comprises up to 50% of the high-level radioactive waste (HLW) that requires disposition. An ideal Zr-recovery process would not only recover the bulk Zr from the fuel or cladding but would also provide decontamination from the components that give rise to the HLW designation. A simplified decontamination pathway providing recovered Zr in compliance with low-level radioactive waste acceptance criteria could significantly reduce the burden of HLW requiring geologic disposition. A newly developed advanced low-temperature chlorination process presents an opportunity to recover a ZrCl4 product that is effectively decontaminated from the elements of concern. This advanced low-temperature chlorination process uses a mixture of the sulfur-containing chlorination compounds sulfur monochloride (S 2 Cl 2 ) and thionyl chloride (SOCl 2 ).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Annealing of (DU-10Mo)-Zr Co-Rolled Foils

Producing uranium-10wt% molybdenum (DU-10Mo) foils to clad with Al first requires initial bonding of the DU-10Mo foil to zirconium (Zr) by hot rolling, followed by cold rolling to final thickness. Rolling often produces wavy (DU-10Mo)-Zr foils that should be flattened before further processing, as any distortions could affect the final alignment and bonding of the Al cladding to the Zr co-rolled surface layer; this bonding is achieved by a hot isostatic pressing (HIP) process. Distortions in the (DU-10Mo)-Zr foil may cause the fuel foil to press against the Al cladding and thus create thinner or thicker areas in the Al cladding layer during the HIP cycle. Post machining is difficult and risky at this stage in the process since there is a chance of hitting the DU-10Mo. Therefore, it is very important to establish a process to flatten and remove any waviness. This study was conducted to determine if a simple annealing treatment could flatten wavy foils. Using the same starting material (i.e. DU-10Mo coupons of the same thickness), five different levels of hot rolling and cold rolling, combined with five different annealing treatments, were performed to determine the effect of these processing variables on flatness, bonding of layers, annealing response, microstructure, and hardness. The same final thickness was reached in all cases. Micrographs, textures, and hardness measurements were obtained for the various processing combinations. Based on these results, it was concluded that annealing at 650°C or higher is an effective treatment to appreciably reduce foil waviness.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Synchrotron micro-computed tomography analysis of neutron-irradiated U-Mo fuel

The three-dimensional (3D) microstructure of neutron-irradiated uranium-10 wt.% molybdenum (U-10Mo) fuel with a burn-up of 9.8 × 10 21 fissions/cm 3 was characterized using a novel, multi-modal synchrotron micro-computed tomography approach combining propagation-based phase-contrast enhanced and absorption contrast techniques. The porosity development, porosity interconnectedness, swelling, composition, local thickness of the zirconium (Zr) diffusion barrier, and the influence of the fuel–cladding interaction on the local composition and pore morphology, were uniquely determined in 3D. Two cuboids were produced using a focused ion beam-scanning electron microscope at the Zr diffusion barrier–fuel interface and in the bulk fuel. The bulk fuel sample swelled by 53.3 [+9.7/−3.1]%, while the fuel near the Zr–fuel interface swelled by 63.3 [+14.7/−7.2]%. The average local thickness of the Zr diffusion barrier decreased by 53 %, compared to the expected pre-irradiated thickness. Four pore morphology regions were identified initiating parallel to the fuel–Zr interaction region: (1) an interaction layer of suppressed porosity, (2) a layer of elongated and interconnected porosity, (3) a transition zone of low porosity, and (4) a layer of unoriented porosity representative of the bulk fuel behavior. The increase in porosity near the diffusion barrier corresponded to a higher U concentration compared to that in the bulk fuel. The interconnected porosity in the fuel near the diffusion barrier was extensive and oriented parallel to the diffusion barrier, while the bulk fuel had more compact and isolated pore networks. The interaction layer, despite having suppressed porosity, was nearly 100 wt.% U. Porosity suppression at the diffusion barrier corresponds to the expected reduction in radiation-driven diffusion of Xe at the interface despite the anticipated increase in fission product nucleation originating from a higher U concentration. In conclusion, the novel 3D insights of the porosity, swelling, and compositional variations characterized herein can improve the fidelity of fuel performance codes for proliferation-resistant fuels for research and test reactors.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Application of Phase Field Simulations to Fuel Behavior

The application of the phase filed method to simulate the formation and the stress induced re-orientation of zirconium hydride during dry storage of the spent fuel and clad assembly is discussed. The phase field technique is able to capture qualitatively the effect of external stress on the hydride orientation in Zr-H system. However, the modeling effort to-date is far from adequate and several issues remain to be addressed before the simulations can be used as a predictive tool for the behavior of the clad during long time dry storage.

elastic energy↗

UNCERTAINTIES FOR IN-REACTOR TESTING OF TRITIUM LOADED GETTERS WITH TEMPERATURE CONTROL

The fourth experiment in TPBAR Materials Irradiation Separate-Effects Test (TMIST) series (TMIST-4) is planned to experimentally determine the effect of neutron irradiation on the equilibrium vapor pressure of tritium over a tritium loaded Nickel-Plated Zirconium (NPZ) getter in a simulated TPBAR service environment. This pressure will be used to estimate the tritium permeation rate. In the thermal design in the TMIST-4, two evaluations are required. 1) The cladding temperature is calculated to estimate the feasibility of detecting potential irradiation enhancement of the partial pressure for an NPZ getter. This work is required to obtain a precise cladding temperature for measurement of a low tritium partial pressure. This work has been completed and indicated that the required/target cladding temperatures based on the TMIST-4 test plan can be satisfied under the test condition range by modifying the capsule component shapes and inserting a thermally conductive metal sleeve. 2) The evaluation of uncertainties associated with the test design and operation is performed. This includes fabrication tolerances, and power and nuclear operating conditions. These factors will impact the component temperatures inside capsules and resulting the tritium partial pressure. The tritium permeation rate is a function of temperature and tritium partial pressure. The prediction of tritium permeation rates affects the feasibility of obtaining measurement resolutions required to reach reasonable conclusion for potential irradiation enhanced performance. This work will investigate the uncertainties.

TTP, TPBAR, TMIST-4, TPBAR Materials Irradiation S↗

Microstructural characterization of as-fabricated monolithic plates with boron carbide, aluminum boride, and zirconium boride burnable absorbers

The use of burnable absorbers can be beneficial for nuclear reactors by extending the fuel’s operational cycle, providing additional criticality control, and flattening the power profile. In this work, three burnable absorber materials (boron carbide, aluminum boride, and zirconium boride) embedded in aluminum have been fabricated into foils and clad in AA-6061 for potential use in high performance research reactors. The as-fabricated boron-containing phases were determined using transmission electron microscopy to be AlB2, B4C, and ZrB2. TEM also revealed weak bonding at the B4C-matrix interface. SEM showed a relatively uniform spatial distribution of boron-containing phases for all the candidate materials. Higher porosity was observed in the foil containing ZrB2 in its as-rolled condition. The porosity in the ZrB2 foil was reduced by hot isostatic pressing. The size and shape distributions of the boron-containing phases were analyzed on the criteria of cross-sectional area, perimeter, roundness, circularity, and aspect ratio. A method of converting the 2D burnable absorber dispersoids seen in cross-sectional microscopy images into 3D volumes was derived using both spherical and ellipsoidal geometry models. The difference in calculated burnable absorber dispersoid average volume between the two models ranges from 20% to 100%, which could impact burnable absorber burnout rates due to differences in neutron self-shielding.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Compatibility of refractory materials for nuclear reactor poison control systems

Metal-clad poison rods have been considered for the control system of an advanced space power reactor concept studied at the NASA Lewis Research Center. Such control rods may be required to operate at temperatures of about 140O C. Selected poison materials (including boron carbide and the diborides of zirconium, hafnium, and tantalum) were subjected to 1000-hour screening tests in contact with candidate refractory metal cladding materials (including tungsten and alloys of tantalum, niobium, and molybdenum) to assess the compatibility of these materials combinations at the temperatures of interest. Zirconium and hafnium diborides were compatible with refractory metals at 1400 C, but boron carbide and tantalum diboride reacted with the refractory metals at this temperature. Zirconium diboride also showed promise as a reaction barrier between boron carbide and tungsten.

Sinclair, J. H.↗

Excitation Function Calculations of Neutron-Induced Reactions of Some Zirconium Target Isotopes

Nuclear structures with high performance materials will be critical for the success of future fusion energy. Zirconium alloys are extensively used for nuclear reactor core materials as fuel cladding and guide tubes due to excellent radiation and corrosion resistant properties. In this paper, the excitation functions of {sup 90}Zr(n,2n){sup 89}Zr, {sup 90}Zr(n,α){sup 87}Sr, {sup 91}Zr(n,p){sup 91}Y and {sup 92}Zr(n,p){sup 92}Y nuclear reactions were calculated for energies up to 25 MeV. Besides, ALICE/ASH and TALYS 1.6 codes were used for the cross section calculations. The obtained calculations were compared with the experimental data in the literature.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Metal Matrix Microencapsulated (M3) fuel neutronics performance in PWRs

Metal Matrix Microencapsulated (M3) fuel consists of TRISO or BISO coated fuel particles directly dispersed in a matrix of zirconium metal to form a solid rod (Fig. 1). In this integral fuel concept the cladding tube and the failure mechanisms associated with it have been eliminated. In this manner pellet-clad-interactions (PCI), thin tube failure due to oxidation and hydriding, and tube pressurization and burst will be absent. M3 fuel, given the high stiffness of the integral rod design, could as well improve grid-to-rod wear behavior. Overall M3 fuel, compared to existing fuel designs, is expected to provide greatly improved operational performance. Multiple barriers to fission product release (ceramic coating layers in the coated fuel particle and te metal matrix) and the high thermal conductivity zirconium alloy metal matrix contribute to the enhancement in fuel behavior. The discontinuous nature of fissile material encapsulated in coated particles provides additional assistance; for instance if the M3 fuel rod is snapped into multiple pieces, only the limited number of fuel particles at the failure cross section are susceptible to release fission products. This is in contrast to the conventional oxide fuel where the presence of a small opening in the cladding provides the pathway for release of the entire inventory of fission products from the fuel rod. While conventional metal fuels (e.g. U-Zr and U-Mo) are typically expected to experience large swelling under irradiation due to the high degree of damage from fission fragments and introduction of fission gas into the lattice, this is not the case for M3 fuels. The fissile portion of the fuel is contained within the coated particle where enough room is available to accommodate fission gases and kernel swelling. The zirconium metal matrix will not be exposed to fission products and its swelling is known to be very limited when exposed solely to neutrons. Under design basis RIA and LOCA, fuel performance will be superior to the conventional oxide fuel since PCMI and rod burst, respectively, have been mitigated. Under beyond design basis accident scenarios where the fuel is exposed to high temperature steam for prolonged periods, larger inventory of zirconium metal in the core could negatively affect the accident progression. A thin steam resistant layer (e.g. alumina forming alloy steel), integrated into the solid rod during fabrication by co-extrusion or hot-isostatic-pressing, offers the potential to provide additional fuel protection from steam interaction: blanketing under a range of boiling regimes and under severe accident conditions up to high temperatures well beyond what is currently possible in the conventional fuel. A crucial aspect to the viability of M3 fuel in light water reactors is the reduced heavy metal load compared to standard pellet fuel. This study evaluated the design requirements to operate a Pressurized Water Reactor (PWR) with M3 fuel in order to obtain fuel cycle length, reactivity coefficients, and power peaking factors comparable to that of standard fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Microanalysis of Irradiated Metallic Hydride Nuclear Fuel (U{sub 0.17}ZrH{sub 1.6})

Metallic hydride nuclear fuels (U{sub 0.17} ZrH{sub 1.6}) have been under consideration for use in Light Water Reactors (LWRs). The fuel matrix consists of isolated particles of uranium metal within a zirconium hydride matrix. Erbium was also added as a neutron poison enabling higher reactor performance. These fuels were encased in a Zircaloy-2 cladding with a Bi/Pb eutectic liquid metal filled-gap to improve thermal conductivity. The inner and outer cladding surfaces were oxidized to nominal 1 μm thickness to eliminate hydrogen attack. The fuels were termed UCB to note the location of fabrication as the University of California-Berkeley. Irradiations were performed in the MITR research reactor. The details are described elsewhere. We originally reported on post-irradiation analysis of the fuel elements of two of the rodlets using Scanning Electron Microscopy (SEM) and x-ray energy dispersive spectroscopy (EDS). In this further study, funded as a rapid turnaround experiment (RTE) through the Nuclear Science User Facilities (NSUF) program, we performed high-resolution Scanning Transmission Electron Microscopy (STEM) of thin lift-out specimens prepared from specific regions in the fuel matrix using an SEM-Focused Ion Beam (FIB) instrument, and again compared these results to the unirradiated material. Earlier investigations using SEM-EDS showed that ∼8% of the Zircaloy cladding had dissolved in the Pb-Bi eutectic during irradiation over 1000 hrs. However, the SEM-EDS failed to show any detectable evidence of damage of the fuel matrix. There was no obvious swelling or migration of elements; hence, we focused on these specific regions in greater detail. Much of the data on hydride fuels come from the Space Nuclear Auxiliary Power (SNAP) program from the 1960's. The principle difference between oxide and hydride fuel is the high thermal conductivity of the latter. This feature greatly decreases the temperature drop over the fuel during operation, thereby reducing the release of fission gases to the fraction due only to recoil. However, very unusual early swelling due to void formation around the uranium metal particles has been reported in hydride fuels over 700 deg. C. In this investigation, the fuel did not reach these extreme temperatures. Phases formed in this system have been previously experimentally investigated using thermal analysis techniques, and wavelength and energy dispersive spectroscopy (EDS/WDS) in scanning electron microscopes (SEM). Major changes were observed in the liquid metal and cladding components but at the scale of the SEM observations, it was not readily apparent that any major changes had occurred to the fuel matrix (i.e. U metal particles in the zirconium hydride matrix with interdispersed erbium metal). Rapid oxidation of the SEM mechanically polished cross-sections, may have obscured our ability to see major changes. By using the SEM-FIB slices, it was possible to remove oxide coatings and the smoother surfaces were found to be less susceptible to oxidation once removed from the vacuum chamber. The high spatial resolution of STEM allowed characterization of individual matrix phases.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗