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DOE OSTI2025

Stabilization of Preternatural Barium Oxidation States as an Unexpected Byproduct of β-Decay: Discovery of a New Halide Semiconductor Alloy

137 Cs has a wide range of roles in the nuclear industry. The solid material, safely encapsulated in CsCl as 137 CsCl, is stored as fission product waste from nuclear power production and legacy waste from nuclear weapons production; it has also served as a radiation source in food and sewage irradiators as well as medical devices. However, because of the solubility of the chloride salt and the relatively high specific activity of 137 Cs, damaged or broken capsules can lead to severe radiological accidents. Safe capsule design and material recycling are complicated by the unclear structural evolution during β-decay, which remains ambiguous due to the differing oxidation states of Cs (1+) and Ba (2+). Here, in this study, we use first-principles calculations to investigate the evolving structure–property relationships of Cs 1–x Ba x Cl during β-decay. Despite the well-established 2+ formal oxidation state of alkali-earth metals, we find that Ba 1+ can be stabilized in the form of a mixed-valence alloy at low concentrations. Specifically, we identify three regimes for the β-decay of 137 Cs into CsCl: Ba-doped CsCl (Ba ≤ 14%), wherein Ba has the expected 2+ oxidation state; Cs–Ba–Cl alloys, where Ba has a mix of the usual Ba 2+ and highly unusual Ba 1+ oxidation state in the form of a quasi-disordered mixed-valence alloy (Ba = 25%); and phase separation into a CsCl + BaCl 2 + Ba (m) mechanical mixture, where Ba reverts to its expected 2+ oxidation state (Ba > 25%). Surprisingly, the Cs 0.75 Ba 0.25 Cl mixed-valence alloy is a narrow indirect band gap semiconductor (1.05 eV) despite the insulating nature of both CsCl and BaCl 2 . It also exhibits strongly excitonic polarized optical properties, has glass-like ultralow thermal conductivity (directional average of 0.21 W/mK at 300 K), and shows greater resistance to deformation under both tensile and volumetric strengths compared with the original CsCl structure (e.g., shear and Young’s modulus of 9.04 and 31.62 GPa, respectively). These findings imply that transmutation of 137 Cs leads to highly unusual chemical bonding that stabilizes Ba 1+ in local regions of the quasi-disordered Cs 0.25 Ba 0.75 Cl, resulting in anomalous physical properties. Moreover, this discovery provides valuable insight for safe nuclear waste capsule design, which can aid in preventing environmental or human exposure to radioactive materials.

Fuhr, Addis S. [Oak Ridge National Laboratory (ORN↗

DOE OSTI2015

Where Are We Heading in Nanotechnology Environmental Health and Safety and Materials Characterization?

Every chemist, material scientist, physicist, engineer, or commercial enterprise involved in the synthesis and/or production of engineered nanomaterials (ENM) or nano-enabled products aspires to develop safe materials. Nanotechnology environmental health and safety (nanoEHS) is a research discipline that involves the study of the possible adverse health and biological effects that nanomaterials may have on humans and environmental organisms and ecosystems. NanoEHS research has provided a body of experimental evidence indicating the possibility of hazardous outcomes as a result of the interactions of unique ENM physicochemical properties with similar scale processes occurring at a wide range of nano/bio interfaces, including at biomolecular, cellular, subcellular, organ, systemic, whole organism, or ecosystems levels. This projected hazard and risk potential warrants rigorous attention to safety assessment, safe use, safe implementation, benign design, regulatory oversight, governance, and public awareness to address the possibility and prevention of nanotoxicity, now or at any time in the future.1 Thus, we should understand the properties of the ENMs that are responsible for the toxicological response, so that we can re-engineer their physicochemical characteristics for risk prevention and safer ENM design.2 However, in spite of widespread use, no human toxicological disease or major environmental impact has been reported for ENMs. Thus, while “Nanotoxicology” is a thriving sub-discipline of Nano-EHS, the use of the “root” word toxicology may elicit a feeling that nanomaterials are inherently toxic despite the fact that toxicity has not been established in real-life use so far. As a community, we may want to rename this sub-discipline as “Nanosafety,” since the objective is to use toxicology information to guide the design of safer nanomaterials for use in medicine, biology, electronics, lighting systems, etc. At ACS Nano, we are interested in publishing articles and forward-looking Perspectives and Reviews that determine and establish ENM physicochemical properties, structure-activity relationships, catalytic effects at the nano/bio interface, mechanistic injury responses, in vitro to in vivo prediction making, safer-by design strategies, actionable screening and detection methods, hazard and risk ranking, fate and transport, ENM categorization, theory and modeling, societal implications, and regulatory/governance decisions.3 Context is important in the immediate and longer-range impact of this research, as we are interested in realistic nanoEHS exposure scenarios conducted with systematic variation of ENM physicochemical properties rather than investigations of a single or a limited number of materials in isolated in vitro studies that only address cytotoxicity at unrealistic doses. In order to make these data useful for researchers, government and regulatory agencies, and other interested parties, these studies, where possible, should include either appropriate positive and negative controls or benchmark materials to answer the important question, “as compared to what?” Dosimetry should be explained in terms of appropriate dose metrics relative to the type of materials, their mechanisms of injury, and exposure conditions, using in vitro to in vivo extrapolations where possible. Another important component of these studies includes appropriate physicochemical characterization of the nanomaterials.

Nel, Andre↗

DOE OSTI2017

Reversible capture and release of Cl 2 and Br 2 with a redox-active metal–organic framework

Extreme toxicity, corrosiveness, and volatility pose serious challenges for the safe storage and transportation of elemental chlorine and bromine, which play critical roles in the chemical industry. Solid materials capable of forming stable nonvolatile compounds upon reaction with elemental halogens may partially mitigate these challenges by allowing safe halogen release on demand. Here we demonstrate that elemental halogens quantitatively oxidize coordinatively unsaturated Co(II) ions in a robust azolate metal-organic framework (MOF) to produce stable and safe-to-handle Co(III) materials featuring terminal Co(III)-halogen bonds. Thermal treatment of the oxidized MOF causes homolytic cleavage of the Co(III)-halogen bonds, reduction to Co(II), and concomitant release of elemental halogens. The reversible chemical storage and thermal release of elemental halogens occur with no significant losses of structural integrity, as the parent cobaltous MOF retains its crystallinity and porosity even after three oxidation/reduction cycles. Finally, these results highlight a material operating via redox mechanism that may find utility in the storage and capture of other noxious and corrosive gases.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Addressing the Safety of Next-Generation Batteries

Owing to increasing demand for low-cost energy storage with secure material supply chains, the battery community is approaching a pivotal shift beyond conventional lithium-ion (Li-ion) towards next-generation cells. Technologies that include alkali-metal anodes, solid electrolytes and earth-abundant materials such as sodium (Na) and sulfur (S) are reaching commercialization in cells. The abuse tolerance and thermal runaway hazards of such technologies diverge from conventional Li-ion cells. Consequently, designing safe batteries with next-generation materials requires a holistic approach to characterize cells and to understand their responses to abuse conditions from the beginning to the end of life. Here we provide a Perspective on how the safety and abuse tolerance of cells are likely to change for up-and-coming technologies; challenges and opportunities for reimagining safe cell and battery designs; gaps in our knowledge; capabilities for understanding the hazards of thermal runaway and how to address them; how standard abuse tests may need to adapt to new challenges; and how research needs to support affected professionals, from pack designers to first responders, to manage hazards and ensure safe roll-out of next-generation cells into applications like electric vehicles (EVs). Finally, given the large number of next-generation technologies being explored, we encourage giving priority to safety-focused research in proportion to the rate of manufacturing scale-up of each specific technology.

25 ENERGY STORAGE↗

DOE OSTI2014

Non-linear dynamic characteristics and optimal control of giant magnetostrictive film subjected to in-plane stochastic excitation

The non-linear dynamic characteristics and optimal control of a giant magnetostrictive film (GMF) subjected to in-plane stochastic excitation were studied. Non-linear differential items were introduced to interpret the hysteretic phenomena of the GMF, and the non-linear dynamic model of the GMF subjected to in-plane stochastic excitation was developed. The stochastic stability was analysed, and the probability density function was obtained. The condition of stochastic Hopf bifurcation and noise-induced chaotic response were determined, and the fractal boundary of the system's safe basin was provided. The reliability function was solved from the backward Kolmogorov equation, and an optimal control strategy was proposed in the stochastic dynamic programming method. Numerical simulation shows that the system stability varies with the parameters, and stochastic Hopf bifurcation and chaos appear in the process; the area of the safe basin decreases when the noise intensifies, and the boundary of the safe basin becomes fractal; the system reliability improved through stochastic optimal control. Finally, the theoretical and numerical results were proved by experiments. The results are helpful in the engineering applications of GMF.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Stochastic bifurcation and fractal and chaos control of a giant magnetostrictive film-shape memory alloy composite cantilever plate subjected to in-plane harmonic and stochastic excitation

Stochastic bifurcation and fractal and chaos control of a giant magnetostrictive film–shape memory alloy (GMF–SMA) composite cantilever plate subjected to in-plane harmonic and stochastic excitation were studied. Van der Pol items were improved to interpret the hysteretic phenomena of both GMF and SMA, and the nonlinear dynamic model of a GMF–SMA composite cantilever plate subjected to in-plane harmonic and stochastic excitation was developed. The probability density function of the dynamic response of the system was obtained, and the conditions of stochastic Hopf bifurcation were analyzed. The conditions of noise-induced chaotic response were obtained in the stochastic Melnikov integral method, and the fractal boundary of the safe basin of the system was provided. Finally, the chaos control strategy was proposed in the stochastic dynamic programming method. Numerical simulation shows that stochastic Hopf bifurcation and chaos appear in the parameter variation process. The boundary of the safe basin of the system has fractal characteristics, and its area decreases when the noise intensifies. The system reliability was improved through stochastic optimal control, and the safe basin area of the system increased.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Scenario development for safety assessment in deep geologic disposal of high-level radioactive waste and spent nuclear fuel: A review

Radiation and radioactive substances result in the production of radioactive wastes which require safe management and disposal to avoid risks to human health and the environment. To ensure permanent safe disposal, the performance of a deep geological repository for radioactive waste is assessed against internationally agreed risk-based standards. Assessing postclosure safety of the future system's evolution includes screening of features, events, and processes (FEPs) relevant to the situation, their subsequent development into scenarios, and finally the development and execution of safety assessment (SA) models. Global FEP catalogs describe important natural and man-made repository system features and identify events and processes that may affect these features into the future. By combining FEPs, many of which are uncertain, different possible future system evolution scenarios are derived. Repository licensing should consider both the reference or “base” evolution as well as alternative futures that may lead to radiation release, pollution, or exposures. Scenarios are used to derive and consider both base and alternative evolutions, often through production of scenario-specific SA models and the recombination of their results into an assessment of the risk of harm. Furthermore, while the FEP-based scenario development process outlined here has evolved somewhat since its development in the 1980s, the fundamental ideas remain unchanged. A spectrum of common approaches is given here (e.g., bottom–up vs. top–down scenario development, probabilistic vs. bounding handling of uncertainty), related to how individual numerical models for possible futures are converted into a determination as to whether the system is safe (i.e., how aleatoric uncertainty and scenarios are integrated through bounding or Monte Carlo approaches).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

TH-C-18C-01: MRI Safety

Clinical diagnostic medical physicists may be responsible for implementing and maintaining a comprehensive MR safety program. Accrediting bodies including the ACR, IAC, Radsite and The Joint Commission each include aspects of MR Safety into their imaging accreditation programs; MIPPA regulations further raise the significance of non-compliance. In addition, The Joint Commission recently announced New and Revised Diagnostic Imaging Standards for accredited health care organizations which include aspects of MR Safety. Hospitals and clinics look to the physicist to understand guidelines, regulations and accreditation requirements related to MR safety. The clinical medical physicist plays a significant role in a clinical practice by understanding the physical basis for the risks and acting as a facilitator to successfully implement a safety program that provides well-planned siting, allows for the safe scanning of certain implanted devices, and helps radiologists manage specific patient exams. The MRI scanning of specific devices will be discussed including cardiac pacemakers and neurostimulators such as deep brain stimulators. Furthermore for sites involved in MR guided interventional procedures, the MR physicist plays an essential role to establish safe practices. Creating a framework for a safe MRI practice includes the review of actual safety incidents or close calls to determine methods for prevention in the future. Learning Objectives: Understand the requirements and recommendations related to MR safety from accrediting bodies and federal regulations. Understand the Medical Physicist's roles to ensure MR Safety. Identify best practices for dealing with implanted devices, including pacemakers and deep brain stimulators. Review aspects of MR safety involved in an MR guided interventional environment. Understand the important MR safety aspects in actual safety incidents or near misses.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2015

SU-E-T-649: Quality Assurances for Proton Therapy Delivery Equipment

Purpose: The number of proton therapy centers has increased dramatically over the past decade. Currently, there is no comprehensive set of guidelines that addresses quality assurance (QA) procedures for the different technologies used for proton therapy. The AAPM has charged task group 224 (TG-224) to provide recommendations for QA required for accurate and safe dose delivery, using existing and next generation proton therapy delivery equipment. Methods: A database comprised of QA procedures and tolerance limits was generated from many existing proton therapy centers in and outside of the US. These consist of proton therapy centers that possessed double scattering, uniform scanning, and pencil beams delivery systems. The diversity in beam delivery systems as well as the existing devices to perform QA checks for different beam parameters is the main subject of TG-224. Based on current practice at the clinically active proton centers participating in this task group, consensus QA recommendations were developed. The methodologies and requirements of the parameters that must be verified for consistency of the performance of the proton beam delivery systems are discussed. Results: TG-224 provides procedures and QA checks for mechanical, imaging, safety and dosimetry requirements for different proton equipment. These procedures are categorized based on their importance and their required frequencies in order to deliver a safe and consistent dose. The task group provides daily, weekly, monthly, and annual QA check procedures with their tolerance limits. Conclusions: The procedures outlined in this protocol provide sufficient information to qualified medical physicists to perform QA checks for any proton delivery system. Execution of these procedures should provide confidence that proton therapy equipment is functioning as commissioned for patient treatment and delivers dose safely and accurately within the established tolerance limits. The report will be published in late 2015.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2016

SU-F-T-505: A Novel Approach for Sparing Critical Organs at Risk for Cancer Patients Undergoing Radiation Oncology Treatments

Purpose: A major goal of an effective radiation treatment plan is to deliver the maximum dose to the tumor while minimizing radiation exposure to the surrounding normal structures. For example, due to the radiation exposure to neighboring critical structures during prostate cancer treatment, a significant increase in cancer risk was observed for the bladder (77%) and the rectum (105%) over the following decade. Consequently, an effective treatment plan necessitates limiting the exposure to such organs which can best be achieved by physically displacing the organ at-risk. The goal of this study is to present a prototype for an organ re-positioner device designed and fabricated to physically move the rectum away from the path of radiation beam during external beam and brachytherapy treatments. This device affords patient comfort and provides a fully controlled motion to safely relocate the rectum during treatment. Methods: The NiTi shape memory alloy was designed and optimized for manufacturing a rectal re-positioner device through cooling and heating the core alloy for its shaping. This has been achieved through a prototyped custom designed electronic circuit in order to induce the reversible austenitic transformation and was tested rigorously to ensure the integrity of the actuated motion in displacement of the target anatomy. Results: The desirable NiTi shape-setting was configured for easy insertion and based on anatomical constraint. When the final prototype was evaluated, accuracy and precision of the maximum displacement and temperature changes revealed that the device could safely be used within the target anatomy. Conclusion: The organ re-positioner device is a promising tool that can be implemented in clinical setting. It provides a controlled and safe displacement of the delicate organ(s) at risk. The location of the organ being treated could also be identified using conventional onboard imaging devices or MV imaging available on-board most modern clinical accelerators.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2016

SU-G-JeP3-08: Robotic System for Ultrasound Tracking in Radiation Therapy

Purpose: For safe and accurate real-time tracking of tumors for IGRT using 4D ultrasound, it is necessary to make use of novel, high-end force-sensitive lightweight robots designed for human-machine interaction. Such a robot will be integrated into an existing robotized ultrasound system for non-invasive 4D live tracking, using a newly developed real-time control and communication framework. Methods: The new KUKA LWR iiwa robot is used for robotized ultrasound real-time tumor tracking. Besides more precise probe contact pressure detection, this robot provides an additional 7th link, enhancing the dexterity of the kinematic and the mounted transducer. Several integrated, certified safety features create a safe environment for the patients during treatment. However, to remotely control the robot for the ultrasound application, a real-time control and communication framework has to be developed. Based on a client/server concept, client-side control commands are received and processed by a central server unit and are implemented by a client module running directly on the robot’s controller. Several special functionalities for robotized ultrasound applications are integrated and the robot can now be used for real-time control of the image quality by adjusting the transducer position, and contact pressure. The framework was evaluated looking at overall real-time capability for communication and processing of three different standard commands. Results: Due to inherent, certified safety modules, the new robot ensures a safe environment for patients during tumor tracking. Furthermore, the developed framework shows overall real-time capability with a maximum average latency of 3.6 ms (Minimum 2.5 ms; 5000 trials). Conclusion: The novel KUKA LBR iiwa robot will advance the current robotized ultrasound tracking system with important features. With the developed framework, it is now possible to remotely control this robot and use it for robotized ultrasound tracking applications, including image quality control and target tracking.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2020

Resilient Distributed Field Estimation

We study resilient distributed field estimation under measurement attacks. A network of agents or devices measures a large, spatially distributed physical field parameter. An adversary arbitrarily manipulates the measurements of some of the agents. Each agent's goal is to process its measurements and information received from its neighbors to estimate only a few specific components of the field. Here, we present SAFE, the saturating adaptive field estimator, a consensus + innovations distributed field estimator that is resilient to measurement attacks. Under sufficient conditions on the compromised measurement streams, the physical coupling between the field and the agents' measurements, and the connectivity of the cyber communication network, SAFE guarantees that each agent's estimate converges almost surely to the true value of the components of the parameter in which the agent is interested. Finally, we illustrate the performance of SAFE through numerical examples.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2018

A Coupled Electrochemical-Thermal Failure Model for Predicting the Thermal Runaway Behavior of Lithium-Ion Batteries

Thermal runaway is always a troublesome problem that hinders the safe application of high energy lithium-ion batteries. There is an urgent need to interpret the voltage and temperature changes and their underlying mechanisms during thermal runaway, in order to guide the safe design of a battery system. This paper is dedicated to building a coupled electrochemical-thermal model that can well predict the voltage drop and temperature increase during thermal runaway. The model can capture the underlying mechanism of 1) the capacity degradation under high temperature; 2) the internal short circuit caused by the thermal failure of the separator; and 3) the chemical reactions of the cell components that release heat under extreme temperature. The model is validated using by experimental data, therefore the modeling analysis has high fidelity. We employ the model to analyze 1) the capacity degradation under extreme temperature; 2) the influence of the SEI decomposition and regeneration on the thermal runaway behavior; 3) the heat generation by internal short circuit in the thermal runaway process. In conclusion, the discussions presented here help extend the usage of lithium-ion batteries at extreme high temperature (>80 degrees C), and guide the safe design of lithium-ion batteries with less hazard level during thermal runaway.

25 ENERGY STORAGE↗

DOE OSTI2020

Heat Generation versus Heat Dissipation Maps for Batteries (Battery Safety Maps) [SWR-21-27]

NREL's Battery Safety Map (Heat Generation versus Heat Dissipation Maps for Batteries) generates a response surface that is grouped into regions where the battery is deemed safe from the propagation of thermal runaway, those where an engineering solution would render the battery safe, and finally instances where thermal runaway is inevitable. The demarcation for the different regions is provided by specifications or constraints imposed by the end user. NREL's Battery Safety Map is a user-defined subroutine that sweeps through a set of parameters describing the operating conditions and short-circuit scenarios for battery safety simulations. For each run, the electrochemical-thermal model implementing reaction kinetics and gas generation are run to evaluate the amount of heat generated. A thermal model then captures the amount of heat dissipation based on boundary conditions defined (e.g., forced convection, constant temperature at the surface, etc.). Based on the rate of heat transfer and the amount of heat generated, each run is classified into "safe," "mitigation possible," or "unsafe" zones. These categories are defined based on constraints or tolerance specifications provided by the end user.

Santhanagopalan, Shriram↗

DOE OSTI2018

Development of the Electromagnetic Boom and MOP System (EMOP)

Several large-scale oil spills typically occur in the USA and other places around the world. Such events threaten the Great Lakes as well. The cleanup process is not necessarily efficient or environmentally safe. In addition, the remediation and recovery process is time consuming, expensive and can lead to harmful environmental effects. An innovative electromagnetic approach by Natural Science, LLC uses materials that are reusable, recoverable, and environmentally safe. When micron-sized magnetite (Fe3O4) particles are dispersed in oil on water, the particles form a unique and preferential bond with the oil due to a combination of forces, e.g. Van der Waals. Magnetic fields can then be used to manipulate, trap and remove the oil in an environmentally safe manner with high efficiency. In the case of oil spills on water, the water becomes the primary transport medium for manipulating the oil. Videos demonstrating the process will be shown. Both the particles and the oil are recaptured and separated for reuse. This process is being applied to electromagnetic systems that can replace and/or increase the efficiency of the passive boom and skimmer systems used today.

43 PARTICLE ACCELERATORS↗

DOE OSTI2015

Risk Management for Sodium Fast Reactors.

Accident management is an important component to maintaining risk at acceptable levels for all complex systems, such as nuclear power plants. With the introduction of self - correcting, or inherently safe, reactor designs the focus has shifted from management by operators to allowing the syste m's design to manage the accident. While inherently and passively safe designs are laudable, extreme boundary conditions can interfere with the design attributes which facilitate inherent safety , thus resulting in unanticipated and undesirable end states. This report examines an inherently safe and small sodium fast reactor experiencing a beyond design basis seismic event with the intend of exploring two issues : (1) can human intervention either improve or worsen the potential end states and (2) can a Bayes ian Network be constructed to infer the state of the reactor to inform (1). ACKNOWLEDGEMENTS The author s would like to acknowledge the U.S. Department of E nergy's Office of Nuclear Energy for funding this research through Work Package SR - 14SN100303 under the Advanced Reactor Concepts program. The authors also acknowledge the PRA teams at A rgonne N ational L aborator y , O ak R idge N ational L aborator y , and I daho N ational L aborator y for their continue d contributions to the advanced reactor PRA mission area.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2015

Advance Liquid Metal Reactor Discrete Dynamic Event Tree/Bayesian Network Analysis and Incident Management Guidelines (Risk Management for Sodium Fast Reactors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2015

Interim Status Report for Risk Management for SFRs

Accident management is an important component to maintaining risk at acceptable levels for all complex systems, such as nuclear power plants. With the introduction of passive, or inherently safe, reactor designs the focus has shifted from management by operators to allowing the system's design to take advantage of natural phenomena to manage the accident. Inherently and passively safe designs are laudable, but nonetheless extreme boundary conditions can interfere with the design attributes which facilitate inherent safety, thus resulting in unanticipated and undesirable end states. This report examines an inherently safe and small sodium fast reactor experiencing a variety of beyond design basis events with the intent of exploring the utility of a Dynamic Bayesian Network to infer the state of the reactor to inform the operator's corrective actions. These inferences also serve to identify the instruments most critical to informing an operator's actions as candidates for hardening against radiation and other extreme environmental conditions that may exist in an accident. This reduction in uncertainty serves to inform ongoing discussions of how small sodium reactors would be licensed and may serve to reduce regulatory risk and cost for such reactors.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗