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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Generation of the TSL for Zirconium Hydrides from Ab Initio Methods

Zirconium hydride (ZrHx) is a moderator material used in TRIGA and other reactors that may exist in multiple phases with varying stoichiometry, which include the δ phase and the ϵ phase. Current ENDF/B-VIII.0 ZrHx thermal scattering law (TSL) evaluations do not distinguish between phases. These sub-libraries were generated with the LEAPR module of NJOY using historic phonon spectra derived from a central force model and assume incoherent elastic scattering for both bound hydrogen and zirconium, which neglects the effects of crystal structures important for scattering from zirconium bound in ZrHx. In this work, the TSLs for hydrogen and zirconium bound in δ-ZrHx and ϵ-ZrH2 were generated from phonon spectra derived from modern ab initio lattice dynamics methods and ab initio molecular dynamics. Subsequently, TSLs for hydrogen and zirconium in ZrHx and ZrH2 were generated using the Full Law Analysis Scattering System Hub (FLASSH) code. The built-in generalized coherent elastic routine was used to generate the previously neglected elastic contribution from zirconium for this material. The present TSLs provide both a re-evaluation of the current ZrH sub-libraries and expansion of the set of TSLs available for the examination of neutrons in systems with zirconium hydride, permitting explicit treatment of δ and ϵ phases.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2018

Synchrotron X-ray diffraction study of zirconium hydride distribution in Zr-2.5%Nb and its redistribution during thermal cycling

Highlights: • Differently oriented grains were studied in situ using synchrotron diffraction. • The effect of thermo-mechanical history on hydrogen location in α-Zr is considered. • Hydrogen redistribution in alpha-Zr matrix during thermal cycling discussed. - Abstract: Hydride distribution in a dual-phase hydrided Zr-2.5wt%Nb has been studied. Samples having different prior thermo-mechanical processing history were thermally cycled within a 86 keV X-ray photon beam. The diffraction patterns generated with this technique allow the evaluation of the relative quantity of hydrides within differently oriented grain sets. It was found that hydrides exist primarily within two different α-Zr grain-sets. One grain-set has its {0002} α-Zr direction oriented very close to the hoop direction while the other exists within a plane approximately 20° away from it. During thermal cycling, the proportion or hydrides oriented within different grain sets was shown to change from the distribution associated with the prior thermomechanical processing, to that corresponding to the current thermal cycling conditions. It was also shown that the ability for hydrogen to redistribute in the matrix correlates with the cooling rate of the specimen.

36 MATERIALS SCIENCE↗
DOE OSTI2024

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↗
DOE OSTI2020

Stability of zirconium hydride

This reports complete Milestone M2.2.1 Stability of zirconium hydride: Experimental investigation of the hydrogen concentration of encapsulated zirconium hydride before and after joining. In this milestone, we first report the successful fabrication of crack-free bulk zirconium hydride by using the ORNL static hydriding system. The fabricated hydride was characterized by using X-ray diffraction (XRD) and X-ray computed tomography (XCT). XRD results showed that the δ-phase zirconium hydride, α-zirconium, and ε-phase hydride were present. XCT confirmed the absence of the internal cracking. The hydrogen concentration was determined by the weight change before and after hydrogen loading, given the fact that the oxide phase was not found during XRD analysis. Two metallic cladding materials, i.e., molybdenum and FeCrAl, were selected to encapsulate the fabricated zirconium hydride pellets. Demonstration capsules were designed and machined. Mo crucible was successfully sealed by using a combination of electron beam welding and gas tungsten arc welding. Due to the undesired neutronics property of Mo, further investigation of this cladding material was not pursued. Electron beam welding and laser beam welding were employed to seal the FeCrAl capsules. XRD were performed on the zirconium hydride before and after the sealing. The results showed that the welding process has negligible impact on the hydrogen content in the FeCrAl-canned zirconium hydride. The presented work fulfilled the proposed work under this milestone and paves a pathway to fabricate single-phase zirconium hydride and to develop robust cladding materials to can bulk zirconium hydride.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Nanoindentation study of bulk zirconium hydrides at elevated temperatures

Here, the mechanical properties of zirconium hydrides was studied using nano-indentation technique at a temperature range of 25 – 400 °C. Temperature dependency of reduced elastic modulus and hardness of δ- and ε-zirconium hydrides were obtained by conducting nanoindentation experiments on the bulk hydride samples with independently heating capability of indenter and heating stage. The reduced elastic modulus of δ-zirconium hydride (H/Zr ratio =1.61) decreased from ~113 GPa to ~109 GPa while temperature increased from room temperature to 400°C. For ε-zirconium hydrides (H/Zr ratio=1.79), the reduced elastic modulus decreased from 61 GPa to 54 GPa as temperature increased from room temperature to 300 °C. Whereas, hardness of δ-zirconium hydride significantly decreased from 4.1 GPa to 2.41 GPa when temperature increased from room temperature to 400 °C. Similarly, hardness of ε-zirconium hydride decreased from 3.06 GPa to 2.19 GPa with temperature increase from room temperature to 300°C.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Non-equilibrium molecular dynamics studies of thermal diffusion of hydrogen isotopes in low concentration zirconium hydrides

Tritium permeability in zirconium-based tritium getter critically impacts tritium storage and environmental safety during operation of tritium-producing burnable absorber rods (TPBARs). Previous experiments indicated that during irradiation operation, the hydrogen equilibrium pressured is increased. Further experimental and modeling studies suggested that the enhanced tritium release observed for reactor scale assemblies might be related to a thermal diffusion known as the Soret effect. A direct measurement of the Soret factor, however, has not been performed. To improve TPBAR and other nuclear applications, here we have applied two non-equilibrium molecular dynamics methods to study thermal diffusion of hydrogen isotopes in low-concentration zirconium hydrides. One of the methods produces sufficiently converged results to distinguish crystal orientation, isotope type, and concentration effects. In conclusion, with this method, crystal orientation, isotope type, and concentration effects are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Comparative Critical Mass Calculations for NNL and ENDF/B-VIII.0 Zirconium Hydride Thermal Neutron Scattering Laws

Zirconium hydride (ZrH x ) is a moderator material for TRIGA reactors and historical space reactor systems, such as SNAP-10A. Thermal neutron scattering laws (TSL) for two phases of this material, δ and ε, have been previously evaluated by Naval Nuclear Laboratory (NNL) and submitted to the National Nuclear Data Center (NNDC) for inclusion in the US national ENDF/B-VIII.1 nuclear data library. In contrast to the current ENDF/B-VIII.0 TSL evaluations, which consider only a single phase, the new evaluations are derived from separate ab initio calculations for both phases and include coherent elastic effects of the zirconium sublattice. To estimate the impact of these changes to the TSL evaluation of this material, comparative critical mass calculations were performed with MC21 for homogenous mixtures of high- enriched uranium (HEU) and ZrH x in bare and water reflected sphere configurations. These calculations yield an impact on the estimated critical mass as a function of 235 U loading density with maximum differences as large as 1% - 5% for over-moderated thermal spectrum systems. Consequently, the NNL TSL evaluations are anticipated to have a small impact on criticality calculations of thermal reactor systems regardless of the material phase. Nevertheless, characteristic differences exist in the predicted thermal spectra as function of energy for the two sets of TSL evaluations, which are attributed to difference in the underlying phonon density of states of hydrogen bound in ZrH x .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Comparative critical mass calculations for NNL and ENDF/B-VIII.0 - Zirconium hydride thermal neutron scattering laws

Zirconium hydride (ZrH{sub x}) is a moderator material for TRIGA reactors and historical space reactor systems, such as SNAP-10A. Thermal neutron scattering laws (TSL) for two phases of this material, δ and ε, have been previously evaluated by Naval Nuclear Laboratory (NNL) and submitted to the National Nuclear Data Center (NNDC) for inclusion in the US national ENDF/B-VIII.1 nuclear data library. In contrast to the current ENDF/B-VIII.0 TSL evaluations, which consider only a single phase, the new evaluations are derived from separate ab initio calculations for both phases and include coherent elastic effects of the zirconium sublattice. To estimate the impact of these changes to the TSL evaluation of this material, comparative critical mass calculations were performed with MC21 for homogenous mixtures of high-enriched uranium (HEU) and ZrH{sub x} in bare and water reflected sphere configurations. These calculations yield an impact on the estimated critical mass as a function of {sup 235}U loading density with maximum differences as large as 1% - 5% for over-moderated thermal spectrum systems. Consequently, the NNL TSL evaluations are anticipated to have a small impact on criticality calculations of thermal reactor systems regardless of the material phase. Nevertheless, characteristic differences exist in the predicted thermal spectra as function of energy for the two sets of TSL evaluations, which are attributed to difference in the underlying phonon density of states of hydrogen bound in ZrH{sub x}. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Technology Enabling Zero-EPZ Micro Modular Reactors: Fabrication of Zirconium Hydride with Controlled Hydrogen Loading

This report completes Milestone M2.2.2 - ZrH pellet fabricated with controlled hydride loading: ZrH1.5±0.1 single phase pellets fabricated with controlled and thermally stable hydride loading. Hydrogen content to be quantified and single-phase confirmed by X-ray diffraction. In this milestone, we report the successful fabrication of delta-phase zirconium hydride pellets using the ORNL bulk metal hydriding system. The successful deployment of zirconium hydride moderator in advanced reactors requires development of a consistent and affordable production pathway along with implementation of a hydrogen retention solution throughout the reactor life. Fabrication of delta-phase zirconium hydride is challenging since the absorption of a large amount of hydrogen into alpha-zirconium induces significant volume expansion and the present hydrogen concentration gradient results in cracking. A fully programmable hydriding system with continuous hydrogen partial pressure and flow control to facilitate processing of massive metal hydride has been developed at ORNL. In this report, the working principle of the hydriding system will be introduced. Characterization of the produced zirconium hydride includes X-ray powder diffraction to identify the present phases and X-ray Computed Tomography to visualize the internal microstructure (including cracks). The results indicate that single delta-phase zirconium hydride pellets with various sizes have been successfully produced.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Comparative Critical Mass Calculations for NNL and ENDF/B-VIII.0 Zirconium Hydride Thermal Scattering Laws [Slides]

Zirconium Hydride (ZrH x ) is a moderator material for TRIGA reactors and SNAP-10A.The thermal scattering has the behavior of quantum oscillator favorable for moderator feedback. ZrH x occurs as a corrosion product in LWR. Previously new phase specific TSL evaluations were generated and submitted to ENDF/B- VIII.1. These include the effects of crystal structure on elastic scattering of Zr(ZrH x ), permit flexibility in stoichiometry for use in reactor physics calculations and fuel characterization, and expand the TSL material sub-library. ENDF/B-VIII.0 ZrH TSLs do not distinguish between material phase. Current work involves preliminary validation & verification testing on the effect of TSLs on critical mass and associated thermal flux.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Site-specific nanoscale characterization of zirconium hydrides in the hydride rim structure of hydrogen-charged zircaloy-4 cladding

Zircaloy-4 cladding tubes were hydrogen-charged using a static pressure hydrogen charging method to experimentally produce a zirconium-hydride rim structure similar to that observed in Zircaloy-4 cladding tubes after operation in commercial light-water nuclear reactors. Detailed characterization was performed using electron energy loss spectroscopy (EELS) and four-dimensional scanning transmission electron microscopy (4D-STEM). By mapping the position of the plasmon peak in the low-loss EELS spectrum, it was determined that the zirconium hydrides formed were predominantly solid δ-phase zirconium hydrides. 4D-STEM was used to generate phase and strain maps at nanoscale. The interactions between two zirconium hydride platelets less than 200 nm apart leads to the localized lattice rotations and possible phase change, revealing a potential hydride growth mechanism.

4D-STEM↗
DOE OSTI2018

Experimental determination of zirconium hydride precipitation and dissolution in zirconium alloy

In this study, synchrotron X-Ray transmission diffraction experiments were performed to study hydride precipitation and dissolution in the zirconium/zirconium-hydride system while it occurs. Evidence was found that the hysteresis between the terminal solid solubility for precipitation and dissolution is not observed when hydride particles are already present at the beginning of sample cooldown. Additionally, experimental results show that, during a temperature hold, the concentration of hydrogen in solid solution becomes lower than the terminal solid solubility for hydride precipitation and eventually reaches the terminal solid solubility for hydride dissolution, indicating that the latter is the actual thermodynamic solubility limit.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Elastic strain tensor of zirconium hydrides in Zr2.5%Nb pressure tubes by synchrotron X-ray diffraction

Zirconium alloys are used in fuel cladding and structural components of nuclear power plants. Hydrogen enters the Zr matrix during plant operation and precipitates as hydride particles that degrade the mechanical properties of the alloy, limiting service life. Knowledge of the stress state within hydride precipitates is important to understand stress-induced degradation mechanisms such as delayed hydride cracking, but no direct quantification has yet been reported in the literature. Here, measurements are reported of the average elastic strain tensor within δ zirconium hydride precipitates in Zr2.5%Nb pressure tube material from CANDU power plants. Complete intensity and strain pole figures for the hydride were obtained by synchrotron X-ray diffraction experiments on specimens with hydrogen contents ranging from ~100 wt p.p.m. hydrogen to nearly 100% δ-hydride. Zirconium hydride precipitates by a process involving a martensitic transformation, with two hydride variants possible from a single α-Zr grain. A synthetic model of the hydride crystallographic texture allowed the interpretation of the measured strain pole figures and quantification of the elastic strain tensor for both texture components. It was found that the two variants appear in nearly equal proportion but with different stress states, differing in the sign of the shear strain components (~±3000 µ$\epsilon$). This difference is possibly associated with the shear movement of Zr atoms during the phase transformation. This suggests that hydride clusters are composed of stacks of smaller hydrides in alternating hydride variants. Stresses were estimated from a set of rather uncertain hydride elastic constants. Overall, both variants showed compressive strains along the tube axial direction (~5000 µ$\epsilon$). For low hydrogen concentrations, the hydrides' stress tensor is dominated by compressive stresses of ~300 MPa along the axial direction, probably caused by the elongated morphology of hydride clusters along this direction, and variant-dependent shear stresses of ~±100 MPa, probably from the shear movement of the Zr atoms involved in the phase transformation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Study of Anharmonicity in Zirconium Hydrides Using Inelastic Neutron Scattering and Ab-Initio Computer Modeling

The anharmonic phonon behavior in zirconium hydrides and deuterides, including ϵ-ZrH 2 , γ-ZrH, and γ-ZrD, has been investigated from aspects of inelastic neutron scattering (INS) and lattice dynamics calculations within the framework of density functional theory (DFT). The harmonic model failed to reproduce the spectral features observed in the experimental data, indicating the existence of anharmonicity in those materials and the necessity of further explanations. Here, we present a detailed study on the anharmonicity in zirconium hydrides/deuterides by exploring the 2D potential energy surface of hydrogen/deuterium atoms and solving the corresponding 2D single-particle Schrödinger equation to obtain the eigenfrequencies, which are then convoluted with the instrument resolution. The convoluted INS spectra qualitatively describe the anharmonic peaks in the experimental INS spectra and demonstrate that the anharmonicity originates from the deviations of hydrogen potentials from quadratic behavior in certain directions; the effects are apparent for the higher-order excited vibrational states, but small for the ground and first excited states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

First-principles studies of the concentration-dependent tritium diffusion in the zirconium hydrides with and without Sn impurity

We performed first-principles calculations to study the 3 H diffusion in the zirconium hydrides with or without Sn impurity. Our results show that the formation of Zr 3 H x becomes preferable as the 3 H concentration increases. Based on the most stable configurations of Zr 3 H x (x = 0.5, 1.0, 1.5, 2.0), we studied the interstitial 3 H diffusion with or without Sn impurity. The results show that the interstitial 3 H diffusion becomes less probable in the hydrides with a higher 3 H concentration. When introducing a substitutional Sn impurity, the diffusion barriers increase. Therefore, the substitutional Sn in the diffusion pathway hampers the 3 H diffusion in Zr hydrides.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Site specific dependencies of hydrogen concentrations in zirconium hydrides

Here, Zircaloy-4 specimens were H-charged up to 1230 wppmH. Intra-, inter- and trans-granular zirconium hydride precipitates (or ZrH 2–x where 1/(2–x) is the Zr/H molar ratio) were observed throughout the α-Zr matrix. Transmission Electron Microscopy and electron diffraction confirmed that the ZrH 2–x precipitates were face-centred cubic structures consistent with the δ-ZrH 2–x phase. Electron Energy Loss Spectroscopy analysis of the δ-ZrH 2–x precipitates at three different nucleation spots displayed shifts in the plasmon energy loss peaks that can be attributed to local variations of the H content of the δ-ZrH 2–x precipitates rather than the presence of different ZrH 2–x phases as has previously been assumed.

36 MATERIALS SCIENCE↗