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DOE OSTI2026

Recent Advances in Cladding Material Extraction from Fuels in Nuclear Fuel Cycles

An improved recycling and recovery process for the cladding material from spent nuclear fuels is very important toward confirming nuclear energy to support ongoing sustainable development of nuclear management by reducing waste and conserving resources. Nuclear spent fuel cladding materials such as zirconium alloys have economic values and can be recovered, and their recovery eliminates problems in waste disposal and conserves valuable resources. Over 110 published reports and journal articles are reviewed and summarized herein, with a main focus on documenting recovery techniques used to recover cladding materials from spent nuclear fuel and recent developments. Several recovery techniques which are used at present times, such as mechanical separation, chemical dissolution, and hydrometallurgical processes have been covered with examples and discussions. Difficulties within the recovery process are also discussed, and most probable areas for future research in improving efficiency and sustainability of recovering cladding material are identified and discussed at the end. Here, this review could be an important document to the field of spent nuclear fuel reprocessing, recovering valuables and thereby offering guidance on how to effectively manage, safely handle, and reduce nuclear waste. In addition to reducing the volume and radiotoxicity of high-level waste, this review also highlights the potential economic benefit of recovering zirconium from spent fuel cladding by relating typical zirconium metal prices to the mass of cladding per tonne of spent fuel, illustrating that the recoverable material value is non-negligible compared with back-end fuel-cycle costs.

Mondal, Kunal [Oak Ridge National Laboratory (ORNL↗

NASA NTRS1977

An analysis of the back end of the nuclear fuel cycle with emphasis on high-level waste management, volume 1

The programs and plans of the U.S. government for the "back end of the nuclear fuel cycle" were examined to determine if there were any significant technological or regulatory gaps and inconsistencies. Particular emphasis was placed on analysis of high-level nuclear waste management plans, since the permanent disposal of radioactive waste has emerged as a major factor in the public acceptance of nuclear power. The implications of various light water reactor fuel cycle options were examined including throwaway, stowaway, uranium recycle, and plutonium plus uranium recycle. The results of this study indicate that the U.S. program for high-level waste management has significant gaps and inconsistencies. Areas of greatest concern include: the adequacy of the scientific data base for geological disposal; programs for the the disposal of spent fuel rods; interagency coordination; and uncertainties in NRC regulatory requirements for disposal of both commercial and military high-level waste.

Source record↗

NASA NTRS1976

Application of gaseous core reactors for transmutation of nuclear waste

An acceptable management scheme for high-level radioactive waste is vital to the nuclear industry. The hazard potential of the trans-uranic actinides and of key fission products is high due to their nuclear activity and/or chemical toxicity. Of particular concern are the very long-lived nuclides whose hazard potential remains high for hundreds of thousands of years. Neutron induced transmutation offers a promising technique for the treatment of problem wastes. Transmutation is unique as a waste management scheme in that it offers the potential for "destruction" of the hazardous nuclides by conversion to non-hazardous or more manageable nuclides. The transmutation potential of a thermal spectrum uranium hexafluoride fueled cavity reactor was examined. Initial studies focused on a heavy water moderated cavity reactor fueled with 5% enriched U-235-F6 and operating with an average thermal flux of 6 times 10 to the 14th power neutrons/sq cm-sec. The isotopes considered for transmutation were I-129, Am-241, Am-242m, Am-243, Cm-243, Cm-244, Cm-245, and Cm-246.

Schnitzler, B. G.↗

DOE OSTI2026

Quantitative 14 N NMR with Monte Carlo Uncertainty Analysis of Nitrate/Nitrite in Alkaline Nuclear Waste

While monitoring of nitrate and nitrite concentrations is important for managing corrosion in nuclear waste systems, existing analytical methods are hindered by turbidity, spectral interference, and delays from sample handling. Here, we demonstrate quantitative 14 N nuclear magnetic resonance (qNMR) spectroscopy as a direct, matrix-tolerant approach for nitrate and nitrite detection at natural abundance. Monte Carlo resampling was integrated into the workflow to quantify random error, establish precision–time tradeoffs, and separate noise-limited uncertainty from systematic bias arising from shimming, transmitter offset, or excitation pulse conditions. Quantification of nitrate and nitrite were validated in controlled alkaline matrix challenges and in 18-component Hanford-type simulants. These results establish 14 N qNMR as a practical, uncertainty-bounded tool for monitoring redox-active nitrogen species in chemically complex environments and provide a generalizable framework for quantitative analysis of quadrupolar nuclei.

Graham, Trent R. [Pacific Northwest National Labor↗

DOE OSTI2026

Lessons Learned from Site Selection Efforts for Deep Geological Disposal

This report discusses international experiences from site selection of deep geological repositories (DGR) for radioactive waste disposal. Based on experiences from three countries with recent or ongoing site selections, the report describes different site selection approaches and summarizes lessons learned. The German and Swiss programs are two slightly different examples of one end of the spectrum of potential siting approaches: Starting with the entire country, a technically based downselection is performed to select the repository site. The Canadian program is an example of the other end of the spectrum: Here, the program started with an extensive engagement program with Canadians to collaboratively develop a socially acceptable and technically sound national approach for the long-term management of used nuclear fuel. This was followed by the launch of a collaboratively developed consent-based siting process designed to seek an informed and willing host with suitable sites, considering both technical and community well-being site requirements.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI1993

Nuclear Safety [Vol. 34, No. 1, January-March 1993]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 An Integrated Regional Approach To Risk Management of Industrial Systems, S. Chakraborty and R. Stratton; 9 Annual Technical Meeting of the NRC Cooperative Severe Accident Research Program, E. G. Silver; ACCIDENT ANALYSIS: 13 Deterministic Severe Accident Criteria as Severe Accident Design Criteria and Policy for the New Production Reactor-Heavy Water Reactor, P. T. Rhoads; 20 Proposed Deterministic Severe Accident Criteria for the Heavy Water Reactor-New Production Reactor Containment, K. D. Bergeron, S. E. Slezak, and C. E. Leach; 33 Quasi-Static Core Liquid Level Depression and Long-Term Core Uncovery During a PWR LOCA, Y. Kukita, R. R. Schultz, H. Nakamura, and J. Katayama; 49 LIRA: An Advanced Containment System to Minimize the Accidental Radioactivity Releases, A. Turricchia; 63 Errata to “A Review of Hydrogen Production During Melt/Water Interaction in LWRs,” Vol. 33, No. 4; CONTROL AND INSTRUMENTATION: 64 The Nuplex 80+™ Advanced Control Complex from ABB Combustion Engineering, F. Ridolfo, D. Harmon, and K. Scarola; DESIGN FEATURES: 76 A Scheme for Passive Isolation of the Containment of a Reactor, A. K. Ghosh, V. V. Raj, and K. Kakodkar; 84 Utility Requirements for Safety in the Passive Advanced Light-Water Reactor, T. U. Marston, W. H. Layman, and G. Bockhold, Jr.; WASTE AND SPENT FUEL MANAGEMENT: 91 Activities Related to Waste and Spent Fuel Management, Compiled by M. D. Muhlheim and E. G. Silver; OPERATING EXPERIENCES: 103 Testing Deficiencies in Auxiliary Systems Feedwater Systems, J. D. Kueck; 110 Reactor Shutdown Experience, Compiled by J. W. Cletcher; 113 Selected Safety-Related Events, Compiled by G. A. Murphy; 115 Operating U.S. Power Reactors, Compiled by M. D. Muhlheim and E. G. Silver; RECENT DEVELOPMENTS: 133 General Administrative Activities, Compiled by M. D. Muhlheim and E. G. Silver; 145 Reports, Standards, and Safety Guides, D. S. Queener; 150 Proposed Rule Changes as of Sept. 30, 1992; ANNOUNCEMENTS: 75 Harvard Short Course on Risk: Science, Assessment, and Management; 102 International Conference on Reactor Physics and Reactor Computations; 102 The Fourth International Conference on Nuclear Waste Reprocessing and Waste Management [RECOD ’94]; 132 International Symposium on the Radiological Exposure of the Population of the European Community from Radioactivity in the Mediterranean Sea [MARINA-MED]; 162 International High-Level Radioactive Waste Conference ‘Technology Integration—Above and Below”; 154 The Authors; 158 Indexes to Nuclear Safety, Volume 33.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Low Activity Waste Glass Optimization with Property Models from Machine Learning, Part 2: Experimental Validation and Active Learning

The United States Department of Energy is responsible for managing legacy nuclear waste stored in underground tanks at the Hanford Site. To treat the waste, it is planned as the current baseline to separately vitrify low-activity waste (LAW) and high-level waste fractions. Previously, machine learning (ML) based glass property models (e.g., chemical durability, viscosity, electrical conductivity and SO3 solubility) were developed with prediction uncertainties. A waste glass optimization approach was then established to enable the capability of using these ML models in LAW glass formulation. In this study, the previous ML models were first experimentally validated, and the results were incorporated back into the database to update the ML models. The updated models and formulations showed increased waste loading while reducing the failure rate, demonstrating improved predictive accuracy, reduced uncertainties, and the effectiveness of active learning in guiding high-dimensional, nonlinear LAW glass design. This represents the first experimental validation of ML based LAW glass formulation, with practical benefits such as higher waste loading, shorter mission duration, and lower operational risk.

Lu, Xiaonan (ORCID:0000000179708148)↗

DOE OSTI1993

Nuclear Safety [Vol. 34, No. 1, January-March 1993]

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI1978

An Assessment of the Nevada Test Site for Low-Level Waste Management

This report presents a summary of description information, facilities, and operating practices at the Nevada Test Site. It is concluded that NTS is not only a feasible location for surface and near-surface storage of low-level wastes, but also a potential site for underground storage of higher level wastes.

052002* -- Nuclear Fuels-- Waste Disposal & Storag↗

NASA NTRS1982

Aerospace technology and commercial nuclear power; Proceedings of the Workshop Conference, Williamsburg, VA, November 18-20, 1981

An attempt has been made to compare the technologies, institutions and procedures of the aerospace and commercial nuclear power industries, in order to characterize similarities and contrasts as well as to identify the most fruitful means by which to transfer information, technology, and procedures between the two industries. The seven working groups involved in this study took as their topics powerplant design formulation and effectiveness, plant safety and operations, powerplant control technology and integration, economic and financial analyses, public relations, and the management of nuclear waste and spent fuel. Consequential differences are noted between the two industries in matters of certification and licencing procedures, assignment of responsibility for both safety and financial performance, and public viewpoint. Areas for beneficial interaction include systems management and control and safety system technology. No individual items are abstracted in this volume

Grey, J.↗

DOE OSTI2025

An international study on THM modelling of the full-scale heater experiment at Mont Terri laboratory

We present results from an international model comparison study of the Full-Scale Emplacement (FE) experiment in Opalinus Clay at the Mont Terri Laboratory, Switzerland. Based on a provided parameter set the teams decided which parameters they adopted for their models, whether they considered the excavation and the ventilation phase in addition to the heating phase and if they included technical features like the shotcrete or the EDZ. The teams were able to reproduce the measured parameters temperature, relative humidity and pore pressure. The modelled results for temperature agree very closely between the teams especially in the sensors in Opalinus Clay. All teams were able to reproduce the redistribution of water in the bentonite backfill due to heating. The evolution of the relative humidity showed similar trends with differences in the intensity of the dry out effect. To model the pore pressure evolution is more complex because it comprises the full interaction of the coupled THM processes. The spread between the pore pressure modelled by the teams was larger, with some teams overestimating the pressure increase due to heating and some teams overestimating the extent of drainage. The agreement of modelled results with measurements improves with larger distance to the heater. We conclude that the EDZ and the shotcrete potentially influence the behaviour of the rock causing higher differences closer to the heater. Further research is needed to better implement those influences into the models. Based on the calibrated models, the future evolution of temperature, relative humidity and pore pressure was predicted over the next 10 years following a change of the heat power applied in 2023 and 2024. Again, the predicted temperatures agree very closely between the teams. Most teams do not expect an increase in relative humidity during the next 10 years after the initial dry-out.

58 GEOSCIENCES↗

DOE OSTI2025

Spent nuclear fuel receipt rate analysis within an integrated waste management system (IWMS) architecture that includes consolidated storage

A key parameter in analyzing the performance of an integrated waste management system (IWMS) architecture for the disposition of spent nuclear fuel (SNF) is the SNF receipt rate from reactor and other custodian sites. Receipt rate in this paper means how much SNF is accepted per year for transport in the IWMS from such sites. Introducing one or more federal consolidated interim storage facilities (CISFs) into the IWMS architecture can potentially accelerate the receipt rate profile over time relative to system architectures without a CISF. This raises the question of what an optimal SNF receipt rate profile for an IWMS architecture might be in view of practical constraints and desired system performance attributes and associated metrics. This paper describes a sensitivity study on SNF receipt rates and the associated results for a selected set of IWMS scenarios aimed at informing near-term planning for interim storage capabilities and transportation assets. Two different strategies for CISF operation while awaiting availability of a disposal system to receive SNF are compared: one that relatively quickly fills an initial CISF and then idles the transportation system; and another that aims for more continuous use of transportation assets and receipt capabilities at the CISF. This study examines cost considerations and other factors, such as the timing of clearing reactor sites of SNF, efficient use of capital assets, and some other metrics that might be important to a CISF host community. Based on the analysis, an initial approach is presented that targets a continuous receipt strategy while maintaining the flexibility to step up receipt capabilities to a reasonable degree when needed and beneficial, within overall system constraints.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI1996

Nuclear Safety [Vol. 37, No. 1, January-March 1996]

Nuclear Safety is a journal that covers significant issues in the field of nuclear safety. Its primary scope is safety in the design, construction, operation, and decommissioning of nuclear power reactors worldwide and the research and analysis activities that promote this goal, but it also encompasses the safety aspects of the entire nuclear fuel cycle, including fuel fabrication, spent-fuel processing and handling, and nuclear waste disposal, the handling of fissionable materials and radioisotopes, and the environmental effects of all these activities. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 A Decision Support System for Maintenance Management of a Boiling-Water Reactor Power Plant, J. H. Shen, A. Ray, and S. Levine; ACCIDENT ANALYSIS: 12 On Prediction of the Ignition Potential of Uranium Metal and Hydride, M. Epstein, W. Luangdilok, M. G. Plys, and H. K. Fauske; 26 An Overview of the Primary Parameters and Methods for Determining Condensation Heat Transfer to Containment Structures, J. Green and K. Almenas; DESIGN FEATURES: 49 Modem Tornado Design of Nuclear and Other Potentially Hazardous Facilities, J. D. Stevenson and Y. Zaho; U.S. NUCLEAR REGULATORY COMMISSION INFORMATION AND ANALYSES: 73 1994 Accident Sequence Precursor Program Results, R. J. Belles, J. W. Cletcher, D. A. Coplnger, B. W. Dolan, J. W. Minarick, and P. D. O'Reilly; ANNOUNCEMENTS: 93 American Institute of Chemical Engineers (AlChE) Spring 1997 National Meeting; 94 European Safety and Reliability Association International Conference on Safety and Reliability ESREL ’97; 95 Criticality Safety Challenges in the Next Decade; 96 21st International Symposium on the Scientific Basis for Nuclear Waste Management; 84 The Authors; 88 Letter to the Editor; 90 Indexes to Nuclear Safety, Volume 36.

05 NUCLEAR FUELS↗

DOE OSTI1996

Nuclear Safety [Vol. 37, No. 1, January-March 1996]

Nuclear Safety is a journal that covers significant issues in the field of nuclear safety. Its primary scope is safety in the design, construction, operation, and decommissioning of nuclear power reactors worldwide and the research and analysis activities that promote this goal, but it also encompasses the safety aspects of the entire nuclear fuel cycle, including fuel fabrication, spent-fuel processing and handling, and nuclear waste disposal, the handling of fissionable materials and radioisotopes, and the environmental effects of all these activities. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 A Decision Support System for Maintenance Management of a Boiling-Water Reactor Power Plant, J. H. Shen, A. Ray, and S. Levine; ACCIDENT ANALYSIS: 12 On Prediction of the Ignition Potential of Uranium Metal and Hydride, M. Epstein, W. Luangdilok, M. G. Plys, and H. K. Fauske; 26 An Overview of the Primary Parameters and Methods for Determining Condensation Heat Transfer to Containment Structures, J. Green and K. Almenas; DESIGN FEATURES: 49 Modem Tornado Design of Nuclear and Other Potentially Hazardous Facilities, J. D. Stevenson and Y. Zaho; U.S. NUCLEAR REGULATORY COMMISSION INFORMATION AND ANALYSES: 73 1994 Accident Sequence Precursor Program Results, R. J. Belles, J. W. Cletcher, D. A. Copinger, B. W. Dolan, J. W. Minarick, and P. D. O'Reilly; ANNOUNCEMENTS: 93 American Institute of Chemical Engineers (AlChE) Spring 1997 National Meeting; 94 European Safety and Reliability Association International Conference on Safety and Reliability ESREL ’97; 95 Criticality Safety Challenges in the Next Decade; 96 21st International Symposium on the Scientific Basis for Nuclear Waste Management; 84 The Authors; 88 Letter to the Editor; 90 Indexes to Nuclear Safety, Volume 36.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI1992

Nuclear Safety [Vol. 33, No. 4, October-December 1992]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 499 Technical Note: Nuclear Regulatory Commission’s Examination Question Bank System, C. L Jensen and N. L. Skinner; 506 Report on the Specialists’ Meeting on Passive and Active Safety Features of Liquid-Metal Fast Breeder Reactors Organized by the International Atomic Energy Agency at Oarai Engineering Centre of Power Reactor and Nuclear Development Corporation, Japan, November 5-7,1991, S. R. Paranjpe; ACCIDENT ANALYSIS: 514 A Review of Hydrogen Production During Melt/Water Interaction in LWRs, D. F. Fletcher, B. D. Turland, and S. P. A. Lawrence; 535 A Review of the U 3 0 8 -Al Reaction as a Potential Heat Source in Research and Test Reactor Accidents, J. L. Snelgrove; CONTROL AND INSTRUMENTATION: 543 Multilevel Interfaces for Power Plant Control Rooms II: A Preliminary Design Space, K. J. Vicente; DESIGN FEATURES: 549 Twenty-Second DOE/NRC Nuclear Air Cleaning and Treatment Conference, R. R. Bellamy, D. W. Moeller, and M. W. First; 562 Book Review: Safety Assessment of Unit 5 (WWER-440/W-213) of the Greifswald Nuclear Power Station, M. H. Fontana; WASTE AND SPENT FUEL MANAGEMENT: 576 Activities Related to Waste and Spent Fuel Management, M. D. Muhlheim and E. G. Silver; OPERATING EXPERIENCES: 586 Analysis of Corrective Actions Applied to Nuclear Power Plant Operations, A. E. Cross; 593 Reactor Shutdown Experience, Compiled by J. W. Cletcher; 596 Operating U.S. Power Reactors, Compiled by M. D. Muhlheim and E. G. Silver; 609 Non-Commercial Power Operating Experience; 614 World Nuclear Performance, Compiled by M. D. Muhlheim; RECENT DEVELOPMENTS: 623 General Administrative Activities, Compiled by M. D. Muhlheim and E. G. Silver; 635 Reports, Standards, and Safety Guides, D. S. Queener; 639 Proposed Rule Changes as of June 30, 1992; ANNOUNCEMENTS: 513 Fourth International Conference on Nuclear Fuel Reprocessing and Waste Management RECOD '94; 585 International Topical Meeting on Advanced Reactors Safety; 622 International Workshop on Implementation of ALARA at Nuclear Power Plants; 648 Short Course on Nuclear Criticality Safety; 648 8th Topical Meeting on Problems in Reactor Physics MEPhi-VOLGA-93; 643 The Authors; 646 Reviewers of Nuclear Safety, Vol. 33

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Spent Nuclear Fuel Receipt Rate Analysis within an Integrated Waste Manage-ment System Architecture that Includes Consolidated Interim Storage

A key parameter in analyzing the performance of an integrated waste management system (IWMS) architecture for the disposition of spent nuclear fuel (SNF) is the SNF receipt rate from reactor and other custodian sites. The introduction of one or more federal consolidated interim storage facilities (CISFs) into the IWMS architecture can enable the receipt rate profile as a function of time to be accelerated relative to system architectures without a CISF. The question then arises as to what an optimal SNF receipt rate profile for an IWMS architecture might be in view of practical constraints and desired system performance attributes and associated metrics. This paper describes a sensitivity study on SNF receipt rates and the associated results for a selected set of IWMS scenarios aimed an in-forming near-term planning for interim storage capabilities and transportation assets. Two different strategies are compared, one that fills an initial CISF quickly and then idles the transportation system while a disposal system is prepared, and a second strategy that aims to provide a more continuous use of transportation assets and receipt capabilities at the IWMS while the disposal system is readied for SNF receipt. Cost considerations and other factors such as impact on timing of clearing reactor sites of SNF, efficient use of capital assets, and other metrics, including those which may be important to a CISF host community, are examined. Based on the analysis, an initial approach is presented targeting a continuous receipt strategy while having the flexibility to step up receipt capabilities to a reasonable degree when needed and beneficial within overall system constraints.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Results from the last DD and DT JET campaigns in the framework of the EUROfusion Tokamak Exploitation Work Package activity

JET, the only tokamak capable of operating with deuterium–tritium (D–T) fuel (since TFTR was shutdown in 1999), has provided essential experimental data to support ITER and DEMO design and operation. Within the EUROfusion Tokamak Exploitation Work Package, JET completed its final campaigns (2022–2023), culminating in the third D–T campaign (DTE3). These experiments addressed key challenges in plasma scenarios, exhaust control, and tritium management under reactor-relevant conditions. Significant progress was achieved in demonstrating ITER-like integrated scenarios with impurity seeding, achieving partial divertor detachment and high confinement ($H_{98}(y,2)$ ≈ 0.85) at 3 MA in D–T plasmas. Advanced exhaust regimes such as quasi-continuous exhaust (QCE) and X-point radiator (XPR) were successfully achieved first in D–D and then extended to D–T operation, confirming their relevance for mixed isotope operation. Operational milestones included a new world record of 69 MJ fusion energy in tritium-rich hybrid plasmas and long-pulse H-mode operation up to 60 s, contributing with unique data to the CICLOP database. Physics studies focused on peeling-limited pedestals in support of ITER and improved understanding of edge stability and impurity screening in metallic environments. Extensive usage of the shattered pellet injector (SPI) on JET provided critical information for the design of the ITER disruption mitigation system (DMS). Real-time control systems for D/T ratio control and plasma exhaust were deployed and demonstrated in D–D and D–T, while energetic particle physics investigations unfolded the role of fast ions in turbulence suppression mechanisms. Comprehensive tritium retention studies using gas balance method, post-mortem analysis, and ITER-relevant laser induced desorption spectroscopy (LIDS) diagnostics provided essential input for tritium accountancy strategies. These results are validating the ITER operational concepts, inform DEMO design, and deliver critical experience in nuclear operation and scenario integration.

disruptions↗

DOE OSTI2025

A systematic exploration of the hydrolysis products of the uranium trioxide polymorphs and their optical vibrational spectra

Study of the uranium trioxide (UO 3 )-water system is complex with inconclusive results and limited details in the literature. The UO 3 system is home to at least seven structural polymorphs and an amorphous phase. The proposed hydrolysis products of UO 3 are just as numerous, yet investigations of these alteration products are sporadic and generally antiquated, thus requiring systematic investigations. Recent developments in the understanding of UO 3 phase space, aided by improvements in analytical and computational techniques, necessitate more modern investigations into the uranyl hydroxide family and their naturally occurring mineral counterparts. We present findings from a systematic investigation of the products formed via hydrothermal reactions of common UO 3 polymorphs and discuss how the equatorial coordination of the uranyl/uranyl-like ions within the UO 3 precursors leads to differences in the optical vibrational spectra of the resulting hydrolysis products. The hypo-stochiometric nature of α-UO 2 (OH) 2 allows for the formation of multiple unique uranyl sites and a distortion of the unit cell to a lower symmetry. This study provides, for the first time, an analysis of β-UO 2 (OH) 2 using modern techniques and instrumentation (Raman/infrared spectroscopy and powder x-ray diffraction) and lays a foundation for future time-dependent investigations into the structural dependence of the hydrolysis kinetics of the UO 3 phases. In conclusion, given the prevalence of UO 3 at both ends of the nuclear fuel cycle, an understanding of its behavior with water has applications ranging from nuclear forensics to waste management and environmental transport.

Uranium trioxide↗