Chemical Processing Waste Remediation in the Plutonium-238 Supply Program
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Apollo postflight analysis of polonium 210 and plutonium 238 radiation shielding for power supplies
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Neptunium dioxide (NpO 2 ) is a key phase in nuclear material processing as a target material for the production of plutonium-238 ( 238 Pu) and has been historically synthesized via the calcination of a Np oxalate precursor. Alternative synthesis methods for NpO 2 are now more prevalent, necessitating their study and comparison with the more common oxalate route. The purpose of this work was to investigate the microstructural properties of NpO 2 synthesized from a nitrate-based Np precursor phase via the assessment of NpO 2 particle size and morphology as a function of calcination temperature and time. Scanning electron microscopy (SEM) was used to probe the primary grain size and morphology of NpO 2 after calcination at temperatures ranging from 700 to 1100 °C and hold times ranging from 1 to 10 h. Post-image analysis using ImageJ software enabled the quantification of mean particle diameter. This analysis indicated that particle diameter increases with both increasing calcination temperature and hold time. Primary particles were shown to be clumped in irregular patterns into the overall rough, blocky aggregates, but this macroscopic morphology was not affected by calcination time or temperature. Although trends in primary grain size of NpO 2 were consistent with available literature from other Np precursor phases, the macroscopic morphology of the NpO 2 aggregates was quite different than reported for other precursors. Through comparison with historical literature on Np oxalate, this work emphasizes the importance of Np precursor on the physical properties of NpO 2 .
Neptunium (Np) possesses a rich and unique chemistry that often diverges from other actinide elements yet remains relatively underexplored compared with the other light actinides. A resurgence of interest in Np has been spurred by the application of 237 Np for plutonium-238 ( 238 Pu) production for use in radioisotope thermoelectric generators (RTGs), necessitating evaluation of Np chemical reactions and materials. The work presented here studied the thermal decomposition of neptunyl ammonium nitrate (NH 4 Np VI O 2 (NO 3 ) 3 ) for synthesis of neptunium dioxide (NpO 2 ), which is the target material used for production of 238 Pu. Additionally, structural characterization of the intermediate solid Np pentoxide (Np 2 O 5 ) was performed. Advanced solid-state characterization techniques, including simultaneous thermal analysis (STA), powder X-ray diffraction (pXRD), Raman spectroscopy, and density functional theory (DFT) modeling have been combined to study the reaction pathways. Analysis revealed that NH 4 Np VI O 2 (NO 3 ) 3 thermally decomposes to a proposed neptunyl nitrate intermediate, followed by Np 2 O 5 and finally NpO 2 , all within the temperature range of 150 °C–600 °C. Further characterization of the pentoxide intermediate provided the first Raman spectra of pure-phase Np 2 O 5 and associated DFT modeling confirmed Raman peak assignments for this phase. These findings provide mechanistic information to advance production of the critical radioisotope 238 Pu and advance the state of knowledge on Np materials chemistry using modern characterization techniques.
The production of plutonium-238 through irradiation of neptunium-237 ( 237 Np) target materials for the use in radioisotope thermoelectric generators is paramount for continued deep space exploration. This work employs scanning electron microscopy to analyze 237 Np materials coupled with a well-developed image analysis framework (Morphological Analysis for Material Attribution, or MAMA) to determine the degree of micron-scale homogeneity in the materials. This work demonstrated how the quantification of particle characteristics can validate production materials and affirm the qualitative similarities observed in micrographs. The 237 Np oxide particle analysis determined that the materials from five production runs were quantitatively homogenous (significant at α = 0.05) in particle area, circularity, equivalent circular diameter, and ellipse aspect ratio, with two of the sampling dates having statistically significant different means for one of the four characteristics. Furthermore, these metrics not only confirm general homogeneity of the material but also expand the application of MAMA workflows to 237 Np materials, demonstrating the utility of MAMA analysis for a wider breadth of nuclear materials than previously reported. In the open literature, this study is the first time that these microanalytical techniques were applied to 237 Np materials to this degree.
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.
Plutonium-238 radioisotope Brayton cycle power system design and vehicle integration
The present difficulties experienced by the United States in launching payloads into space has suggested a number of problems which are associated with the handling of hazardous materials in spacecraft. The question has arisen as to the safety of launching highly radioactive material such as plutonium-238, related to the possibility of its dispersion into the atmosphere during a launch vehicle explosion. An alternative is the use of a small nuclear reactor which is not started until it is in space and contains little or no radioactivity at launch. A first order assessment of six small reactor concepts with power levels up to 100 MWe was performed. Both the nuclear feasibility of these concepts to operate at their rated power levels between 7 and 10 years and the capability of these concepts to remain subcritical both before and during launch and also in the case of water immersion during a potential launch failure or abort were investigated.
The radio-isotope thermoelectric generator (RTG) for Ulysses' electronic supply is described noting that lack of sufficient sunlight renders usual solar cell power generation ineffective due to increased distance from sun. The history of the RTG in the U.S.A. is reviewed citing the first RTG launch in 1961 with an electrical output of 2.7 W and the improved Ulysses RTG, which provides 285 W at mission beginning and 250 W at mission end. The RTG concept is discussed including the most recent RTG technology developed by the DOE, the General Purpose Heat Source RTG (GPHS-RTG). The system relies upon heat generated by radioactive decay using radioactive plutonium-238, which is converted directly to energy using the Seebeck method.
The primary objective of STS-34 was to launch Galileo on its trip to Jupiter. The Galileo spacecraft contains two Radioisotope Thermoelectric Generators (RTG), which contains plutonium. This videotape shows and the accompanying material explains the tests that the RTG containment vessel has been subjected to, and the results of the tests. The videotape shows the trajectory of the Galileo spacecraft, a cutaway view of an RTG, the Plutonium-238 fuel capsule, and seven of the tests on the RTG.
Project Prometheus will enable a new paradigm in the scientific exploration of the Solar System. The proposed JIMO mission will start a new generation of missions characterized by more maneuverability, flexibility, power and lifetime. Project Prometheus organization is established at NASA Headquarters: 1.Organization established to carry out development of JIMO, nuclear power (radioisotope), and nuclear propulsion research. 2.Completed broad technology and national capacity assessments to inform decision making on planning and technology development. 3.Awarded five NRA s for nuclear propulsion research. 4.Radioisotope power systems in development, and Plutonium-238 being purchased from Russia. 5.Formulated science driven near-term and long-term plan for the safe utilization of nuclear propulsion based missions. 6.Completed preliminary studies (Pre-Phase A) of JIMO and other missions. 7.Initiated JIMO Phase A studies by Contractors and NASA.
This study explored the feasibility of replacing the Galileo spacecraft's plutonium-238 fueled radioisotope thermoelectric generators (RTGs) with solar arrays.
A Radioisotope Power System (RPS) generates power by converting the heat released from the nuclear decay of radioactive isotopes, such as Plutonium-238 (Pu-238), into electricity. First used in space by the U.S. in 1961, these devices have enabled some of the most challenging and exciting space missions in history, including the Pioneer and Voyager probes to the outer solar system; the Apollo lunar surface experiments; the Viking landers; the Ulysses polar orbital mission about the Sun; the Galileo mission to Jupiter; the Cassini mission orbiting Saturn; and the recently launched New Horizons mission to Pluto. Radioisotopes have also served as a versatile heat source for moderating equipment thermal environments on these and many other missions, including the Mars exploration rovers, Spirit and Opportunity. The key advantage of RPS is its ability to operate continuously, independent of orientation and distance relative to the Sun. Radioisotope systems are long-lived, rugged, compact, highly reliable, and relatively insensitive to radiation and other environmental effects. As such, they are ideally suited for missions involving long-lived, autonomous operations in the extreme conditions of space and other planetary bodies. This paper reviews the history of RPS for the U.S. space program. It also describes current development of a new Stirling cycle-based generator that will greatly expand the application of nuclear-powered missions in the future.
NASA has begun the development of a combined Stirling cycle power and cooling system (duplex) to enable the long-lived surface exploration of Venus and other harsh environments in the solar system. The duplex system will operate from the heat provided by decaying radioisotope plutonium-238 or its substitute. Since the surface of Venus has a thick, hot, and corrosive atmosphere, it is a challenging proposition to maintain sensitive lander electronics under survivable conditions. This development effort requires the integration of: a radioisotope or fission heat source; heat pipes; high-temperature, corrosion-resistant material; multistage cooling; a novel free-displacer Stirling convertor for the lander; and a minimal vibration thermoacoustic Stirling convertor for the seismometer. The first year effort includes conceptual system design and control studies, materials development, and prototype hardware testing. A summary of these findings and test results is presented in this report.
A Radioisotope Power System (RPS) generates power by converting the heat released from the nuclear decay of radioactive isotopes, such as Plutonium-238 (Pu-238), into electricity. First used in space by the U.S. in 1961, these devices have enabled some of the most challenging and exciting space missions in history, including the Pioneer and Voyager probes to the outer solar system; the Apollo lunar surface experiments; the Viking landers; the Ulysses polar orbital mission about the Sun; the Galileo mission to Jupiter; the Cassini mission orbiting Saturn; and the recently launched New Horizons mission to Pluto. Radioisotopes have also served as a versatile heat source for moderating equipment thermal environments on these and many other missions, including the Mars exploration rovers, Spirit and Opportunity. The key advantage of RPS is its ability to operate continuously, independent of orientation and distance relative to the Sun. Radioisotope systems are long-lived, rugged, compact, highly reliable, and relatively insensitive to radiation and other environmental effects. As such, they are ideally suited for missions involving long-lived, autonomous operations in the extreme conditions of space and other planetary bodies. This paper reviews the history of RPS for the U.S. space program. It also describes current development of a new Stirling cycle-based generator that will greatly expand the application of nuclear-powered missions in the future.