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At least 55 records · Page 3

SR19036 Improve TRP Cutter Head Performance

The Target Rod Preparation (TRP) cutter head motor suffers from overheating problems during Tritium Producing Burnable Absorber Rods (TPBAR) breaching operations. The TRP cell cutter head drive motor must remain below the administrative limit of 100°C during breaching operations. If temperatures in excess of 100°C are reached, work must be stopped, and the motor allowed to cool. The work stoppage due to overheating of the drive motor directly and drastically lowers the efficiency of the TPBAR breaching process, reducing the production of Tritium gas. Due to the increased need for Tritium gas, the overheating problem must be addressed to improve the overall efficiency of the TPBAR breaching process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Assessment of Existing Transportation Packages for Use with HALEU

Commercial light water reactor operators and fuel vendors in the United States are pursuing changes to fuel that include increased 235 U enrichment. Economic studies generally anticipate maximum near-term fuel assembly designs with up to 8 wt.% 235 U. Many next-generation nuclear reactor designs require high-assay low-enriched uranium (HALEU) (19.75 wt.% > 235 U > 5 wt.%) fuel. One necessary element for the commercial-scale use of HALEU is the ability to safely transport large quantities of enriched fuel material in multiple forms. However, there is uncertainty as to whether subcriticality requirements can be satisfied with existing package designs and whether existing critical benchmark experiment data are sufficient to support criticality safety code validation for HALEU transportation applications. This study assesses the potential to use currently licensed transportation packages for the transportation of increased enrichment unirradiated U fuel forms. The assessment uses selected package designs that represent the five categories of fuel form-boiling water reactor pins and assemblies, pressurized water reactor pins and assemblies, UF 6 , U-metal and tristructural isotropic (TRISO) particles, and UO 2 pellets or powder-and focuses on demonstrating subcriticality and identifying benchmark critical experiments appropriate for use in criticality computer code validation. Key quantities of interest that relate to subcriticality are limiting conditions (e.g., optimum moderation), package or package array k eff , package capacity, and package transportation array size. The SCALE TSUNAMI-3D and TSUNAMI Indices and Parameters codes are used for sensitivity and uncertainty calculations and for identification of candidate critical benchmark experiments for code validation. The primary metric for identifying candidate benchmarks is the similarity coefficient, c k . For each fuel form category, a representative package is evaluated. Results provided for each package evaluation include enrichment and packaging limits (e.g., maximum transportation array size as a function of enrichment) and benchmark critical experiment similarity coefficients. Results indicate that there are viable means for increasing enrichments into the HALEU range across the spectrum of fuel forms with differing increase amounts available for different packages. Sources of subcriticality margin to offset increased enrichment reactivity include reduced transportation array size, reduced fissile mass, burnable absorber credit, and safety analysis margin harvesting. For all packages except the DN-30, numerous critical benchmark experiment candidates for validation were identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

First-principles Studies of Tritium Reactivity and Diffusivity on Defective and Carbon Doped Surfaces of $\gamma$-LiAlO 2 Pellets (Tritium Science Program Report FY 2019 )

In tritium-producing burnable absorber rods (TPBARs), tritium ($^{3}_{1}$H,T) is produced in 6 Li isotope enriched γ-LiAlO 2 ceramic pellet. However, a better understanding of $^{3}_{1}$H transport through the pellets, getters and the barrier/cladding system is hampered by a lack of fundamental data about the $^{3}_{1}$H solubility and diffusivity. In the process of $^{3}_{1}$H diffusion from bulk γ-LiAlO 2 to its surface, it is possible that $^{3}_{1}$H atoms bind with surface atoms or become trapped at vacancies sites. By increasing the number of $^{3}_{1}$H diffused from bulk to surface, upon recombination and desorption from surface sites, they will escape from the γ-LiAlO 2 surface to form different $^{3}_{1}$H species (possibly being as T, T 2 , T 2 O, OT, or CT x (x=1-4, with C impurity present at a 100-600 ppm level in pellets) that need to be identified and can become captured by the getter. Therefore, exploring the $^{3}_{1}$H diffusion from bulk to surface, corroborated with surface adsorption, diffusion and recombination and followed by desorption from surface as various types of $^{3}_{1}$H species becomes a very important task as an integral part of the study of $^{3}_{1}$H solubility and diffusivity in the pellets.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fundamental Studies of Tritium Diffusivity in Pure and Defective Zircaloy-4 Getters (Tritium Science Program FY2020 Report)

Zirconium (Zr) alloys are extensively used as tritium (T) getters in nuclear reactors due to their low absorption cross section to thermal neutron, good mechanical properties at high temperature and resistant to corrosion in different environmental conditions. Zr alloys have better thermal properties than many other refractory alloys including stainless steel. The nuclear characteristic is simulated, and T is produced in tritium-producing burnable absorber rods (TPBAR) by the irradiation of neutron flux in pressurized water reactor (PWR). T thus produced diffuses through the pellets and is captured by the getter where it chemically reacts with Zr to form metal hydride (ZrTx). These hydrides are brittle and affect adversely the mechanical properties of alloys. In addition to that, mismatch in the lattice structures after hydride formation creates a stress which needs to be considered in component design and their life evaluation. Therefore, understanding the behavior of T and its species becomes significant as fuel burnup is increased, which leads to increase in hydrogen pickup and oxide formation. The transport of T and its species in pure Zr alloys, and in alloys with certain alloying elements and defects are important to understand in order to enhance the performance of the materials.

36 MATERIALS SCIENCE↗

Fundamental Studies of Tritium Formation and Diffusivity in Pure and Defective Zircaloy-4 Getters

Zirconium (Zr) and its alloys are used as fuel cladding in nuclear reactors. These materials have their low absorption cross-section for thermal neutrons and have good mechanical and thermal properties. In addition, they are used as tritium getters in tritium-producing burnable absorber rods (TPBARs), in the form of nickel-plated Zircaloy-4 tubes. To produce 3 H, the breading blankets such as lithium aluminate are irradiated in pressurized water. 3 H produced in this process is captured by the getter and 3 H reacts chemically with Zr to form metal hydride (ZrTx). The precipitation of metal hydride results in not only the volume increase and hydrogen embrittlement of zircaloy but also changes in getter’s chemical properties. This degrades the getter’s performance. Therefore, understanding the behavior of 3 H (such as diffusion and solubility) in zircaloy is important to understand getter performance.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Light Water Reactor LEU+ Lattice Optimization

Commercial light water reactor (LWR) operators and fuel vendors in the United States are exploring potential changes to nuclear fuel that include low-enriched uranium plus (LEU+) designs to further improve operational economics (e.g., extend cycle length). LEU+ fuel is fuel with a maximum enrichment between 5 wt% and 10 wt% 235 U; it allows for higher assembly burnup but likely requires additional reactivity control, e.g., increased burnable absorbers. This report examines possible LEU+ fuel lattice design changes using the lattice physics code, SCALE/Polaris. An optimization driver called the Metaheuristic Optimization Tool (MOT) is used to automate domain space exploration and optimization of LEU+ lattice designs. Heuristics from previous LWR lattice optimization studies were used to construct the objective function and define the domain space for optimization. This work successfully demonstrated that the optimization algorithms of MOT can generate feasible, nonproprietary LEU+ lattice designs (GE14 10 × 10 and Westinghouse 17 × 17) that meet the constraints of traditional LWR lattices while extending cycle length.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Investigating Hydrogen Isotope Exchange Reactions on Lithium Aluminate Pellets in TPBAR (FY22 Report)

We developed a novel operando Raman spectroscopy method for investigation of hydrogen (H) isotope exchange reactions in the lithium aluminate (γ-LiAlO 2 ) that allows modeling of tritium behaviors in high temperature and in an irradiated environment. The lithium aluminate pellet is a main component in the Tritium-Producing Burnable Absorber Rod (TPBAR). We used deuterium ( 2 H or D) as a surrogate to simulate tritium ( 3 H or T). We used a surface analysis tools in situ/operando Raman spectroscopy to observe the transformation OH and OD compositional changes. We also used ToF-SIMS to analyze the lithium aluminate pellet control sample to build the base line for future in situ/operando analysis. To conduct operando Raman spectroscopy, we developed a custom reaction cell with a detachable micro heater using microelectromechanical systems (MEMS) and 3D printing techniques. Multiple versions were developed and tested. Using the new reaction cell, we demonstrated operando Raman spectroscopy of water (H 2 O) and deuterated water (D 2 O) with nitrogen (N 2 ) exposure onto the lithium aluminate (LiAlO2) pellet specimen, respectively, using a wet gas injection setup. We also successfully developed a detachable microheater that can heat up to ~250°C for ~90 mins. The Raman spectra did not show clear H 2 O and D 2 O characteristic peaks, which indicates that introducing H 2 O and D 2 O onto the surface of the pellet is challenging due to its dense structure nature. Our efforts suggest that various improvements are needed, such as increasing reaction cell operating gas pressure and thinning pellet sample thickness, to obtain meaningful measurements.

07 ISOTOPE AND RADIATION SOURCES↗

First-Principles Studies of Tritium Species Dissociability & Diffusivity Across the Interface of Nickel-Plated Zircaloy-4

Zirconium (Zr) and its alloys (Zircaloy-4) are widely used in nuclear reactors due to their low neutron adsorption cross-section and excellent corrosion resistance. In tritium-producing burnable absorber rods (TPBARs), the metal getter tube located between the cladding and the γ-LiAlO 2 pellets is composed of nickel (Ni)-plated Zircaloy-4, which is used to capture tritium ( 3 H) species (mainly 3 H 2 and 3 H 2 O) generated from γ-LiAlO 2 pellets during irradiation. The 3 H-related products transfer to the surface of metal Ni upon adsorption and dissociation to form new 3 H species and diffuse into the Zircaloy-4 getters to form metal hydrides (Zr 3 H x ). Therefore, exploring 3 H species ( 3 H 2 , 3 H 2 O) dissociation on the surface of Ni and diffusion across the interface of Ni-plated Zircaloy-4 getters can provide a better understanding of 3H species formation and transport from pellets into the getters.

36 MATERIALS SCIENCE↗

Pressurized Water Reactor Gadolinia Pin Location Optimization

This report presents the results of lattice optimization studies performed to find optimum locations for gadolinia burnable absorber (BA) rods in pressurized water reactor (PWR) lattice fuel designs. Initial excess reactivity suppression allows core designers to further improve operational economics by extending cycle length. Gadolinia BAs are commonly used in boiling water reactor assembly designs for this purpose. In recent years, gadolinia absorbers have been used in PWR designs owing to their longer effectiveness for reactivity suppression compared with common BAs used in PWR assemblies. This report examines the optimum gadolinia pin placement in 17 × 17 PWR lattices at different fuel and gadolinia concentrations for optimized lattice performance, using the SCALE/Polaris lattice physics code. The completed work is continuation of the Light Water Reactor LEU+ Lattice Optimization (ORNL/TM-2021/2366) project. An optimization driver called the metaheuristic optimization tool (MOT) is used to automate domain space exploration and optimization of the lattice designs. Heuristics from previous light-water reactor (LWR) lattice optimization studies were used to construct the objective function and define the domain space for optimization. This work successfully demonstrated that the optimization algorithms of MOT can generate feasible, nonproprietary PWR lattice designs with gadolinia.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Hydrogen and Deuterium Reactivity with Carbon Surface Impurities on the TPBAR Getter Ni Plate Studied in situ with Environmental XPS

Tritium for the U.S. Department of Energy’s Tritium Readiness Program is produced in tritium-producing burnable absorber rods (TPBARs) inserted into light-water nuclear reactors. The rods are stainless-steel-clad tubes with a permeation barrier coating and internal components. The internal components have been designed and selected to produce and retain tritium. The TPBAR incorporates a Ni-plated Zircaloy-4 getter tube to capture tritium and prevent it from reaching the rod cladding and permeating into the environment. The role of the Ni coating is to protect the Zircaloy-4 getter from oxidation while allowing for maximum tritium permeability. Ubiquitous surface impurities on the Ni, such as carbon, could limit its protective functionality and permeability if they exist in relatively large concentrations. The reactivity of impurity carbon with permeating tritium can also result in tritiated hydrocarbon impurities on the gas phase. The goal of this work is to determine quantitatively the chemical state and reactivity of potential Ni coating impurities in actual TPBAR getter samples. Using Environmental X-ray Photoelectron Spectroscopy (eXPS), a very sensitive gas/surface chemistry diagnostic, we reveal in situ the source and evolution of carbon on the Ni surface at different hydrogen and deuterium pressure conditions, and how carbon reactivity may result in hydrocarbon gas-evolution at application-relevant temperatures.

36 MATERIALS SCIENCE↗

Assessment and Planning of HFIR Test Articles

Burnable absorbers (BAs) are introduced into nuclear fuels to aid in controlling the activity of the irradiated fuel at the beginning of life in a light water reactor (LWR). This improves the efficiency of the reactor since it allows for higher enrichments (> 5 % 235 U) to be used in a LWR, which increases the burnup limit and therefore the cycle length. The purpose of the BA is to absorb neutrons to prevent power peaking, and the concentration of BA is consumed under irradiation. In order to understand the effect of the BAs on the microstructure and thermophysical properties of the fresh and irradiated fuel, neutron irradiation tests will be carried out at the High Flux Isotope Reactor (HFIR). These tests will include Gd 2 O 3 doped UO 2 fuels with concentrations that vary from 4 to 10 weight % Gd 2 O 3 .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

First-Principles Studies of Tritium Species Diffusivity Across the Interfaces of Ni-NiZr Alloy-Zircaloy-4

A tritium producing assembly, also known as tritium producing burnable absorber rods (TPBARs), consists of a metal getter tube located between the cladding and γ-LiAlO2 pellets. The metal getter tube is composed of a nickel (Ni) layer coated on Zircaloy-4. The getter assembly is used to capture tritium (3H) species (mainly 3H2 and 3H2O) generated from γ-LiAlO2 pellets during irradiation. Exploring 3H species (3H2, 3H2O) dissociation on the Ni surface and diffusion in the Ni layer and across the interface of Ni-plated Zircaloy-4 getters can provide insights on tritium transport and retention in the pellets and the getter materials. . In FY25, based on the ideal interface model of Ni-Zircaloy-4 generated in FY24, we will further explore the diffusion pathways of 3H across such Ni-ZrNi-alloy layer-Zircalory-4 interfaces under different conditions, including with oxide/hydroxide clusters on the Ni layer, and impurities located in ZrNi-alloy and Zircalory-4 layers. Due to the size limitation of DFT simulation, we will separate the 3-layer system into 3 sub-systems: Ni-ZrNi interface, ZrNi alloy layer, ZrNi-alloy-Zircaloy-4 interface, and simulate the diffusion barriers for tritium.

diffusion barrier↗

Fabrication and Characterization of MiniFuel Specimen

Burnable absorbers (BAs) are used in UO 2 fuels to tune the reactivity in a light water reactor (LWR) particularly at the beginning of life of the fuel. BAs are elements that have high neutron absorption cross sections and because of this property can prevent power peaking. The addition of BAs reduces the reactivity at the beginning of life, and this in turn allows for the increase of enrichments from > 5 % 235 U up to ~ 10 %. This also enables the increase of the burnup limit to 75 GWd/MTU and the cycle length to 24 months. The BA are eventually consumed under irradiation, and their concentration is diminished at roughly 10-20 GWd/MTU. The objective of this report is to fabricate UO 2 fuels that have been doped with BAs (Gd 2 O 3 in this case) and subsequently irradiate them in the high flux isotope reactor (HFIR) at Oak Ridge National Laboratory. The test specimen that are fabricated include 4 and 8 weight % Gd 2 O 3 doped UO 2 to investigate the influence of the BAs on the thermophysical properties and microstructure of the fresh and irradiated fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Coated U3Si2 pellets with enhanced water and steam oxidation resistance

A method of forming a water resistant boundary on a fissile material for use in a water cooled nuclear reactor is described. The method comprises coating the fissile material, such as a pellet of U3Si2 and/or the grain boundaries, to a desired thickness with a suitable coating material, such as atomic layer deposition or a thermal spray process. The coating material may be any non-reactive material with a solubility at least as low as that of UO2. Exemplary coating materials include ZrSiO4, FeCrAl, Cr, Zr, Al—Cr, CrAl, ZrO2, CeO2, TiO2, SiO2, UO2, ZrB2, Na2O—B2O3—SiO2—Al2O3 glass, Al2O3, Cr2O3, carbon, and SiC, and combinations thereof. The water resistant layer may be overlayed with a burnable absorber layer, such as ZrB2 or B2O3—SiO2 glass.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Tritium diffusion and formation in the bulk and defective surface of γ-LiAlO2 pellets: First-principles investigation

In tritium-producing burnable absorber rods (TPBAR), γ-LiAlO2 is used in the form of an annular ceramic pellet enriched with the 6Li isotope. When irradiated in a pressurized water reactor (PWR), the <sup>6</sup>Li pellets absorb neutrons and produce tritium (<sup>3</sup>H) through <sup>6</sup>Li + n <sup>3</sup>H + α. The 3H chemically reacts with the metal getter where it is captured and leads to formation of a metal hydride. For TPBARs to enable effective tritium production in PWRs, we investigated the <sup>3</sup>H diffusion pathways in the bulk and surface of γ-LiAlO<sub>2</sub> with different concentrations of lithium defects. The calculated results for bulk and low-index surfaces, thermal conductivity, 3H activation energy barriers, and the 3H diffusion coefficients in γ-LiAlO<sub>2</sub> are in good agreement with the available experimental values. In the bulk, our results show that the smallest activation energy barrier is 0.63 eV for substitutional <sup>3</sup>H diffusion with a diffusion coefficient of 3.25x10<sup>-12</sup> m<sup>2</sup>/s. After <sup>3</sup>H diffused from bulk to the surface, it could form different species (such as <sup>3</sup>H<sub>2</sub>, <sup>3</sup>H<sub>2</sub>O, C<sup>3</sup>H<sub>4</sub>) depending on the surface structure, vacancy types and the impurity carbon. Our results indicate that the <sup>3</sup>H<sub>2</sub> is the main product from γ-LiAlO<sub>2</sub> pellets. As the number of V<sub>Li</sub> vacancies and <sup>3</sup>H atoms increases under irradiation (<sup>3</sup>H-rich condition), <sup>3</sup>H<sub>2</sub>O release could increase from the surface of γ-LiAlO<sub>2</sub> pellets.

Jia, Ting↗

3D printing of additive structures for nuclear fuels

A method for manufacturing a nuclear fuel compact is provided. The method includes forming an additive structure, consolidating a fuel matrix around the additive structure, and thermally processing the fuel matrix to form a fuel compact in which the additive structure is encapsulated therein. The additive structure optionally includes a vertical segment and a plurality of arm segments that extend generally radially from the vertical segment for conducting heat outwardly toward an exterior of the fuel compact. In addition to improving heat transfer, the additive structure may function as burnable absorbers, and may provide fission product trapping.

Terrani, Kurt A.↗

3D printing of additive structures for nuclear fuels

A method for manufacturing a nuclear fuel compact is provided. The method includes forming an additive structure, consolidating a fuel matrix around the additive structure, and thermally processing the fuel matrix to form a fuel compact in which the additive structure is encapsulated therein. The additive structure optionally includes a vertical segment and a plurality of arm segments that extend generally radially from the vertical segment for conducting heat outwardly toward an exterior of the fuel compact. In addition to improving heat transfer, the additive structure may function as burnable absorbers, and may provide fission product trapping.

Terrani, Kurt A.↗