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At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Plutonium Oxidation State Distribution in the Presence of WIPP-Relevant Organics and Iron Corrosion Products

The oxidation state and solubility of plutonium (Pu) in high ionic strength synthetic WIPP (Waste Isolation Pilot Plant) brines as a function of pC H+ in the presence and absence of WIPP-relevant organic ligands (EDTA [Ethylenediaminetetraacetic acid], oxalate, citrate, acetate) and iron corrosion products (magnetite and metallic iron) at 𝑇 = 23 ± 2 ∘C was thoroughly studied by long-term batch solubility experiments (between approximately 800-1,100 days) from an undersaturation approach. The oxidation state of Pu in the WIPP environment has been a topic of interest since the initial Compliance Certification Application (CCA). This study aims to investigate the solubility of Pu under the expected WIPP conditions and to determine the oxidation state of the solid phase that will control the solubility. One of the most important results of this study is that the Pu oxidation state was analyzed both from the surface area of the corrosion products and in the precipitated solid. The analysis of the Pu oxidation state on the surface of the iron mineral from the ongoing undersaturated experiments is more relevant to the performance assessment of nuclear waste disposal than short term batch (plutonium-iron phase) experiments. The X-ray Absorption Near-Edge Spectroscopy (XANES) analysis showed that Pu oxidation state is different on the metal surface and in the precipitated solid. Pu(III) is the dominant oxidation state in the metallic iron (Fe 0 ) system in the presence and absence of organics. Pu(IV) is the dominant oxidation state in the magnetite system in the presence and absence of organics. Also, organics stabilize Pu(IV) in the magnetite system. Analysis of Pu in the precipitated solid by Extended X-ray Absorption Fine Structure (EXAFS) analysis showed that Pu formed an inner-sphere complex with iron with minor amounts of PuO 2 present. X-ray diffraction (XRD) results indicate that metallic iron and magnetite did not oxidize in three years in the alkaline and high ionic strength system. Under these conditions (8 < pC H+ < 10 at T = (22 ± 2) °C under nitrogen atmosphere, the solubility of Pu changes by up to three orders of magnitude (10 -5 and 10 -8 M). The spread in solubility is highest at pC H+ = 9. Pu(III) and Pu(IV) showed different solubility behavior in the synthetic WIPP brine. A summary of the data collected in this report will be submitted to Sandia National Laboratories as part of a parameter update report which will outline the changes to the OXSTAT parameter for the 2026 Compliance Recertification Application (CRA-2026). The experiments performed were done according to the U.S. Department of Energy (DOE) approved Test Plan entitled “Effects of Radiolysis, Organic Complexation, and Redox Conditions on the Speciation and Oxidation State Distribution of Pu(III/IV)” (LCO-ACP-25). All data reported were obtained under the Los Alamos National Laboratory-Carlsbad Office (LANL-CO) Quality Assurance Program, which is compliant with the DOE Carlsbad Field Office, Quality Assurance Program Document (CBFO/QAPD).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Plutonium Detection with Straw Neutron Detectors

A kilogram of weapons grade plutonium gives off about 56,000 neutrons per second of which 55,000 neutrons come from spontaneous fission of 240Pu (~6% by weight of the total plutonium). Actually, all even numbered isotopes (238Pu, 240Pu, and 242Pu) produce copious spontaneous fission neutrons. These neutrons induce fission in the surrounding fissile 239Pu with an approximate multiplication of a factor of ~1.9. This multiplication depends on the shape of the fissile materials and the surrounding material. These neutrons (typically of energy 2 MeV and air scattering mean free path >100 meters) can be detected 100 meters away from the source by vehicle-portable neutron detectors. [1] In our current studies on neutron detection techniques, without using 3He gas proportional counters, we designed and developed a portable high-efficiency neutron multiplicity counter using 10B-coated thin tubes called straws. The detector was designed to perform like commercially available fission meters (manufactured by Ortec Corp.) except instead of using 3He gas as a neutron conversion material, we used a thin coating of 10B.

plutonium, neutron, straw↗
DOE OSTI2013

Technology for Treatment of Liquid Radioactive Waste Generated during Uranium and Plutonium Chemical and Metallurgical Manufacturing in FSUE PO Mayak - 13616

Created technological scheme for treatment of liquid radioactive waste generated while uranium and plutonium chemical and metallurgical manufacturing consists of: - Liquid radioactive waste (LRW) purification from radionuclides and its transfer into category of manufacturing waste; - Concentration of suspensions containing alpha-nuclides and their further conversion to safe dry state (calcinate) and moving to long controlled storage. The following technologies are implemented in LRW treatment complex: - Settling and filtering technology for treatment of liquid intermediate-level waste (ILW) with volume about 1500m{sup 3}/year and alpha-activity from 10{sup 6} to 10{sup 8} Bq/dm{sup 3} - Membrane and sorption technology for processing of low-level waste (LLW) of radioactive drain waters with volume about 150 000 m{sup 3}/year and alpha-activity from 10{sup 3} to 10{sup 4} Bq/dm{sup 3}. Settling and filtering technology includes two stages of ILW immobilization accompanied with primary settling of radionuclides on transition metal hydroxides with the following flushing and drying of the pulp generated; secondary deep after settling of radionuclides on transition metal hydroxides with the following solid phase concentration by the method of tangential flow ultrafiltration. Besides, the installation capacity on permeate is not less than 3 m{sup 3}/h. Concentrates generated are sent to calcination on microwave drying (MW drying) unit. Membrane and sorption technology includes processing of averaged sewage flux by the method of tangential flow ultrafiltration with total capacity of installations on permeate not less than 18 m{sup 3}/h and sorption extraction of uranium from permeate on anionite. According to radionuclide contamination level purified solution refers to general industrial waste. Concentrates generated during suspension filtering are evaporated in rotary film evaporator (RFE) in order to remove excess water, thereafter they are dried on infrared heating facility. Solid concentrate produced is sent for long controlled storage. Complex of the procedures carried out makes it possible to solve problems on treatment of LRW generated while uranium and plutonium chemical and metallurgical manufacturing in Federal State Unitary Enterprise (FSUE) Mayak and cease its discharge into open water reservoirs. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2013

Removal of the Plutonium Recycle Test Reactor - 13031

The 309 Facility housed the Plutonium Recycle Test Reactor (PRTR), an operating test reactor in the 300 Area at Hanford, Washington. The reactor first went critical in 1960 and was originally used for experiments under the Hanford Site Plutonium Fuels Utilization Program. The facility was decontaminated and decommissioned in 1988-1989, and the facility was deactivated in 1994. The 309 facility was added to Comprehensive Environmental Response, Compensation, and Liability Act (CERCLA) response actions as established in an Interim Record of Decision (IROD) and Action Memorandum (AM). The IROD directs a remedial action for the 309 facility, associated waste sites, associated underground piping and contaminated soils resulting from past unplanned releases. The AM directs a removal action through physical demolition of the facility, including removal of the reactor. Both CERCLA actions are implemented in accordance with U.S. EPA approved Remedial Action Work Plan, and the Remedial Design Report / Remedial Action Report associated with the Hanford 300-FF-2 Operable Unit. The selected method for remedy was to conventionally demolish above grade structures including the easily distinguished containment vessel dome, remove the PRTR and a minimum of 300 mm (12 in) of shielding as a single 560 Ton unit, and conventionally demolish the below grade structure. Initial sample core drilling in the Bio-Shield for radiological surveys showed evidence that the Bio-Shield was of sound structure. Core drills for the separation process of the PRTR from the 309 structure began at the deck level and revealed substantial thermal degradation of at least the top 1.2 m (4LF) of Bio-Shield structure. The degraded structure combined with the original materials used in the Bio-Shield would not allow for a stable structure to be extracted. The water used in the core drilling process proved to erode the sand mixture of the Bio-Shield leaving the steel aggregate to act as ball bearings against the core drill bit. A redesign is being completed to extract the 309 PRTR and entire Bio-Shield structure together as one monolith weighing 1100 Ton by cutting structural concrete supports. In addition, the PRTR has hundreds of contaminated process tubes and pipes that have to be severed to allow for a uniformly flush fit with a lower lifting frame. Thirty-two 50 mm (2 in) core drills must be connected with thirty-two wire saw cuts to allow for lifting columns to be inserted. Then eight primary saw cuts must be completed to severe the PRTR from the 309 Facility. Once the weight of the PRTR is transferred to the lifting frame, then the PRTR may be lifted out of the facility. The critical lift will be executed using four 450 Ton strand jacks mounted on a 9 m (30 LF) tall mobile lifting frame that will allow the PRTR to be transported by eight 600 mm (24 in) Slide Shoes. The PRTR will then be placed on a twenty-four line, double wide, self powered Goldhofer for transfer to the onsite CERCLA Disposal Cell (ERDF Facility), approximately 33 km (20 miles) away. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2013

Multiple recycle of REMIX fuel based on reprocessed uranium and plutonium mixture in thermal reactors

REMIX fuel consumption in WWER-1000 is considered. REMIX fuel is fabricated from non-separated mixture of uranium and plutonium obtained during NPP spent fuel reprocessing with further makeup by enriched natural uranium. It makes possible to recycle several times the total amount of uranium and plutonium obtained from spent fuel with 100% loading of the WWER-1000 core. The stored SNF could be also involved in REMIX fuel cycle by enrichment of regenerated uranium. The same approach could be applied to closing the fuel cycle of CANDU reactors. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2013

New method of uranium and plutonium extraction in reprocessing of the spent nuclear fuel

It is shown that a two-stage process of uranium and plutonium extraction during the reprocessing of spent nuclear fuel solves the problem of obtaining a high-concentrated extract without increasing the loss risk with raffinate and avoids the accumulation of plutonium in the unit. A possible further optimization of the process would be the creation of steps inside the stages.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Remote Decommissioning of the Plutonium Experimental Extraction Facility, Sellafield - 17031

A redundant suite of gloveboxes formerly used for an experimental plutonium extraction process required decommissioning to avoid further degradation and a risk to other users of the Analytical Services building on Sellafield site. Following a full option selection process, remote techniques were chosen as the most appropriate (i.e. ALARP) decommissioning method. A nearby ventilation system from a previous project was re-engineered to ventilate the laboratory. Gloveboxes in neighbouring labs were cleared to create space to install a personnel access facility. The containment was reinforced where necessary to provide adequate protection from the remote machinery. Following a campaign of manual waste removal, including approximately 21 tonnes of lead chevron bricks released as exempt waste, a Brokk{sup R} 90 remotely-operated vehicle (ROV) was deployed to perform remote size reduction of the glovebox suite. The resulting plutonium-contaminated material (PCM) was delivered to a Kraft Raptor manipulator for sorting and consignment to an on-site store in 200-litre drums. Despite indications from pre-decommissioning surveys of the presence of ILW in the shielded section, none was found. Following the successful removal of the glovebox suite, and the emergence during the project of additional redundant gloveboxes within the Analytical Services building, the Remediation team has taken the opportunity to retain the decommissioning infrastructure as a remote glovebox breakdown facility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Preparing for safe and compliant open air demolition at Hanford's plutonium finishing plant - 15100

The Plutonium Finishing Plant (PFP), located in the 200 West Area of the U.S. Department of Energy (DOE) Hanford Site, began operations in 1949 and produced plutonium metal during the Cold War. Production was stopped in 1989, the facility was formally shut-down in 1996, and material stabilization completed in 2004. DOE contractor CH2M HILL Plateau Remediation Company (CH2M HILL) is tasked with the plant's deactivation, decommissioning, decontamination and demolition, to be completed by September 30, 2016. The project team, partnering with DOE-Richland Operations Office (DOE-RL), is exploring, evaluating and implementing efficiencies to safely and compliantly prepare the facility for demolition. Since 2008, employees have prepared approximately 75 percent of the complex for demolition. More than 90 percent of the 232 glove boxes have been removed from ventilation and more than 80 percent of pencil tank units have been dispositioned. As decontamination, deactivation and removal nears completion on the remaining glove boxes, pencil tanks and other radiological and chemical processing infrastructure, CH2M HILL and DOE-RL are making preparations to demolish PFP itself, a Hazardous Category II nuclear facility (HazCat II). Conventional techniques used to demolish buildings heavily contaminated with radiological hazards typically involve extensive hands-on work to remove Material at Risk (MAR) and decontaminate the building to low levels before conventional demolition techniques can be used to remove the building. A safe and more cost effective approach is packaging MAR located in hard to access areas of the plant and removing it during demolition. That process, combined with affixing remaining contamination to walls, floors and equipment, performing detailed air dispersion modeling before demolition and air monitoring and dust suppression during demolition, will reduce employee risk and is more efficient in demolishing a HazCat II facility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Measurement of the plutonium hold-up in glove box before dismantling - 15111

The French Bruyeres-Le-Chatel CEA (Commissariat a l'Energie Atomique et aux Energies Alternatives - French Alternatives Energies and Atomic Energy Commission) research center is going through a period of cleaning and dismantling of theses old treatment facilities on fissile materials and others associated nuclides. Some very large glove boxes contained some machines like melting furnace which can't be moved and are dismantled in situ. We need to evaluate the quantity of fissile materials to prevent criticality risk, to bring the evidence to the safety authority, to manage for the best the radioprotection of the workers and to manage waste production. A melting furnace in a glove box was dismantled. Measurements by gamma spectrometry with an HPGe detector (High Purity Germanium) and passive neutron counting (coincidence counting with shift register) are done in situ (furnace in the glove box). In order to refine the measurements, some data acquisitions by sector of glove box were carried out. In view of the geometries to characterize, some modelings have been created, in order to correct the different attenuations and to determine the plutonium masses content in the glove box, including the use of infinite energy technique. For the measurement by passive neutron counting (coincidence counting with shift register), we have used two slabs in high density polythene including nine He3 counters in each slab. This measurement technique is complementary to gamma spectrometry, and allows quantizing the fissile material which would be included in interstice of high Z material. The 100-L and 200-L drums produced during the dismantling were also measured. Based on simplified assumptions to analyze in situ measurements, plutonium weight could be evaluated. This approach of measurement in amount, during and after dismantling, has allowed to quantize the fissile material mass present in the glove box and didn't produce waste package which wouldn't respected the technical specifications of storage outlets. The results show good agreement between in situ and waste measurements. (authors)

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2016

Progression of Safe and Compliant Demolition of Hanford's Plutonium Finishing Plant - 16566

Department of Energy contractor CH2M HILL Plateau Remediation Company (CH2M) is about to begin demolition of the Plutonium Finishing Plant (PFP). The facility is located on the Hanford Site and produced plutonium metal during the Cold War. Production was stopped in 1988, the facility was formally shut-down in 1996 and material processing completed in 2004. The project team, partnering with DOE-Richland Operations Office (DOE-RL), is in the final stages of preparing to demolish the building by the Tri-Party Agreement Milestone date of September 30, 2016. Since 2008, employees have prepared approximately 85 percent of the building for demolition. All of the 52 pencil-shaped processing tanks and 95 percent of the 238 glove boxes have been removed. Work is progressing on dispositioning remaining glove boxes, filter boxes and ventilation ducts and chemical and drain lines. Demolition is scheduled to start in early 2016. In addition to wrapping up tasks like source term removal (or preparation for removal during pre-demolition) and decontamination, the project is also developing the strategy and process to perform physical open air demolition, including the use of 3D renderings and computer generated illustrations of building infrastructure to safely and compliantly demolish the building. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Developing a new criticality methodology to support decommissioning of legacy plutonium facilities

To decommission a legacy plutonium finishing facility, a number of gloveboxes need to be disposed of. These gloveboxes have been in place since the 1960's and were operational until the 1980's. A period of initial clean out and decommissioning took place in the 1990's and the first gloveboxes were removed from the line in the early 2000's. Compliance with downstream waste handling facility requirements meant that the gloveboxes needed to be removed using intensive 'hands-on' methods in order to size reduce them to fit into 200 litre (55 gallon) drums. This is the standard approach for handling waste items known as Plutonium Contaminated Material (PCM) on the Sellafield site and was credited in the criticality safety case for the decommissioning of the gloveboxes as it allowed each waste drum to be individually assayed such that the fissile content of the waste could be known. Not only was this approach time-consuming and laborious but as it involved operators working with cutting tools in a highly contaminated area it was challenged as being overly restrictive to operations and potentially hazardous to the workers. In order to decommission the remaining nine gloveboxes in the facility, a new decommissioning approach and associated criticality methodology has been developed. Instead of intensive size reduction and waste drum assay, the gloveboxes will be removed with little or no size reduction and put into storage crates without assay. The criticality assessor will review the operational history of each glovebox, along with the decommissioning records and relevant plant data, to make an evidence-based judgement that the crated glovebox represents no greater a residual criticality risk than would have been realised from the equivalent number of PCM drums that the standard decommissioning approach would have generated. This method identifies, in conjunction with the plant personnel, a number of review points to ensure that before the glovebox is removed any bulk residue material has been recovered and no more than a safe amount of moderating material (fixative) has been added to fix any remaining fissile contamination. Finally, once these review points have been confirmed to be complete - through a stakeholder meeting with criticality safety, plant operators and project managers - the glovebox will be placed in a crate, and this crate will be declared a Low Criticality Risk crate. No formal assay will be required prior to exporting the crate to the downstream waste handling facility and no fissile mass value will be assigned to the contents of the crate. No further intrusive work will be required on the crate and it can be safely stored without any spacing requirements, pending final disposal. (author)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Lessons Learned from Demolition of Hanford's Plutonium Finishing Plant - 20507

U.S. Department of Energy (DOE) contractor CH2M Hill Plateau Remediation Company (CHPRC), a Jacobs owned company, is making significant progress demolishing the Plutonium Finishing Plant (PFP), which has long been known as one of the most hazardous buildings in the DOE Environmental Management Complex (DOE Complex). The facility is located on the Hanford Site and produced plutonium metal during the Cold War. Production was stopped in 1989, the facility was formally shut down in 1996, and material processing was completed in 2004. After approximately 25 years of demolition preparations, open-air demolition of the main portions of the Hazard Category II nuclear facility began in November 2016. To prepare the PFP for demolition, CHPRC employees performed some of the most hazardous work across the DOE Complex. In addition to extensive demolition preparations, including a wide-reaching communication strategy across the Hanford Site, CHPRC implemented robust controls and monitoring during demolition, and when necessary, adjusted demolition practices and sequence to maintain employee safety and project efficiency. Demolition of the main PFP building began in November 2016. The technical complexity, high hazards and radiological concerns have all led to a difficult demolition environment. Following a spread of contamination at the project site beyond the radiological boundaries in December 2017, work was halted and a recovery plan was generated to allow the demolition work to continue. After the implementation of additional controls and concurrence from regulatory agencies and DOE, the demolition was ready to resume work and reinitiated in August 2018. There are a number of lessons learned from the demolition activities and recovery plan process. This paper allows CHPRC and DoE's Richland Operations Office (RL) to share lessons learned and progress to date with other challenging and hazardous projects across the DOE Complex. Understanding the risk acceptance level is critical to execution of any open-air demolition project and is unique to each facility. Four key lessons learned from this project include: 1) plan execution issues, 2) stakeholder communication issues, 3) watching for summit fever and 4) minimizing exposed contaminated surfaces during demolition. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Combined Effort to De-Inventory the New Brunswick Laboratory of Plutonium Certified Reference Materials - 20504

To de-inventory plutonium Certified Reference Materials standards (CRMs) from the New Brunswick National Laboratory (NBL), the Argonne National Laboratory (ANL) and Savannah River National Laboratory (SRNL) formed a unique team. This teaming arrangement leveraged the different capabilities and expertise of both laboratories, helping to ensure the effort would be performed both safely and cost-effectively. With the NBL then physically housed on the ANL site, ANL served as the host-site, providing the necessary facilities and support services (e.g., supplying everything from hoods, loading equipment, and scales to Health Physics supports). From a packaging perspective, ANL's responsibilities focused mainly on characterizing and preparing the contents for shipment, followed by performing the Shipper of Record activities. With SRNL being the Package Design Authority of the 9978, the Type B packaging used for this effort, SRNL's scope included developing a Safety Analysis Report in Packaging (SARP) Letter Amendment to add the CRMs as authorized contents to the 9978. Recognizing competency, ANL prodigiously tasked SRNL to perform the actual loading of the CRMs into the 9978s, while physically on the ANL site. This paper details five different aspects of this effort. They are: 1. Characterization/validation of the CRM contents. 2. Development of the 9978 SARP Letter Amendment for the content change. 3. Development of the nitrogen inerting method to address SARP identified potential flammability concerns. 4. Renewal of the SRNL 9978 loading procedure. 5. Performance of the actual work execution activities. In 2017, the first nine packages were successfully loaded and shipped from NBL, while in 2019, the last ten were successfully loaded and planned for shipment. Without ANL leveraging SRNL's strengths, the de-inventorying of NBL of its plutonium CRMs would have likely taken many years longer. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Characterization of Plutonium-Contaminated Gloveboxes using a High-Range Alpha Ion Chamber

Between September 2014 and July 2015, personnel at Lawrence Livermore National Laboratory (LLNL) decontaminated, characterized, and removed six high-activity plutonium-contaminated gloveboxes from the Building 332 Plutonium Facility. This project was based on similar decommissioning work that was done at the Rocky Flats Environmental Technology Site (RFETS), using a Ludlum Model 43-132 ion chamber with Model 195 readout unit. This summary describes the process that was used at LLNL to characterize all six gloveboxes as low-level waste. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Forensic investigation of plutonium metal: a case study of CRM 126

In our study, a certified plutonium metal reference material (CRM 126) with a known production history is examined using analytical methods that are commonly employed in nuclear forensics for provenancing and attribution. Moreover, the measured plutonium isotopic composition and actinide assay are consistent with values reported on the reference material certificate. Model ages from U/Pu and Am/Pu chronometers agree with the documented production timeline. Finally, these results confirm the utility of these analytical methods and highlight the importance of a holistic approach for forensic study of unknown materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Static, mixed-array total evaporation for improved quantitation of plutonium minor isotopes in small samples

Actinide isotope measurements are a critical signature capability in the modern nuclear forensics “toolbox”, especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10 -6 ) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Furthermore, results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Ab initio modeling and thermodynamics of hydrated plutonium oxalates

An ab initio study on the plutonium oxalate hydrates: Pu 2 (C 2 O 4 ) 3 ·10H 2 O and Pu(C 2 O 4 ) 2 ·6H 2 O, using PBE exchange-correlation with D3 dispersion correction and Hubbard correction for the plutonium atoms, was performed and compared to experimental vibrational spectral and thermodynamic property values. Here we demonstrated that this technique can accurately predict the experimental infrared spectra Pu(III) oxalate hydrate, as well as the Raman peak of PuO 2 (used to calculate the thermodynamic properties of the oxalates). For Pu(IV) oxalate hydrate we found that our predicted structure agreed qualitatively with PXRD measurements, the only available experimental determination of the structure. Using this method at standard temperature and pressure, we predicted standard enthalpies of formation of -6,755 kJ mol -1 and -3,923 kJ mol -1 and standard Gibbs free energy of formation of -5,899 kJ mol -1 and -3,386 kJ mol -1 for Pu 2 (C 2 O 4 ) 3 ·10H 2 O and Pu(C 2 O 4 ) 2 ·6H 2 O, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Plutonium migration and phase evolution in irradiated U-Pu-Zr metallic fuels: An integrated EPMA-SEM-TEM study

Constituent redistribution is a defining feature of irradiated U-Pu-Zr metallic fuels, yet its mechanisms and effects on fuel performance are not sufficiently resolved to guide model development. Although decades of irradiation testing have established broad trends, a true mechanistic understanding of constituent redistribution has not been achieved. Here, in this study, we use electron probe microanalysis (EPMA), scanning electron microscopy (SEM), and transmission electron microscopy-based (TEM) selective area electron diffraction (SAED) on a EBR-II irradiated U-19 wt.% Pu-6 wt.% Zr fuel pin cross-section to correlate the composition, porosity, and crystallographic phases formed after irradiation. Constituent redistribution is thought to consist of three distinct zones, in which uranium and zirconium migrate while plutonium remains relatively unchanged. Our EPMA results resolve eight distinct compositional regions, and more importantly, show that plutonium redistributes alongside zirconium, contrary to historical assumptions. The distribution of fission products was highly asymmetric with a few large lanthanide precipitates observed at isolated sites on the pin periphery instead of a uniform distribution of smaller precipitates around the periphery. Using thermodynamic data from TAF-ID and the measured EPMA compositions, matrix phase fractions were predicted across the fuel radius. Phase predictions based on composition did not match TEM/SAED results, which revealed a much higher fraction of α−U phase than would be expected if phases were retained from reactor temperatures. These findings highlight the need for expanded SAED phase identification to capture post-irradiation and storage effects, as well as rigorous uncertainty quantification in fuel performance and phase diagram modeling to better constrain predictions from compositional data.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗