Search NASA⌕ Search

SEARCH · Search NASA

Results for “PLUTONIUM ISOTOPES”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 109 records · Page 6

History of Pu-238 Production Restart Efforts at Idaho National Laboratory and Oak Ridge National Laboratory

In the early 2010s, efforts to restart production in the U.S. of plutonium-238 heat source (HSPu) material for NASA deep space missions were initiated. Processes, procedures, hardware, and chemical separations were developed and implemented to enable the production of heat source material at Oak Ridge National Laboratory (ORNL) and Idaho National Laboratory (INL). Here, this review provides an overview of the timeline and efforts associated with the restart of production, as well as upcoming efforts to increase production.

07 ISOTOPE AND RADIATION SOURCES↗

A new TEVA-DGA chromatography procedure to separate Pu, Am, and Np from bulk U materials

Trace actinides present within uranium (U) material are diagnostic signatures of U processing history. For example, the emplacement of U material within the high neutron-flux environment of a nuclear reactor can cause neutron capture of U to form 241-plutonium ( 241 Pu). Plutonium-241 then decays to progeny isotopes 241-americium ( 241 Am) and 237-neptunium ( 237 Np); therefore, the presence and relative abundances of these trace actinides is indicative of the material’s production history and intended employment (Mayer et al., 2013). During a pre-detonation nuclear forensics investigation, measurement of trace actinide 241 Pu, 241 Am, and 237 Np concentrations by an analytical laboratory may be requested. However, chemically purifying these elements from bulk U is a challenging and involved procedure requiring several sequential chromatography columns across 4+ days. To expedite Pu-Am-Np separation from bulk U material, and to improve the yield recovery of these elements, this DHS Postdoc Fellowship has worked to create a new chromatography separation chemistry.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Isotopic Analysis using FRAM [Slides]

FRAM is an isotopic analysis code nominally designed for plutonium and uranium. It stands for Fixed-energy Response-function Analysis with Multiple efficiencies. It has self-calibration using several gamma-ray peaks and can analyze gamma ray data from 30keV to >1MeV of HPGe, CdTe, or LaBr3 detector. The key difference between the MGA family of codes (from LLNL) and FRAM is the use of user-editable analysis parameters in the latter.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Economical Production of Pu-238: NIAC Phase I Final Report

All space exploration missions traveling beyond Jupiter must use radioisotopic power sources for electrical power. The best isotope to power these sources is plutonium-238 (Pu-238). The US supply of Pu-238 is almost exhausted and will be gone within the next decade. The Department of Energy has initiated a production program with a $10M allocation from NASA but the cost is estimated at over $100M to get to production levels. The Center for Space Nuclear Research (CSNR) has conceived of a potentially better process to produce Pu-238 earlier and for significantly less cost. Potentially, the front end capital costs could be provided by private industry such that the government only had to pay for the product produced. In the Phase I NIAC (NASA Innovative Advanced Concepts) grant, the CSNR has evaluated the feasibility of using a low power, commercially available nuclear reactor to produce 1.5 kg of Pu-238 per year. The impact on the neutronics of the reactor have been assessed, the amount of Neptunium target material estimated, and the production rates calculated. In addition, the size of the post-irradiation processing facility has been established. Finally, as the study progressed, a new method for fabricating the Pu-238 product into the form used for power sources has been identified to reduce the cost of the final product. In short, the concept appears to be viable, can produce the amount of Pu-238 needed to support the NASA missions, can be available within a few years, and will cost significantly less than the current DOE program.

Plutonium↗

Risk Analysis of Radiological Release from Pu-238 Targets During Manual Handling

Pu-238 Isotope Production Targets are routinely installed in the Advanced Test Reactor (ATR) core, transferred, and stored in the spent fuel canal. These evolutions involve manual handling and manipulation of the targets underwater using long handled tools. The ATR Safety Analysis Report (SAR) postulates a design basis accident which results in damage from manual manipulation of targets, and radiological consequences must be determined for receptors inside the reactor facility, as well as public receptors. This presentation presents the analysis used to determine the radiological consequences due to potential target damage in the ATR canal. The analysis considered radionuclide release fractions, damage ratios for handling evolutions, and entrainment of radionuclides in the canal water.

Advanced Test Reactor↗

Protecting People and Planet

To produce energy, civilian nuclear power plants require fuel. The majority of existing plants rely on solid ceramic fuels that contain concentrations of about 3 to 5% of the element uranium-235. This specific isotope is well suited to sustaining the type of chain reaction required for a nuclear reactor to harness the heat produced by nuclear fission. Title I of the United States Atomic Energy Act of 1954 defines “special nuclear material” as plutonium, uranium-233, or uranium enriched in the isotopes uranium-233 or uranium-235. This label identifies materials that at high concentrations can be used to produce nuclear weapons. The United States and broader international community are fully committed to ensuring the peaceful use of nuclear energy by committing to practices known as safeguards.

99 GENERAL AND MISCELLANEOUS↗

Lunar Surface Stirling Power Systems Using Isotope Heat Sources

For many years, NASA has used the decay of plutonium-238 (Pu-238) (in the form of the General Purpose Heat Source (GPHS)) as a heat source for Radioisotope Thermoelectric Generators (RTGs), which have provided electrical power for many NASA missions. While RTGs have an impressive reliability record for the missions in which they have been used, their relatively low thermal to electric conversion efficiency and the scarcity of plutonium-238 (Pu-238) has led NASA to consider other power conversion technologies. NASA is considering returning both robotic and human missions to the lunar surface and, because of the long lunar nights (14.75 Earth days), isotope power systems are an attractive candidate to generate electrical power. NASA is currently developing the Advanced Stirling Radioisotope Generator (ASRG) as a candidate higher efficiency power system that produces greater than 160 W with two GPHS modules at the beginning of life (BOL) (~32% efficiency). The ASRG uses the same Pu-238 GPHS modules, which are used in RTG, but by coupling them to a Stirling convertor provides a four-fold reduction in the number of GPHS modules. This study considers the use of americium-241 (Am-241) as a substitute for the Pu-238 in Stirling- convertor-based Radioisotope Power Systems (RPS) for power levels from tens of watts to 5 kWe. The Am-241 is used as a substitute for the Pu-238 in GPHS modules. Depending on power level, different Stirling heat input and removal systems are modeled. It was found that substituting Am-241 GPHS modules into the ASRG reduces power output by about one-fifth while maintaining approximately the same system mass. In order to obtain the nominal 160 W of electrical output of the Pu-238 ASRG requires 10 Am-241 GPHS modules. Higher power systems require changing from conductive coupling heat input and removal from the Stirling convertor to either pumped loops or heat pipes. Liquid metal pumped loops are considered as the primary heat transportation on the hot end and water pumped loop/heat pipe radiator is considered for the heat rejection side for power levels above 1 kWe.

Schmitz, Paul C.↗

Neptunium mononitride as a target material for Pu-238 production

Deep space exploration requires specialized sources for both thermal and power applications. Radioactive decay heat of plutonium-238 (238Pu) provides these sources in the form of radioisotope thermoelectric generators (RTGs). The 238 Pu is produced via neutron capture reaction involving neptunium-237 ( 237 Np) target material. Continual optimization of 237 Np target materials and evaluation of potential alternative targets for production of 238 Pu RTGs are advantageous for meeting ongoing space power system resource requirements. Current production of 238 Pu for RTGs for the United States space program utilizes neptunium dioxide ( 237 NpO 2 ) targets; however, the use of neptunium mononitride ( 237 NpN) presents an opportunity to increase the mass of 237 Np per target compared to the dioxide form, as well as increase the thermal conductivity of the target. To assess the viability of a 237 NpN target material, the material chemistry must be thoroughly evaluated, including synthesis methods and dissolution and reprocessing schemes. This review presents a summary of synthesis pathways for 237 NpN based on published literature on actinide mononitrides. Specific literature on 237 NpN is limited, necessitating evaluation of other actinide systems to gather parallels. This suggests a need for additional experimental studies on 237 NpN. A particular limitation in the existing literature is a lack of information on the differences in material characteristics, such as morphology, particle size, and trace chemical impurities, as a function of synthesis method. These parameters may affect subsequent reactor performance or dissolution of irradiated targets. The evaluation of existing literature is presented with a focus on the efficacy of 237 NpN targets for 238 Pu production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Combination of DGA and LN Columns: A Versatile Option for Isotope Production and Purification at Oak Ridge National Laboratory

The chromatographic resins DGA and LN have been used sequentially to separate curium, californium, plutonium, and various fission products (FPs) to obtain products with a pure radioisotope or a radioelement with high isotopic purity. This 2-step combination of resins has found applications in the 252 Cf and 238 Pu campaigns performed at Oak Ridge National Laboratory. Experiments have been carried out in glove boxes, shielded caves, and hot cells, demonstrating that these resins are adequate and maintain their performance in highly radiolytic environments. We find that using these resins has led to the recovery of curium highly enriched (>95%) in 248 Cm, the clean separation of 251 Cf for the superheavy element research, and the recovery of 147 Pm from the FP stream obtained during the 238 Pu production campaign while demonstrating that the raffinate post DGA is essentially free of transuranic elements.

07 ISOTOPE AND RADIATION SOURCES↗

Evaluating FRAM v.6.1 with LANL and Euratom data

The United States Department of Energy and the European Atomic Energy Community (EURATOM) collaborate to test, evaluate, and improve the performance of the FRAM 6.1 code with various nuclear materials, especially mixed oxide (MOX) containing an isotopic blend of uranium and very high burnup plutonium. This joint effort is intended to promote effective implementation of the FRAM 6.1 code into nuclear material verification methods.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Diversion Path Analysis: A Proposed Methodology to Develop an MC&A Approach for Liquid-Fueled Molten Salt Reactors

Nuclear material control and accounting (MC&A) is a critical element of both the US Nuclear Regulatory Commission (NRC) and US Department of Energy (DOE)’s domestic safeguards and security requirements. NRC licensees are required, under Title 10 of the Code of Federal Regulations (10 CFR) Part 74 to establish and maintain an MC&A program that captures and records the quantities and locations of special nuclear material (SNM) at the facility. Along with physical protection, MC&A is a key element of domestic nuclear material safeguards that enables the NRC to ensure that SNM is controlled and accounted for. SNM, per 10 CFR Part 74, refers to plutonium, 233 U, and uranium enriched in the isotope 233 U or 235 U, but does not include source material. Periodic physical inventories, coupled with material balance evaluations, are effective and demonstrated tools to account for and detect theft or diversion of SNM in facilities containing SNM in bulk material form (i.e., not in discrete, countable items). Historically in the United States, these types of facilities have included fuel fabrication, conversion, and enrichment facilities. In comparison, reactors have relied on item counting of assemblies and control of SNM while in containment (e.g., a sealed reactor pressure vessel) because, to date, reactor fuel has been in item form. In liquid-fueled molten salt reactors (MSRs), unlike traditional light water reactors (LWRs) or bulk facilities, bulk SNM quantities can change significantly during operation as a result of depletion and transmutation. This introduces challenges to the use of traditional periodic physical inventories and material balance evaluations to detect theft or diversion of SNM in reactors that use SNM in bulk material form. Liquid-fueled (i.e., salt-fueled) MSR facilities are MSRs that use SNM within a salt eutectic as the fuel. The SNM is in a bulk material form any time it is outside of fresh or spent fuel storage containers. Some examples of when SNM will be in bulk form in the facility are during addition of fuel to the reactor system, while fuel is circulating in operation, and while fuel is in a drain tank. Periodic physical inventories and material balance evaluations can likely be effectively applied to many portions of an MSR facility, including all areas where depletion and transmutation are not significantly changing the quantities of SNM within the control area. Within an MSR facility, this would include fresh fuel receipt and loading, waste streams that may contain SNM, irradiated fuel storage outside of the reactor core, and any irradiated fuel processing that may happen after SNM has been removed from the reactor. All of these process steps could rely on measurements of SNM quantities compared with documented inventories. Any discrepancies from predicted (i.e., book) inventories and measured inventories could be quantified as inventory differences, consistent with traditional MC&A guidance from the NRC (e.g., in NUREG-1065 Revision 2, NUREG-2159 Revision 1, and RG 5.29 Revision 2). Within the reactor system, additions and removals to the book inventory include depletion of the SNM (e.g., fission of 235 U), which complicates the use of physical inventories. SNM control, however, can also likely be effectively applied to detect theft of SNM throughout a liquid-fueled MSR facility. To complement these approaches, prior technical reports have identified that a diversion path analysis may be a useful, risk-informed, and performance-based tool to determine suitable elements of an MC&A approach for the reactor system within a liquid-fueled MSR facility.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Isotope Production for UK PhD Student Visit [Slides]

Overview of INL isotope production work, including organizational structures, the current work and future plans of plutonium fuel supplies, cobalt-60 production, and BRR cask shipping.

07 ISOTOPE AND RADIATION SOURCES↗

Analysis of an irradiated uranium sample for source attribution without chemical separation using microplasma ionization and ultrahigh resolution mass spectrometry

The use of element isotope ratios has great potential in not only determining the reactor type used to produce plutonium (Pu) but also in determining the burnup and the time since irradiation. While a powerful nuclear forensic technique, determining element isotope ratios is complicated by severe isobaric interferences when performed on typical inductively coupled plasma mass spectrometers. Such analyses require extensive chemical separations prior to analysis to alleviate the inter-elemental isobars. Ultrahigh mass resolution spectrometry provides a potential alternative, greatly reducing the complexity of sample preparation and turnaround times for these critical measurements. To demonstrate the power of the approach, a sample of irradiated, depleted uranium was analyzed with the liquid sampling—atmospheric pressure glow discharge ion source coupled to an Orbitrap mass spectrometer. The Orbitrap is augmented with an external data acquisition system, Spectroswiss’s FTMS-Booster X2T, allowing collection of extended ion transients, providing higher mass resolution. In using this approach, the 150 Sm/ 149 Sm and 152 Sm/ 149 Sm isotope ratios were found to be within 20% of predicted values without any chemical separations and without mass bias corrections. In addition, the 240 Pu/ 239 Pu isotope ratio was determined, free from the 238 UH + interferences common to the ICP-MS platforms, while at the same time allowing for the determination of U isotopic signatures. While these demonstrative results are from a single sample, the advantages of the microplasma/ultrahigh mass resolution approach to intra-element isotope ratio determinations are clear.

Fuel burnup↗

Two-watt radioisotope power generators for underwater applications

Materials and design considerations are discussed for a low-cost, reliable radio-isotope-fueled thermoelectric generator for use in an undersea application. Plutonium has been selected as fuel, and the generator has to meet design goals of 2 watts after 20 years with a direct output voltage of 6-8 volts. The pressed and sintered form of Bi2Te3 appears to be the most appropriate thermoelectric material. Both fibrous and multilayer foil insulation could be used with proper processing and quality control, but there is less risk with fibrous type insulation. Min-K 1400 is recommended with a nitrogen cover gas. The heat source recommended is a three-layer capsule using T-111 for both the liner and strength member with an outer liner of Hastelloy-C.

Caputo, R. S.↗

Actinide Mixing Optimization Solver

The Actinide Mixing Optimization Solver (AMOS) is a set of programs written in MATLAB that computes theoretical mixes of different uranium, plutonium, thorium, and other actinide materials given a list of isotopic reference materials. Constraints are applied depending on the desired product and a mixture is computed to meet the specified requirements. The optimal mixture consists of a product that uses the lowest possible number of initial actinide materials and has the lowest cost. AMOS is currently applied to particular reference material requests from the sponsoring agency (NNSA) on behalf of the IAEA.

Baldwin, Aaron Taylor↗

A multi-collector ICP-MS method for quantification of plutonium, uranium, and americium in hair and nails of occupationally or medically exposed individuals

The 239 Pu, 238 U, and 241 Am concentrations and 239 Pu/ 240 Pu, 235 U/ 238 U, and 236 U/ 238 U atom ratios were measured in the hair and nail samples from individuals who donated their bodies to the United States Transuranium and Uranium Registries. Further, the concentration of 239 Pu ranged from 0.22–15.8 ng/kg. The 240 Pu/ 239 Pu isotopic ratios ranged from 0.026 to 0.127 which is consistent with weapons-grade plutonium. Concentration of uranium fell between 1.84 µg/kg and 29.5 µg/kg and 235 U/ 238 U ratios ranged from 4.8×10 -3 to 7.6×10 -3 . Elevated 236 U/ 238 U atom ratios were measured in two cases and ranged from 5.0×10 -6 – 2.4×10 -5 indicating exposure to spent or reprocessed uranium material. The concentration of 241 Am was measured in four hair samples and ranged from 0.02–0.21 ng/kg.

61 RADIATION PROTECTION AND DOSIMETRY↗

Measuring Neptunium Concentration using Optical Spectrometry for the Pu-238 Supply Program

Targets containing 237 Np are irradiated at the High Flux Isotope Reactor at Oak Ridge National Laboratory to produce 238 Pu, as plutonium dioxide (PuO 2 ), a heat source material for use in future NASA space missions. Kilogram quantities of Np are processed yearly and developing methods to efficiently characterize and monitor the Np processing streams with optical spectroscopy and real-time monitoring software is a critical aspect of this effort. Here, we evaluate how ultraviolet/visible/near-infrared (UV-Vis-NIR) absorbance and Raman spectroscopic techniques are applicable to characterizing concentrated Np solutions and provide proof-of-principle and proof-of-concept results for each technique. Both techniques were tested in lab-scale studies and should improve the timeliness of production efforts. However, spectrophotometry is the more mature option and has been successfully demonstrated in a hot cell environment. An overview of the initial findings, a brief demonstration, and areas for future work will be highlighted in this report.

07 ISOTOPE AND RADIATION SOURCES↗

140,142 Cerium Resolved Resonance Region Evaluation [Slides]

The presentation covers an overview of 140,142 Ce Isotopes, including new evaluations of 140,142 Ce that were requested by the Hanford Plutonium Finishing plant to the Nuclear Criticality Safety Program. It also discusses current ENDF/B-VIII.0 evaluation, which has an error in the 1-2 keV range. It was evaluated using multi-level Breit-Wigner and 142Ce has room for extending resolved resonance region current upper limit from 13 keV. The presentation also discusses new transmission and capture measurements of nat Ce and 142 Ce from Klaus Guber. It also states that no known integral experiments prominently feature Cerium.

07 ISOTOPE AND RADIATION SOURCES↗