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At least 415 records · Page 23

Nanocrystalline SiC and Ti 3 SiC 2 Alloys for Reactor Materials: Diffusion of Fission Product Surrogates

MAX phases, such as titanium silicon carbide (Ti 3 SiC 2 ), have a unique combination of both metallic and ceramic properties, which make them attractive for potential nuclear applications. Ti 3 SiC 2 has been suggested in the literature as a possible fuel cladding material. Prior to the application, it is necessary to investigate diffusivities of fission products in the ternary compound at elevated temperatures. This study attempts to obtain relevant data and make an initial assessment for Ti 3 SiC 2 . Ion implantation was used to introduce fission product surrogates (Ag and Cs) and a noble metal (Au) in Ti 3 SiC 2 , SiC, and a dual-phase nanocomposite of Ti 3 SiC 2 /SiC synthesized at PNNL. Thermal annealing and in-situ Rutherford backscattering spectrometry (RBS) were employed to study the diffusivity of the various implanted species in the materials. In-situ RBS study of Ti 3 SiC 2 implanted with Au ions at various temperatures was also performed. The experimental results indicate that the implanted Ag in SiC is immobile up to the highest temperature (1273 K) applied in this study; in contrast, significant out-diffusion of both Ag and Au in MAX phase Ti 3 SiC 2 occurs during ion implantation at 873 K. Cs in Ti 3 SiC 2 is found to diffuse during post-irradiation annealing at 973 K, and noticeable Cs release from the sample is observed. This study may suggest caution in using Ti 3 SiC 2 as a fuel cladding material for advanced nuclear reactors operating at very high temperatures. Further studies of the related materials are recommended.

36 MATERIALS SCIENCE↗

Phase-field modeling of stacking structure formation and transition of δ-hydride precipitates in zirconium

d-hydride structures in Zr nuclear fuel-rod cladding significantly affect mechanical properties. In this work, a micromechanical phase-field model is developed to investigate the effect of interfacial energy anisotropy and elastic interaction on the nucleation, stacking structure formation, and stacking structure transition of d-hydride precipitates. It is found that the nucleation probability and growth of d-hydride near pre-existing hydrides are strongly spatially dependent. Results show that (1) the d-hydride precipitate has a platelet-like shape. The large shear deformation associated with lattice mismatches and a small interfacial energy of its broad interface cause the orientation of the plate-like d-hydride off the basal plane a small angle of approximately 14.7°. (2) Stress-induced nucleation of d-hydride precipitates near a pre-existing hydride results in the unique stacking structure formation of d-hydride precipitates. (3) The morphology and alignment of hydride stacking structures, called as macroscopic hydrides which consist of microscopic hydrides with certain stacking sequences, change under stresses. The alignment of macroscopic hydrides changes from along the circumferential direction to along the radial direction under tensile hoop stress while the orientation of microscopic hydrides remains parallel to the basal plane. These results are in agreement with experimental observations. The simulations reveal that stress-induced heterogeneous nucleation and growth is the mechanism for the formation and transition of unique macro-hydride stacking structures observed in in Zr nuclear fuel-rod cladding.

Han, G. M.↗

Status Report on the Development of Cladding Inner-wall and Outer-wall Coatings

Advanced cladding is critical for nuclear reactors with enhanced performance in radiation tolerance, neutron transparency and reactor safety. Using advanced cladding will ensure the adequate thermal conductivity and mechanical stability of the cladding base material, corrosion resistance and high-temperature coolant compatibility of the cladding surface, and chemical stability in the cladding inner wall against fuel cladding chemical interaction (FCCI). An innovative cladding with a three-layer structure (i.e., a modified outer surface, a robust clad base material, and a modified inner wall) promises to meet all these requirements. In this status report, the initial efforts on the development of cladding inner-wall and outer-wall coatings are summarized. The activities covered in this report are (1) High-resolution TEM studies of TiN/HT-9 interface atomic structure and chemistry after ion irradiation, (2) High-resolution TEM studies of TiN/14YWT ODS interface atomic structure after thermal cycling, (3) Inner-wall TiN coating for an experimental 14YWT ODS cladding, and (4) Corrosion test of TiN coated Ziracloy-4 bar samples.

36 - MATERIALS SCIENCE↗

Potential Impact of Interfacial Bonding Efficiency on High-Burnup Spent Nuclear Fuel Vibration Integrity during Normal Transportation

Finite element analysis (FEA) was used to investigate the impacts of interfacial bonding efficiency at pellet pellet and pellet clad interfaces on spent nuclear fuel (SNF) vibration integrity. The FEA simulation results were also validated and benchmarked with reverse bending fatigue test results on surrogate rods consisting of stainless steel (SS) tubes with alumina-pellet inserts. Bending moments (M) are applied to the FEA models to evaluate the system responses of the surrogate rods. From the induced curvature, , the flexural rigidity EI can be estimated as EI=M/ . The impacts of interfacial bonding efficiency on SNF vibration integrity include the moment carrying capacity distribution between pellets and clad and the impact of cohesion on the flexural rigidity of the surrogate rod system. The result also indicates that the immediate consequences of interfacial de-bonding are a load carrying capacity shift from the fuel pellets to the clad and a reduction of the composite rod flexural rigidity. Therefore, the flexural rigidity of the surrogate rod and the bending moment bearing capacity between the clad and fuel pellets are strongly dependent on the efficiency of interfacial bonding at the pellet pellet and pellet clad interfaces. The above-noted phenomenon was calibrated and validated by reverse bending fatigue testing using a surrogate rod system.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Impacts of Ionizing Radiation on Sulfur Chloride Compounds for Advanced Fuel Cladding Decontamination Processes

Tripling the nation’s nuclear energy capacity is a critical component for significantly increasing energy production and reducing energy costs for American families and businesses. Achieving this vision requires fuel cycle technologies that maximize resource utilization while minimizing radioactive waste generation. Advanced sulfur chloride–based chlorination technologies are being developed to enable efficient recycling of fuel cladding materials, which account for a significant fraction of used nuclear fuel. However, the impacts of ionizing radiation on the longevity and performance of these sulfur chloride compounds are not well established. Here, we will explore the effects of gamma and electron-beam irradiation on the chemical composition of select sulfur chloride reagents, specifically sulfur monochloride (S2Cl2) and thionyl chloride (SOCl2), and the impacts of pre-irradiation on the chlorination yield/chemical dissolution of surrogate aluminum alloy 6061 (AA6061-T6) materials.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗

Purification of Zirconium Tetrachloride (ZrCl{sub 4}) from UNF Cladding - A Progress Report

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 and/or recovery and reuse of these materials would significantly reduce the amount of high level waste associated with light water nuclear energy reactors and could provide a new source of hafnium free zirconium for the fabrication of new nuclear components. A step in a strategy to recycle zirconium from used cladding materials is the direct, high yield chlorination reaction that produces zirconium tetrachloride (ZrCl{sub 4}). The ZrCl{sub 4} so obtained is contaminated with other metal chloride species (FeCl{sub 3}, NbCl{sub 5}, NbOCl{sub 3}, SnCl{sub 4}, CsCl, SbCl{sub 5}, etc.) that originate from the alloying metals present initially as well as contaminants from oxide layers on the cladding, trace fission products, fuel residues, activation byproducts, and tritium. The suggested strategy to remove the metal chloride impurities is based on sublimation at atmospheric pressure combined with chemical treatments influencing volatility of the impurities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Investigations into the Gas Phase Reactions of Zirconium Tetrachloride (ZrCl) from UNF Cladding

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. A step in a strategy to recycle zirconium from used cladding materials is the high yield chlorination of Zircaloys to produce zirconium tetrachloride (ZrCl{sub 4}). The ZrCl, is contaminated with other metal chloride species that originate from the alloying metals as well as contaminants from oxide layers on the cladding, trace fission products, fuel residues, activation byproducts, and tritium. The properties of these complex mixtures must be better understood before purification protocols can be developed that will allow zirconium chloride to be recycled further. First order thermodynamic modeling of high temperature mixtures of ZrCl, and other metal chlorides in the gas phase may not accurately predict their properties. Computational modeling studies indicate that mixed metal adducts may form under the conditions of sublimation-based purification protocols. In light of these predictions, alternate strategies may also be needed to obtain pure ZrCl, from such mixtures. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Potential Impact of Cladding Wettability on LWR Transient Progression

The US Department of Energy Office of Nuclear Energy (DOE-NE) Advanced Fuels Campaign (AFC) is working closely with the nuclear industry to develop fuel and cladding candidates with potentially enhanced accident tolerance. This type of fuel is also known as accident tolerant fuel (ATF). Two promising cladding material candidates with potentially enhanced accident tolerance are silicon carbide (SiC) and an iron-chromium-aluminum (FeCrAl) alloy. The FeCrAl alloy features significantly enhanced oxidation resistance versus the Zr-based alloys currently used in state-of-the-art light water reactors (LWRs). Thermal-fluid characteristics are a vital element of a holistic engineering evaluation of ATF concepts. One characteristic related to boiling heat transfer is the critical heat flux (CHF). At CHF, the efficacy of heat transfer rapidly degrades and components can heat up rapidly. CHF is the heat flux at which the departure from nucleate boiling (DNB) occurs in PWRs. DNB is directly relevant to the departure from nuclear boiling ratio (DNBR), which is the ratio between the critical heat flux and the actual heat flux. Surface wettability is an important factor that influences CHF. CHF plays a significant role in determining safety margins during normal operation and also in the progression of potential transient or accident scenarios. Significant changes in CHF properties and boiling heat transfer characteristics will impact the progression of transient and accident events and reactor safety characteristics. Additionally, the behavior of the candidate cladding materials post-CHF impacts reactor safety. A brief description of the relationship between cladding material properties and CHF is provided, followed by an analysis of two hypothetical transient scenarios: a super-prompt reactivity-initiated accident (RIA) and an anticipated transient without scram with instability (ATWS-I). The analysis illustrates the potential impact of cladding material properties on safety margins via direct alteration of calculated CHF values. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

TEM characterization of two variants of fuel cladding chemical interaction in a HT-9 Clad U-10Zr Fuel. Variant 1: FCCI with a Zr Rind

Here, this study investigated the fuel cladding chemical interaction (FCCI), a key factor that limits operational temperature and burnup, in an HT-9 clad U-10Zr nuclear fuel sample irradiated to a high burnup of 13.1 at.% at a time-averaged peak inner cladding temperature (PICT) of 530 °C. Previous results showed this fuel sample exhibited two distinct levels of FCCI at d. This paper analyzed the FCCI at an azimuthal position showing an interdiffusion layer of <10 µm using transmission electron microscopy to examine chemical and crystallographic nature of phases at the fuel-cladding interface at the nanoscale level. A ZrC layer and a Zr 3 Si phase were identified at the interface; these, along with the relatively low local temperature, potentially contributed to limit interdiffusion, behaving as inhibitors for deleterious interactions. Lanthanides (Ln) partially consumed the ZrC layer and interacted with Fe, forming a Zr-Ln compound and a (Zr,Ce)Fe 2+x phase while also infiltrating up to 4 µm into the cladding. Neither U nor Zr were observed in the cladding, whereas Fe diffused up to 3–5 µm in the fuel. Fe infiltration formed a ternary U-Zr-Fe ε-phase and likely promoted the precipitation of a Cr-rich α’ phase on the cladding interface. Additionally, a Cr-rich χ-phase, likely formed by the dissociation of pre-existing M 23 C 6 carbide precipitates, was identified about 2–5 µm from the fuel-cladding interface. Irradiation-induced nano-voids were also observed in the HT-9 bulk. These findings provide critical insights into FCCI mechanisms at representative irradiation conditions, essential for developing models simulating in-pile metallic fuel behaviors for next-generation reactors.

36 - MATERIALS SCIENCE↗

A study on texture stability and the biaxial creep behavior of as-hydrided CWSR Zircaloy-4 cladding at the effective stresses from 55 MPa to 65 MPa and temperatures from 300°C to 400°C

The creep rupture of high burnup used nuclear fuel (> 45 GWD/MTU) cladding is regarded as one of the failure mechanisms during long-term dry storage. A high amount of zirconium hydride in the cladding matrix would degrade the mechanical properties of the cladding especially leading to delayed hydride cracking. To better understand the influence of zirconium hydride on the biaxial thermal creep performance and the crystalline texture stability of Zircaloy-4 cladding, the pressurized tube technique is applied to test the durability of the as-hydrided material. Tests were performed on as-received Zircaloy-4 tubular specimens as well as-hydrided ones with targeted 300 wt parts per million (wppm) or 750 wppm hydrogen. The biaxial creep experiments were conducted at temperatures from 300 degrees C to 400 degrees C and at equivalent stresses at mid-wall from 55 MPa to 65 MPa. The hydridation process prior to creep tests induces the formation of FCC delta-hydride platelets along the circumferential direction of the tube. This alignment and phase structure of hydride show no significant change after biaxial creep tests. The creep strain-rate negatively depends on the hydrogen content. The synchrotron wide-angle X-ray diffraction (WAXD) technique and electron backscatter diffraction (EBSD) analysis were applied for the study of the crystallographic orientation relationship. zirconium-to-hydride grain orientation follows Shoji-Nishiyama crystallographic relationship. This relationship is stable before and after creep deformation. These results of creep performance and texture stability of Zircaloy-4 claddings can help support the design basis of interim and long-term dry storage facilities.

creep↗

A Degradation Model and Testing Protocol for Metallic Waste Forms

Metallic waste forms developed to immobilize high-level radioactive wastes generated in advanced (closed) fuel cycles are being evaluated as part of the US DOE Fuel Cycle Research and Development program. The electrometallurgical reprocessing of used metallic fuels to recover U and Pu generates two waste streams: salt waste comprised of electro-refiner salt contaminated with oxidized fission products and metallic waste comprised of activated cladding and metallic fission products that were not oxidized under the processing conditions. Metallic waste forms can be made by directly melting the cladding and fuel wastes with small amounts of trim metals to form a multiphase alloy material in which radionuclides and other waste constituents are immobilized within chemically durable intermetallic and iron-based solid solution phases. Some components of the waste streams serve as important constituents of phases comprising the waste form, such as Mo and Zr, which form Fe{sub 2}Mo and Fe{sub 2}Zr intermetallic phases. Other waste constituents are accommodated as substitutional contaminants, such as Tc within the Fe{sub 2}Mo intermetallic and U/TRU within the Fe{sub 2}Zr intermetallic. Sufficient amounts of these host phases must be available to accommodate all radionuclides in the waste stream. The compositional flexibility of the host phases to incorporate waste components is being utilized to formulate metal waste forms that will accommodate variations in waste streams compositions that will occur over long-term fuel reprocessing operations. Small amounts of trim metals can be added to tailor the phase assembly to match the waste stream composition and facilitate waste form processing. For example, additional Zr may be added during waste form production to ensure all U/TRU is sequestered in a durable Fe{sub 2}Zr host phase and trim Cr, Mo, and Ni can be added to supplement the amounts provided by the steel cladding to improve the durability of a metallic waste form. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nondestructive Evaluation on Hydrided LWR Fuel Cladding by Small Angle Incoherent Neutron Scattering of Hydrogen

A non-destructive neutron scattering method was developed to precisely measure the uptake of total hydrogen in nuclear grade Ziraloy-4 cladding. The hydriding apparatus consists of a closed stainless steel vessel that contains Zr alloy specimens and H gas. By controlling the initial H gas pressure in the vessel and the temperature profile, target H concentrations from tens of ppm to a few thousands of wppm have been successfully achieved. Following H charging, the H content of the hydrided specimens was measured using the vacuum hot extraction method (VHE), by which the samples with desired H concentration were selected for the neutron study. Small angle neutron incoherent scattering (SANIS) were performed in the High Flux Isotope Reactor at Oak Ridge national Laboratory (ORNL). Our study indicates that a very small amount ( 20 ppm) H in commercial Zr cladding can be measured very accurately in minutes for a wide range of H concentration by a nondestructive method. The H distribution in a tube sample was obtained by scaling the neutron scattering rate with a factor, which is determined by calibration process with direct chemical analysis method on the specimen. This scale factor can be used for future test with unknown H concentration, thus provide a nondestructive method for absolute H concentration determination.

Yan, Yong↗

An impedance-based diameter gauge for in-pile fuel deformation measurements

During irradiation, the fuel-cladding interface of a nuclear fuel rod can experience significant mechanical and chemical interaction. In-situ measurement of the radial deformation of the cladding can quantify the extent of this interaction and the state of the cladding. Existing capabilities to perform in-pile diameter measurements are limited by required contact and an intrusive presence of a device near to a specimen. To overcome these limitations, researchers have developed and evaluated an electrical impedance based diameter gauge using a benchtop system. The sensor consists of an electrically conductive concentric ring around the fuel cladding such that the electrical impedance between the ring and cladding is measured. Additionally, the cladding diameter is determined through a measurement of the electrical impedance between the electrodes with a known ring electrode diameter. Analytic and 3-D finite element analyses (FEA) were used to quantify the measurement sensitivity, uncertainty, and off-design conditions. The experimental sensor measured diameters with <20 µm of error, and had a measurement resolution of <1 µm for diameters ranging from 9.5 to 9.6 mm. Lastly, the uncertainty analysis for the experimental setup estimated an uncertainty of 20 µm, consistent with the experimentally measured results.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Diffusion Behavior of Oversized Fission Products in bcc Fe Cladding: A First-Principles Study

Fuel-Cladding Chemical Interaction (FCCI) poses significant challenges in nuclear reactors, where fission products from nuclear fuel interact with Fe-based cladding materials, potentially compromising their structural integrity. This study investigates the diffusion behavior of oversized fission products, Pr, Nd, Ce, and La, within bcc Fe cladding using density functional theory (DFT), nudged elastic band (NEB) method, and self-consistent mean field (SCMF) theory. Our results reveal significant long-range vacancy binding energies, particularly up to the 6th nearest neighbor, with La exhibiting the strongest binding affinity, followed by Nd, Ce, and Pr. The NEB calculations indicate significant high barriers for the dissociation of 1nn vacancy-solute pairs for all fission products. The tracer diffusion coefficients of these fission products was derived in Arrhenius form. The significant trapping effect of vacancies by a very dilute amount of fission products reduces vacancy mobility, leading to an oversaturation of point defects, void nucleation, and swelling. These are critical issues for irradiated cladding materials. The tracer diffusion coefficients indicate that Nd diffuses the fastest, followed by La, Ce, and Pr. This study provides essential insights for developing advanced cladding materials and design strategies to mitigate FCCI, ultimately enhancing nuclear reactor safety and performance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Tiamat

Tiamat is the driver program for coupling three application codes together to simulate a nuclear reactor core. This code is used to study pellet clad interaction failures in commercial nuclear light water It generates stress plots and temperature profiles for fuel rods in the reactor core. The driver program initializes the underlying applications, initiates the overall solve process, generates consistent input files and manages the data transfers between the applications. It contains the top level driver code, the data transfer code, input file parsing and corresponding unit tests. Tiamat was developed under the CASL Energy Innovation Hub. The Tiamat code DOES NOT include any source code for the actual coupled physics application components or solvers. The application codes and solver libraries must be obtained separately from the Tiamat source code. Tiamat will be released open source under a BSD license.

Source record↗

Characterization of Fuel-Cladding Bond Strength Using Laser Shock

This paper describes new laser-based capabilities for characterization of fuel-cladding bond strength in nuclear fuels, and presents preliminary results obtained from studies on as-fabricated monolithic fuel consisting of uranium-10 wt.% molybdenum alloys clad in 6061 aluminum by hot isostatic pressing. Two complementary experimental methods are employed, laser-shock testing and laser-ultrasonic imaging. Measurements are spatially localized, non-contacting and require minimum specimen preparation, and are therefore ideally suited for applications involving radioactive materials, including irradiated materials. The theoretical principles and experimental approaches employed in characterization of nuclear fuel plates are described. The ability to measure layer thicknesses, elastic properties of the constituents, and the location and nature of laser-shock induced debonds is demonstrated, and preliminary bond strength measurement results are discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗