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DOE OSTI2024

Evaluating Material Design Principles for Calcium-Ion Mobility in Intercalation Cathodes

Multivalent-ion batteries offer an alternative to Li-based technologies, with the potential for greater sustainability, improved safety, and higher energy density, primarily due to their rechargeable system featuring a passivating metal anode. Although a system based on the Ca 2+ /Ca couple is particularly attractive given the low electrochemical plating potential of Ca 2+ , the remaining challenge for a viable rechargeable Ca battery is to identify Ca cathodes with fast ion transport. In this work, a high-throughput computational pipeline is adapted to (1) discover novel Ca cathodes in a largely unexplored space of empty intercalation hosts and (2) develop material design rules for Ca-ion mobility. One candidate from the screening, W 2 O 3 (PO 4 ) 2 , is confirmed to have a low Nudged Elastic Band (NEB) barrier of 168 meV within a one-dimensional (1D) ion percolation topology. This candidate is subsequently synthesized and electrochemically tested, achieving reversible Ca cycling with a capacity of 25 mA h/g. To further accelerate the screening for promising Ca intercalation electrodes, machine learning (ML) Random Forest (RF) and Extreme Gradient Boosting (XGB) classification models are created with local environment descriptors based on a large, structurally and chemically diverse dataset of minimum energy pathways, spanning over 5,000 density functional theory (DFT) site energy calculations. Accuracies of 92% are achieved, material design metrics are quantified, ML force-fields are leveraged in an accelerated iteration of the screening, and a total of 27 novel Ca cathode materials are highlighted for further investigation.

25 ENERGY STORAGE↗

DOE OSTI2023

Assessment of Modeling and Simulation Technical Gaps in Safety Analysis of High Burnup Accident-Tolerant Fuels

The United States nuclear industry is facing a strong challenge to maintain regulatory-required levels of safety while ensuring economic competitiveness to stay in business. Safety remains a key parameter for all aspects related to the operation of light water reactor (LWR) nuclear power plants (NPPs), and it can be achieved more economically by using a risk-informed ecosystem, such as that being developed by the Risk-Informed Systems Analysis (RISA) Pathway under the U.S. Department of Energy (DOE) Light Water Reactor Sustainability (LWRS) Program. The LWRS Program is promoting a wide range of research and development activities to maximize both the safety and economically efficient performance of NPPs through improved scientific understanding, especially given that many plants are considering second license renewal. The RISA Pathway has two main goals: The deployment of methodologies and technologies that enable better representation of safety margins and the factors that contribute to cost and safety, and; The development of advanced applications that enable cost-effective plant operation. As part of the RISA Pathway, the Enhanced Resilient Plant (ERP) project refers to an NPP where safety is improved by implementing various measures, such as accident-tolerant fuels (ATF), diverse and flexible coping strategy (FLEX), enhancements to plant components and systems, incorporation of augmented or new passive cooling systems, and utilization of advanced battery technologies. The objective of the ERP research is to use novel methods and computational tools to enhance existing reactors’ safety while reducing operational costs. Many U.S. utilities are targeting implementation of ATFs instead of traditional fuel in the near future since ATFs offer benefits in terms of improved performance and cost savings. The robust properties of ATF make it possible to extend the refueling cycle from 18 to 24 months in addition to the opportunity to use less of fuel. Extensive safety assessments are required to support regulatory requirements and obtain the approvals to use ATFs and the ERP project support the industry by developing novel effective methodologies for safety evaluations. In this project, the technical gaps in the modeling and simulation of the high burnup (HBU) ATF were assessed in terms of the fuel cladding behavior during the postulated accident events. The issues were identified in modeling the cladding deformation, the hydrodynamic change due to cladding deformation and the critical heat flux (CHF). The RELAP5-3D cladding deformation model was assessed by multiple verification tests and validation with the instrumented fuel assembly (IFA) experiment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Safety Analysis of FeCrAl Accident-Tolerant Fuels with Increased Enrichment and Extended Burnup

The U.S. nuclear industry is facing a strong challenge to maintain regulatory-required levels of safety while ensuring economic competitiveness to stay in business. Safety remains a key parameter for all aspects related to the operation of light water reactor nuclear power plants (NPPs), and it can be achieved more economically by using a risk-informed ecosystem, such as that being developed by the Risk-Informed Systems Analysis Pathway under the U.S. Department of Energy Light Water Reactor Sustainability Program. This program is promoting a wide range of research and development activities to maximize both the safety and economically efficient performance of NPPs through improved scientific understanding, especially given that many plants are considering a second license renewal. The Risk-Informed Systems Analysis Pathway has two main goals: (1) The deployment of methodologies and technologies that enable a better representation of the safety margins and factors that contribute to cost and safety, and (2) The development of advanced applications that enable cost-effective plant operation. As part of this pathway, the Enhanced Resilient Plant project refers to an NPP where safety is improved by implementing various measures, such as accident-tolerant fuels, diverse and flexible coping strategies, enhancements to plant components and systems, incorporation of augmented or new passive cooling systems, and utilization of advanced battery technologies. The objective of the Enhanced Resilient Plant project is to use novel methods and computational tools to enhance existing reactors’ safety while reducing operational costs. This report documents research and development conducted in support of deployment of accident-tolerant fuels. This project performed safety analyses for the steady-state normal operation, anticipated operational occurrences, and design-basis accidents of a representative four-loop pressurized water reactor model with Zr and FeCrAl accident-tolerant fuel clad with higher enrichment and burnup supporting plant refueling cycles of 18 and 24 months. The source terms and environmental impacts were studied for a large-break loss of coolant accident, including uncertainty analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Mitigation of Failure Propagation in Li-Ion Batteries

Propagation of thermal events from one damaged cell in a battery module to adjacent cells is a safety concern. A team of researchers from Sandia National Laboratories (SNL) and the National Renewable Energy Laboratory (NREL) have developed a “safety-map” to evaluate propensity for failure propagation. The model results were used to evaluate passive thermal management designs for Li-ion battery modules.

25 ENERGY STORAGE↗

DOE OSTI2021

High safety and cycling stability of ultrahigh energy lithium ion batteries

High-nickel layered oxide Li-ion batteries (LIBs) dominate the electric vehicle market, but their potentially poor safety and thermal stability remain a public concern. Here, we show that an ultrahigh-energy LIB (292 Wh kg –1 ) becomes intrinsically safer when a small amount of triallyl phosphate (TAP) is added to standard electrolytes. TAP passivates the electrode-electrolyte interfaces and limits the maximum cell temperature during nail penetration to 55°C versus complete cell destruction (>950°C) without TAP. The downside of this reliable safety solution is higher interfacial impedance and hence lower battery power; however, thermal modulation for battery operation around 60°C can restore power completely. When cycled at 60°C, the cell stabilized with TAP achieved 2,413 cycles at 76% capacity retention. Such an unconventional combination of interface-passivating electrolyte additive with cell thermal modulation renders the most energy-dense LIBs even safer than LiFePO 4 chemistry, while enjoying high power and cycling stability concurrently.

25 ENERGY STORAGE↗

DOE OSTI2025

The Effects of Manufacturing Techniques on Neutron-Irradiated C26M Mechanical Properties

Nuclear energy provides 13% of the total energy produced globally. To further improve the safety and reliability of nuclear reactors material challenges need to be successfully resolved. C26M/FeCrAl alloy systems can improve the safety and reliability of current Generation III reactors due to the potential benefits of a stable passivation layer from the Al, which can protect against corrosion, and promising mechanical performance at boiling- and light-water reactor temperatures. However, information is limited on how manufacturing techniques affect the mechanical performance of C26M in neutron-irradiated environments. In this research, C26M specimens were manufactured using three techniques and then irradiated at the Advanced Test Reactor at Idaho National Laboratory. This research aims to bridge this gap by investigating how the manufacturing techniques affects the mechanical performance of irradiated C26M at Generation III reactor relevant temperatures.

36 - MATERIALS SCIENCE↗

DOE OSTI2021

Al 2 O 3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

Among the many emerging technologies under investigation as alternatives to the successful Lithium-ion battery, the magnesium battery is promising due to the wide availability of magnesium, its high volumetric capacity, and the possibility for safety improvements. One of the largest challenges facing rechargeable magnesium batteries is the formation of a passivation layer at the Mg metal anode interface when reactive species in the electrolyte are reduced at the electrode-electrolyte interface. To control the solid electrolyte interphase in Lithium batteries, protective layers called artificial solid electrolyte interphase (ASEI) layers have been successful in improving Li metal anode performance. The approach of protecting Mg metal anodes from electrolyte degradation has been demonstrated by fewer studies in the literature than Li systems. In this work, we discuss the properties of Al 2 O 3 thin films deposited using atomic layer deposition as an artificial solid electrolyte interphase at the Mg anode. Our results demonstrate that Al 2 O 3 does prevent electrolyte degradation due to the reductive nature of Mg. However, undesirable properties such as defects and layer breakdown lead to Mg growth that causes soft-shorting. The soft-shorting occurs with and without the protection layer, indicating the ALD layer does not prevent it and hinders Al 2 O 3 from being an ideal candidate for a protection layer. Crucial effects of this layer on Mg electrochemistry at the interface were observed, including growth of Mg deposits leading to soft-shorting of the cell whose morphology showed a dependence on the Al 2 O 3 layer. These results may provide guidelines for the future design and development of protective ASEI layers for Mg anodes.

25 ENERGY STORAGE↗

DOE OSTI2026

Self-Healing Lithium Dendrites through Spontaneous Passivating Layer Formation for Stable Solid-State Lithium–Metal Batteries

All-solid-state lithium–metal batteries have attracted significant attention, owing to their high energy density and superior safety. However, lithium–metal penetration through the solid electrolyte, leading to short-circuiting, remains a critical failure mode that demands comprehensive mitigation strategies. Most existing strategies are effective only prior to the initiation of lithium-dendrite formation and fail once dendrites begin to propagate through the electrolyte. In this study, we propose a self-healing mechanism in which the penetrated lithium reacts with a self-healing agent to form a passivating layer along the particle boundaries. Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was incorporated into a Li 6 PS 5 Cl solid electrolyte as the self-healing agent to suppress lithium-dendrite propagation even after dendrite formation initiated under high current densities. The self-healing induced by LiTFSI was verified through comprehensive experimental analyses and was further demonstrated in a full-cell configuration. Moreover, LiTFSI incorporation plays an important role in increasing the critical current density by reducing the overall electronic conductivity of the solid electrolyte and facilitating the formation of a robust LiF-containing solid-electrolyte interphase.

25 ENERGY STORAGE↗

DOE OSTI2026

Phenomena Identification and Ranking Tables for High Temperature Gas-Cooled Microreactors

Micro-scaled high-temperature gas-cooled reactors (micro-HTGRs) offer a promising option for reliable power in remote or off-grid locations. While the safety characteristics of modular HTGRs have been widely studied, a micro-HTGR configuration alters several key thermal-fluid phenomena that govern both normal operation and passive decay-heat removal. In many proposed concepts, the reactor vessel is oriented horizontally and integrated into an ISO shipping container to enhance transportability and modular deployment. This report documents a Phenomena Identification and Ranking Table (PIRT) exercise focused on the thermal hydraulic safety phenomena relevant to all micro-HTGRs. The objective is to systematically identify, describe, and rank the importance, uncertainty, and modeling complexity of the key phenomena that control core and vessel temperatures during normal operation, pressurized conduction cooldown (PCC), and depressurized conduction cooldown (with air ingress) conditions.

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Degradation of Lithium Iron Phosphate Sulfide Solid-State Batteries by Conductive Interfaces

The superionic solid-state argyrodite electrolyte Li 6 PS 5 Br can improve lithium and lithium-ion batteries' safety and energy density. Despite many reports validating the conductivity of this electrolyte, it still suffers from passivating electrode degradation mechanisms. At first analysis, lithium iron phosphate (LFP) should be more thermodynamically stable in contact with sulfide electrolytes. However, without substantial improvements to interfacial engineering, we find that LFP is not inherently stable against Li 6 PS 5 Br. We hypothesize argyrodite oxidation favorably competes with LFPAs delithiation, insulating the electrolyte-electrode interface and causing large overpotential losses. We show that compared to LiNi x Mn y Co z O 2 , LFP has no actual electrochemical stability advantage despite operating at a lower voltage. We utilize tender energy XAS and XPS to show that chemical reactions occur between LFP and the Li 6 PS 5 Br solid electrolyte and these reactions are exacerbated by cycling. We also show that electrochemical degradation occurs at the interface between the solid electrolyte ion conductor and any electron conductor, namely the active material and carbon additives. We further demonstrate that LiNbO 3 cathode coatings on LFP can delay electrochemical degradation by electronically insulating the LFP-sulfide electrolyte interface but not prevent its occurrence at the carbon-electrolyte interface.

25 ENERGY STORAGE↗

DOE OSTI2021

Development of electronically passivating surfaces to enhance battery performance

For many decades, lithium metal batteries (LMBs) have been studied for their high energy density, though they suffer from high reactivity, which safety concerns such as explosions and fires. These events can occur as a result of degradation due to redox reactions and lithium morphology that evolve during cycling. Mostly, the failure is caused by the electrolyte degradation leading to the creation of a solid electrolyte interphase (SEI), which tends to induce electron leakage, lithium dendrite growth, and capacity decay. SEI formation is practically inevitable. This work investigated the minimization of degradation events by modifying different battery configurations. Modifications were made by exchanging electrolytes, electrode surfaces, and even annexing innovative components. Our goal is to achieve a configuration where Li-ion transfer is facilitated, and electron transfer is limited which would enable a longer lithium metal battery life cycle. When performing these modifications and testing their electrochemical performance, a current reduction was observed when the electrodes were spontaneously coated with preformed SEI. Herein several classes of artificial SEI layers are explored for their ability to form passivating layers through use of a redox active molecule.

25 ENERGY STORAGE↗

DOE OSTI2025

Forced flow transient safety analysis of irradiation device with adjustable orifice for research reactor fuel assemblies

The Belgium Reactor 2 (BR2) of the Belgian Nuclear Research Centre (SCK CEN) has several irradiation devices or rigs that are dedicated to the fuel performance and qualification demonstration testing of research reactor fuels. In support of the U.S. High Performance Research Reactor (USHPRR) LEU conversion project, a new flexible irradiation apparatus, MUSTANG-R, has been constructed. SCK CEN has completed the design and safety study, in cooperation with Idaho National Laboratory (INL) and Argonne National Laboratory (ANL), to allow for the irradiation testing of a full-size fuel assembly in a 200 mm diameter channel in the BR2 reactor. The moveable valve is a key design feature of the device and acts like an adjustable orifice enhancing or restricting the flow through a coolant channel inlet located in the BR2 upper plenum. This moveable valve allows the flow through the device to be adjusted prior to each BR2 cycle to obtain the necessary conditions for the fuel qualification test. This ensures accurate and representative thermal-hydraulic conditions of the fuel design are achieved. The device was designed and qualified as passively safe, implying verification by a combination of mechanical and thermal-hydraulic analysis and testing. This includes characterization of the safety margin required for a scenario where the moveable valve is assumed to be erroneously closed during irradiation. A simplified and conservative method is proposed for analyzing the corresponding forced flow transient using a critical heat flux criterion. In conclusion, this allows the required minimum valve opening to be determined for the experiments' design and safety studies.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Modeling glass degradation and release of radionuclides from vitrified waste for performance assessment simulations

The release of radionuclides initially encapsulated in a slowly degrading solid waste form and contained in an eventually corroding canister defines the source term for numerical simulations for the assessment of a geologic repository for high-level radioactive waste. While the details of waste degradation, canister corrosion, and dissolution and mobilization of the radionuclides in pore water include complex chemical reaction and transport processes that are coupled to the thermal, hydrological, microbiological, and mechanical conditions in the repository, the source-term model suitable for use in a numerical performance assessment model should be a defensible abstraction of these mechanisms. We developed a radiological source-term model and implemented it into a non-isothermal flow and transport simulator. While the proposed source-term model is applicable to various waste forms, canister systems, and disposal concepts, we specifically considered radionuclide releases from vitrified high-level waste placed in a cylindrical canister disposed in a deep vertical borehole repository. In this model, waste degradation is a function of temperature, and it can be adjusted to evaluate the influence of and propagate uncertainties in pH, passivation reactions, and chemical conditions as well as geometrical factors. The time-dependent, congruent release of safety-relevant radionuclides present in the decaying inventory is then calculated. Finally, the radionuclides are mobilized by diffusive and advective transport according to the thermo-hydraulic conditions prevailing in the near field of the repository, from where they migrate through the geosphere to the accessible environment. We examine the influence of the source-term model’s parameters on performance assessment calculations through sensitivity and uncertainty propagation analyses, identifying influential factors and confirming the upper bound of their impact. These considerations align with the overarching goal of repository design, which is to demonstrate that engineered and natural barriers can collectively delay radionuclide migration for timescales far exceeding human planning, thereby providing multiple, redundant barriers against environmental contamination.

iTOUGH2↗

DOE OSTI2021

Modular High Temperature Gas-cooled Reactor: Accident Analysis

Types of Potential Accidents and Reactor Response Codes and Tools Experimental Validation Safety Analysis Approach Licensing Modernization Project Use of PRA in LMP, ASME/ANS, Non-LWR PRA Standard Methods for Incorporating Passive System Reliability into a PRA

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Development of a Reconstruction Methodology Based on X-Ray Computed Tomography to Generate Realistic 3D Concrete Microstructures in MOSAIC

Despite being passive components, concrete structures represent a major capital investment in nuclear power plants. However, some concrete components are critical for the safety and long-term operation of the reactors: the concrete containment building protects the reactors from external aggression. The concrete biological shield (CBS) contains the radiation exiting the reactor to protect equipment and personnel. Depending on the design, the CBS also has a function for supporting the reactor’s systems. This function needs to be ensured in-service and during accident scenarios. After several decades of use, the CBS is exposed to high-energy irradiation over an extended operation time, exceeding the fluence level currently considered detrimental for the concrete’s structural properties. Such conditions occur at different times depending on the reactor’s operation and design. Nevertheless, from the perspective of subsequent license application, it is mandatory to assess the potential effects of prolonged irradiation on concrete. Unlike steel components, concrete structures are built with local constituents (cement, sand, and coarse aggregates) to avoid prohibitive transportation costs. Thus, concrete performance is determined by the tolerance or the susceptibility of its constituents against any aging mechanism. The tolerance against irradiation of the CBSs may vary greatly among the 56 nuclear power plants and 93 nuclear power reactors that form the current US light-water reactor fleet. Irradiation-induced degradation is mainly a result of amorphization-induced expansions of the silicated minerals present in the aggregates. The neutron irradiation–induced expansion varies from one rock-forming mineral to another: well framework–structured silicates (e.g., quartz and feldspars) exhibit higher swelling than chained (e.g., pyroxene) or isolated silicates (e.g., garnet). Silicates make up nearly 90% of the Earth’s crust. Other common minerals present in construction aggregates are carbonates found, for example, in limestone. Irradiated carbonates exhibit only very minor expansions.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Metal fuel relocation experiments with pressure injection

A pool-type sodium-cooled fast reactor (SFR) using metal fuels has a number of inherent safety features that can support benign consequences for design basis accidents (DBAs). Even in postulated severe accident conditions, the core is designed to remain under sub-critical condition in a passive coolable geometry. In case of the postulated severe accidents in SFRs, fuel relocation in the core region along the coolant channel is an important negative reactivity feedback factor that lowers the reactor power level and consequently eliminates the possibility of recriticality. Therefore, understanding the relocation behavior of fuels and the coolability of the relocated fuels in the postulated severe accident is one of the most important factors in the safety assessment of SFRs. In the present study, the relocation behavior of the metal fuel in a pin bundle geometry was investigated by injecting the metal fuels into the coolant channels with pressure. The first metal fuel relocation with pressure injection (RPI-1) experiment showed that many of the metal fuels levitated to upper plenum. In case of RPI-2 experiment, the Real Time X-ray Video System (RTXVS) was constructed and used to obtain a real time X-ray video of the experiment. This real time X-ray video clearly showed the relocation behavior of the pressure injected metallic uranium in the sodium coolant channel. Through this video, it was confirmed that part of the fuel was dispersed downward and part of the fuel was dispersed upward, and the relocation behavior of the injected fuel proceeded simultaneously in the downward and upward directions. So, it can be concluded that in case of pressure injection of the metallic fuel, there is a possibility that the metallic fuel can be quickly removed from the core region, resulting in a negative reactivity feedback effect.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Electronic and Geometric Contributors to Hydrogen Binding in Uranium Oxide Grain Boundaries

Hydrogen induced corrosion of uranium, which leads to the formation of toxic and pyrophoric UH 3 , raises significant safety concerns for long-term storage of nuclear materials. Previous work suggests hydrogen diffuses through the grain boundaries (GBs) of the passivating oxide layer to initiate hydriding reactions. However, the atomistic mechanisms underlying this phenomenon and the structural factors that control its initiation are not well understood. To address this knowledge gap, here we use a high-throughput density functional theory (DFT) workflow to investigate the adsorption of H and H 2 in the defective bulk UO 2 . Specifically, we have exhaustively investigated the adsorption of H (107 sites) and H 2 (26 sites) in three different coincident site lattice (CSL) GBs: Σ3, Σ5, and Σ9. Compared to the binding energies in pristine UO 2 , we observe significantly stronger hydrogen adsorption at these GB sites. Interestingly, we find that the trends in H and H 2 adsorption vary considerably across the three GB models. In particular, while a small number of sites in Σ5 and Σ9 show exothermic adsorption of H and H 2 , respectively, no such sites are found in Σ3. These results provide fundamental atomistic insights that could guide the development of future corrosion mitigation strategies for the storage of nuclear materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Design Status and Experimental Strategy for Initial Molten Salt Irradiation Experiments in HFIR

The development and deployment of molten salt reactor (MSR) technologies require experimental capabilities that can evaluate molten fuel salt behavior and structural material performance under representative irradiation conditions. Although modeling and separate effects testing provide important insight, there remains a critical lack of in-pile data that capture the coupled effects of neutron irradiation, temperature, salt chemistry, and time. Informed by lessons learned from historical MSR programs and recent international irradiation efforts, this report presents a structured approach to addressing existing gaps in molten salt irradiation testing using the High Flux Isotope Reactor (HFIR). A phased irradiation strategy is presented that incrementally increases experimental complexity while managing cost, risk, and facility constraints. The framework progresses from passive, nonfueled static capsule experiments to fueled, instrumented, and ultimately circulating molten salt systems, providing a pathway for materials screening, mechanistic understanding, and qualification-relevant testing. The report defines a near-term Phase 1 passive capsule concept, associated irradiation conditions, and a conceptual post-irradiation examination strategy. Ongoing modeling, out-of-pile testing, and safety analysis activities are described to support continued capability maturation and to enable future phases of molten salt irradiation testing in support of MSR technology deployment.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗