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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

A Brief Overview of Radiochemistry: Californium-252: Unique and Versatile Man-made Radioisotope

This chapter summarizes radiochemistry and its applications with a focus on areas where computational science can be beneficial. This is presented for a target audience of computational scientists and chemists, and the general public who are interested in radiochemistry topics that may benefit from the use of computational methods. Past, present, and future applications of radiochemistry are presented along with a brief examination of the field’s workforce. Discussions of the current state of several radiochemistry specialty areas are also included. These discussions generally exemplify topics that are readily amenable to computational tools. Topics discussed include medical uses for radioactive materials and related computational needs; the current and future trends in the separations of the f-block elements; production and uses of Californium-252; and the need for exascale computing to solve current problems in the chemistry of Americium and Plutonium.

Ezold, Julie↗
DOE OSTI2023

An Overview of the Radioisotope Electromagnetic Isotope Separation Capabilities at Idaho National Laboratory

Electromagnetic isotope separation (EMIS) has been an effective tool for the enrichment of isotopes for over 80 years. In the early 1990’s the U.S. reduced or eliminated electromagnetic isotope separation capabilities, but in the last decade, increased demand for both stable and radioactive enriched isotopes have led to the reestablishment of small-medium scale EMIS capabilities in the U.S. National Laboratory Complex.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

The Evolution of of Radioisotope Thermal Generators

Introduction The advancement of space exploration started in 1957 with the launch of Sputnik 1 which was quickly followed by the launch of Explorer 1 in 1958. The advancement in space exploration had much to do about the development of nuclear power in space. Enabling satellites to draw more power than before and carry out long term mission. The Radio Isotopic thermal generator (RTG) was first invented in 1954 and earned its place in the inventor’s hall of fame in 2015. The RTG has been the key to our success in the exploration of deep space. With in this paper the evolution of the RTG will be covered including the missions they facilitated. In addition, the ever present political and public view of nuclear material will play a role in the history of the RTG and the modern possibilities for nuclear power in space.

Belian, Olivia↗
DOE OSTI2023

CRADA Number NFE-19-07859 with Purist, Inc. (CRADA Final Report)

Cooperative Research and Development Agreement (CRADA) NFE-19-07859 between Oak Ridge National Laboratory (ORNL) and Purist Inc. (Purist) focused on developing a technology for production of high purity radioisotopes using small-scale underutilized research nuclear reactors. Purist is developing a novel production mechanism that will produce, and efficiently isolate radioisotopes with high specific activity at small-scale research reactors. The goal of this technology is to enable underutilized smaller scale reactors, typically not capable of producing medical grade radioisotopes, to be utilized as a production supply source. Such radioisotope production facilities will complement production efforts of the few larger production facilities to reduce and prevent risk in the medical isotope supply chain. The work done under this CRADA explored target development, to maximize isotope production and separation using Purist’s technology to ultimately obtain a radioisotope product with high specific activity for use in medical applications. Furthermore, under this CRADA post production, capture, concentration and encapsulation of the radioisotope product was studied by developing post irradiation midi to microscale processes to capture, store and release the separated radioisotopes from large volumes of the capture matrix after production, via automated High-Pressure Ion Chromatography (HPIC) and microfluidic purification/separation systems. This will enable concentration of the radioisotope product obtained into small volumes, which will aid in packaging and transporting the final radioisotope product to users.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Chemical separation and measurement of platinum activation products

Here, a method has been developed to purify and measure platinum radioisotopes in the presence of fission products and environmental constituents. The method uses a combination of cation exchange and anion exchange chromatography and selective precipitation steps to remove other radioisotopes from the sample. The addition of stable platinum carrier allows for a gravimetric determination of the chemical yield of the procedure. Overall, the method is fast, simple, and potentially applicable for rapid turnaround of unknown samples. Using this method, multiple platinum radioisotopes were measured in two different irradiation experiments. The measured ratios of the platinum radioisotopes clearly reflect the neutron spectrum of the irradiation, suggesting that platinum radioisotopes could be valuable signatures in nuclear forensic analyses.

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

Heavy-ion production of 77 Br and 76 Br

Many radioisotopes with potential medical applications are difficult to produce routinely, especially those on the proton-rich side of the valley of stability. Current production methods typically use light-ion (protons or deuteron) reactions on materials of similar mass to the target radioisotope, which limits the elemental target material available and may require the use of targets with poor thermal properties (as is the case for the production of radiobromine). These reactions may also create significant amounts of proton-rich decay products which require chemical separation from the desired product in a highly radioactive environment. A promising alternative method using heavy-ion fusion-evaporation reactions for the production of the medically relevant bromine radioisotopes 76 Br (t 1/2 = 16.2 h) and 77 Br (t 1/2 = 57.0 h) is presented. Heavy-ion beams of 28 Si and 16 O were used to bombard natural chromium and copper targets just above the Coulomb barrier at the University of Notre Dame's Nuclear Science Laboratory to produce these bromine and precursor radioisotopes by fusion-evaporation reactions. Production yields for these reactions were measured and compared to PACE4 calculations. In addition to using more robust targets for irradiation, a simple physical–chemical separation method is proposed that will lead to very high radiopurity yields. A summary of accelerator facility requirements needed for routine production of these radioisotopes is also presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

National User Resource for Biological Accelerator Mass Spectrometry

The National User Resource for Biological Accelerator Mass Spectrometry (User Resource) will provide isotopic analysis (primarily radiocarbon or 14C) by accelerator mass spectrometry (AMS) for NIH- funded researchers across the United States and will be the only User Resource of its type in the United States. The User Resource will provide measurement capability and expertise to a research community that requires highly sensitive, quantitative isotope analyses. Since commissioning a new accelerator mass spectrometer in June 2014, we have measured over 4000 samples a year for collaborators and service users. The User Resource will enable us to continue to meet these research needs, as well as provide for new users whose research programs would benefit from AMS as a measurement tool. The User Resource’s forte will be ultra-high sensitivity quantitation of radiocarbon and selected other radioisotopes for research studies where isotopes are required. Radioisotope labeling studies have been and will continue to be an important tool for addressing many complex biomedical science problems. AMS is a specialized and unique type of mass spectrometry that provides absolute quantitation of radiocarbon and other relevant radioisotopes with extreme sensitivity, having limits of detection in real samples on the order of a few attomol/mg of sample at measurement precisions of ~3%. It is the only instrumental method capable of quantifying radioisotope-labeled agents routinely in real-world samples with such precision and sensitivity. The sensitivity of AMS allows for the quantification of radiolabeled metabolites in extremely complex matrices of cells and organisms at very low concentrations and in small samples. AMS allows studies to be conducted without perturbing metabolism leading to more relevant quantification of metabolic rates and pathways. In addition, it enables quantification of pharmacokinetic and metabolic properties of toxicants at environmentally relevant concentrations in model systems as well as the ability to quantify pharmacokinetics and other molecular endpoints directly in humans. Such quantitative assessments can 1) improve risk assessment for toxicants, 2) address safety and efficacy considerations for therapeutic entities, 3) deepen understanding of xenobiotic and intermediary metabolism, 4) help understand the interactions between critical molecular pathways, and 5) improve efforts to model and predict various metabolic and biological states. These capabilities have been applied in a number of areas including research in carcinogenesis, toxicology, nutrition, pharmacology/drug development and basic biological science. As a NIGMS National Resource the National User Resource for Biological Accelerator Mass Spectrometry will help NIH funded scientists achieve a deeper understanding of the etiology of human health concerns by (1) enabling the quantification of pharmacokinetics and other molecular endpoints directly in humans; (2) offering the ability to conduct quantitative studies using biologics such as proteins or lipids, and thereby reducing the amount of radioisotope usage in biomedical labs; and (3) enabling more relevant studies of metabolic pathways in health and disease through the use of much lower, more biologically-relevant, concentrations of metabolic substrates in cells and intact organisms. Such studies support NIGMS’s basic biomedical research areas that contribute to the understanding of fundamental cellular and physiological principles and enable research supported by the Biophysics, Biomedical Technology, and Computational Biosciences (BBCB); Genetics and Molecular, Cellular, and Developmental Biology (GMCDB); Pharmacology, Physiology, Biological Chemistry (PPBC) and Training, Workforce Development, and Diversity (TWD) Divisions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

National User Resource for Biological Accelerator Mass Spectrometry (Final Report)

The National User Resource for Biological Accelerator Mass Spectrometry (User Resource) will provide isotopic analysis (primarily radiocarbon or 14C) by accelerator mass spectrometry (AMS) for NIH- funded researchers across the United States and will be the only User Resource of its type in the United States. The User Resource will provide measurement capability and expertise to a research community that requires highly sensitive, quantitative isotope analyses. Since commissioning a new accelerator mass spectrometer in June 2014, we have measured over 4000 samples a year for collaborators and service users. The User Resource will enable us to continue to meet these research needs, as well as provide for new users whose research programs would benefit from AMS as a measurement tool. The User Resource’s forte will be ultra-high sensitivity quantitation of radiocarbon and selected other radioisotopes for research studies where isotopes are required. Radioisotope labeling studies have been and will continue to be an important tool for addressing many complex biomedical science problems. AMS is a specialized and unique type of mass spectrometry that provides absolute quantitation of radiocarbon and other relevant radioisotopes with extreme sensitivity, having limits of detection in real samples on the order of a few attomol/mg of sample at measurement precisions of ~3%. It is the only instrumental method capable of quantifying radioisotope-labeled agents routinely in real-world samples with such precision and sensitivity. The sensitivity of AMS allows for the quantification of radiolabeled metabolites in extremely complex matrices of cells and organisms at very low concentrations and in small samples. AMS allows studies to be conducted without perturbing metabolism leading to more relevant quantification of metabolic rates and pathways. In addition, it enables quantification of pharmacokinetic and metabolic properties of toxicants at environmentally relevant concentrations in model systems as well as the ability to quantify pharmacokinetics and other molecular endpoints directly in humans. Such quantitative assessments can 1) improve risk assessment for toxicants, 2) address safety and efficacy considerations for therapeutic entities, 3) deepen understanding of xenobiotic and intermediary metabolism, 4) help understand the interactions between critical molecular pathways, and 5) improve efforts to model and predict various metabolic and biological states. These capabilities have been applied in a number of areas including research in carcinogenesis, toxicology, nutrition, pharmacology/drug development and basic biological science. As a NIGMS National Resource the National User Resource for Biological Accelerator Mass Spectrometry will help NIH funded scientists achieve a deeper understanding of the etiology of human health concerns by (1) enabling the quantification of pharmacokinetics and other molecular endpoints directly in humans; (2) offering the ability to conduct quantitative studies using biologics such as proteins or lipids, and thereby reducing the amount of radioisotope usage in biomedical labs; and (3) enabling more relevant studies of metabolic pathways in health and disease through the use of much lower, more biologically-relevant, concentrations of metabolic substrates in cells and intact organisms. Such studies support NIGMS’s basic biomedical research areas that contribute to the understanding of fundamental cellular and physiological principles and enable research supported by the Biophysics, Biomedical Technology, and Computational Biosciences (BBCB); Genetics and Molecular, Cellular, and Developmental Biology (GMCDB); Pharmacology, Physiology, Biological Chemistry (PPBC) and Training, Workforce Development, and Diversity (TWD) Divisions. Over the next five years, our goals are to: 1. Improve the efficiency of operation for AMS measurements through installation of new interfaces to our AMS systems, technical modifications to improve gas accepting ion source efficiency and upgrading our data analysis software for improved ease of use and data reporting. 2. Increase the accessibility and visibility of ultra-sensitive 14C measurements for the biomedical research community by training of new investigators and expanding our national user base. 3. Provide high throughput, ultra-sensitive 14C analysis for the NIGMS and NIH user community.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Production Pathways for Medically Interesting Isotopes

Radioisotopes are commonly used in nuclear medicine for treating cancer and new, more effective treatment options are always desired. As a result, there is a national need for new radioisotopes and ways to produce them. A computer program was created that evaluates the daughters for all known reactions of projectiles (gamma rays, protons or neutrons) with every stable target isotope by comparing the cross-sections for each reaction at a desired energy, and outputs a list of the potential daughter isotopes that are most likely to be generated. The program then evaluates the decay chains of these daughters to provide a list of the possible decay chains that contain the radioisotope of interest. By knowing the daughter production and decay chain for each isotope, it is possible to go from the desired radioisotope to the stable isotope that can be used as a target for its production. This project would facilitate the search for new pathways to creating useful theranostic isotopes.

Hutton, A.↗
DOE OSTI2023

National User Resource for Biological Accelerator Mass Spectrometry Annual Report

The National User Resource for Biological Accelerator Mass Spectrometry (User Resource) will provide isotopic analysis (primarily radiocarbon or 14C) by accelerator mass spectrometry (AMS) for NIH- funded researchers across the United States and will be the only User Resource of its type in the United States. The User Resource will provide measurement capability and expertise to a research community that requires highly sensitive, quantitative isotope analyses. Since commissioning a new accelerator mass spectrometer in June 2014, we have measured over 4000 samples a year for collaborators and service users. The User Resource will enable us to continue to meet these research needs, as well as provide for new users whose research programs would benefit from AMS as a measurement tool. The User Resource’s forte will be ultra-high sensitivity quantitation of radiocarbon and selected other radioisotopes for research studies where isotopes are required. Radioisotope labeling studies have been and will continue to be an important tool for addressing many complex biomedical science problems. AMS is a specialized and unique type of mass spectrometry that provides absolute quantitation of radiocarbon and other relevant radioisotopes with extreme sensitivity, having limits of detection in real samples on the order of a few attomol/mg of sample at measurement precisions of ~3%. It is the only instrumental method capable of quantifying radioisotope-labeled agents routinely in real-world samples with such precision and sensitivity. The sensitivity of AMS allows for the quantification of radiolabeled metabolites in extremely complex matrices of cells and organisms at very low concentrations and in small samples. AMS allows studies to be conducted without perturbing metabolism leading to more relevant quantification of metabolic rates and pathways. In addition, it enables quantification of pharmacokinetic and metabolic properties of toxicants at environmentally relevant concentrations in model systems as well as the ability to quantify pharmacokinetics and other molecular endpoints directly in humans. Such quantitative assessments can 1) improve risk assessment for toxicants, 2) address safety and efficacy considerations for therapeutic entities, 3) deepen understanding of xenobiotic and intermediary metabolism, 4) help understand the interactions between critical molecular pathways, and 5) improve efforts to model and predict various metabolic and biological states. These capabilities have been applied in a number of areas including research in carcinogenesis, toxicology, nutrition, pharmacology/drug development and basic biological science.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2026

Refining a Novel Process Monitoring Method to Safeguard Continuously Cycling Designs Using Isotopic Ratios

In advanced reactor (AR) designs, a common feature is continuous chemical processing and circulation of the nuclear material. This work bridges a significant measurement gap in safeguarding reactors with circulating fuel or continuous refueling by leveraging and building on the isotope ratio method first developed by our team under an FY21 Advanced Reactors International Safeguards Engagement (ARISE) project (Uribe et al. 2021). In circulating fuel designs, the radioisotope inventory changes from traditional effects (e.g., radioactive decay, fission) but also includes material transport due to pressure and temperature gradients. Such designs may also require regular or continuous additions or removals during operation, which significantly increases the rate of inventory change compared to traditional pressurized water reactor (PWR)s. Thus, directly tracking the nuclear inventory is ineffective since the isotopes are continuously added and removed. The isotope ratio method instead focuses on detecting changes to the input and output flows of radioisotopes. Previous work showed that for well-chosen pairs of isotopes, the isotopic ratio provides a sensitive and lasting indicator of deviation from normal conditions (e.g., startup, shutdown, diversion). The isotope ratio method is a process monitoring method with potential for application in for forward-looking approaches to International Atomic Energy Agency (IAEA) safeguards. The original process monitoring method was developed for a specific case—the decay tank of a thorium-fueled molten salt breeder reactor. In this expanded work, we explored other types of reactors and processes with nonstationary (e.g., flowing) nuclear material, which are difficult to safeguard with traditional methods because of the transient nature of the systems. The goal of the present work is to generalize the isotope ratio method for use in processes with continuously flowing nuclear material. All continuous processes have an average time for isotopes to be replaced in the system. The isotope ratio method works by choosing radioisotopes with half-lives both above and below the processing time. The present work seeks to explore which isotopes are suitable for the method by simulating the nuclear inventory, radioisotope emissions, and detector responses for several classes of advanced reactors. While the method can in principle be applied to other processes (e.g., enrichment or reprocessing facilities), the present work limits scope to ARs with continuously flowing fuel. Section 2 details the mathematics supporting the isotope ratio method, and Section 3 introduces the representative ARs selected for this work. Section 4 discusses how each reactor was analyzed, and Section 5 showcases the results for each representative reactor. Finally, Section 6 provides concluding remarks and suggests pathways for further analysis.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2025

An Evaluation and Qualification of U.S.-Based Research Reactors for Irradiation Capabilities Supporting Advanced Nuclear Systems

Irradiation experiments are a prerequisite for evaluating nuclear reactor system designs, analyzing the performance of these systems, and obtaining licenses. Likewise, irradiation facilities are necessary for producing the radioisotopes used in industrial and medical applications. Recent developments in modeling and simulation capabilities and advancements in computational resources have further enabled the design of irradiation experiments for evaluating radiation-induced phenomena and determining nuclear fuel, material, and system design and safety criteria pertaining to both normal and accident scenarios. These computational tools and models require comprehensive experimental datasets acquired under prototypic radiation conditions—for exploring material and system performance under the uniquely harsh environments found in nuclear reactors—to enable verification and validation for qualification and licensing purposes. However, qualification of irradiation experimental facilities, primarily research and test reactors (RTRs), necessitates that their performance be evaluated based on the irradiation environment (e.g. flux, power, testing capabilities) using an appropriate scoring matrix. Although many university campus RTRs are available for research and development (R&D) activities and initiatives, this study focuses on evaluating and qualifying the irradiation facilities (mostly RTRs) within the United States that are suitable for advanced nuclear fuel, material, and system irradiation experiments aimed at establishing operational-performance limits and informing component and fuel designs so as to improve operational efficiencies and mitigate proliferation vulnerabilities, as well as for radioisotope production aimed at multipurpose applications. As a result, the findings of the present study support the acceleration of nuclear fuel and material qualifications, thus hastening new and advanced nuclear energy system demonstrations and radioisotope production efforts by using extended R&D.

irradiation experiment↗
DOE OSTI2024

Multilabel proportion prediction and out-of-distribution detection on gamma spectra of short-lived fission products

In the machine learning problem of multilabel classification, the objective is to determine for each test instance which classes the instance belongs to. In this work, we consider an extension of multilabel classification, called multilabel proportion prediction, in the context of radioisotope identification (RIID) using gamma spectra data. We aim to not only predict radioisotope proportions, but also identify out-of-distribution (OOD) spectra. We achieve this goal by viewing gamma spectra as discrete probability distributions, and based on this perspective, we develop a custom semi-supervised loss function that combines a traditional supervised loss with an unsupervised reconstruction error function. Our approach was motivated by its application to the analysis of short-lived fission products from spent nuclear fuel. In particular, we demonstrate that a neural network model trained with our loss function can successfully predict the relative proportions of 37 radioisotopes simultaneously. The model trained with synthetic data was then applied to measurements taken by Pacific Northwest National Laboratory (PNNL) to conduct analysis typically done by subject-matter experts. Here, we also extend our approach to successfully identify when measurements are OOD, and thus should not be trusted, whether due to the presence of a novel source or novel proportions.

Anomaly detection↗