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DOE OSTI2017

Advanced Fuel Cycle Cost Basis – 2017 Edition

This report, commissioned by the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), provides a comprehensive set of cost data supporting a cost analysis for the relative economic comparison of options for use in the DOE Nuclear Technology Research and Development (NTRD) Program (previously the Fuel Cycle Research and Development (FCRD) and the Advanced Fuel Cycle Initiative (AFCI)). The report describes the NTRD cost basis development process, reference information on NTRD cost modules, a procedure for estimating fuel cycle costs, economic evaluation guidelines, and a discussion on the integration of cost data into economic computer models. This report contains reference cost data for numerous fuel cycle cost modules (modules A-O) as well as cost modules for a number of reactor types (R modules). The fuel cycle cost modules were developed in the areas of natural uranium mining and milling, thorium mining and milling, conversion, enrichment, depleted uranium disposition, fuel fabrication, interim spent fuel storage, reprocessing, waste conditioning, spent nuclear fuel (SNF) packaging, long-term monitored retrievable storage, managed decay storage, recycled product storage, near surface disposal of low-level waste (LLW), geologic repository and other disposal concepts, and transportation processes for nuclear fuel, LLW, SNF, transuranic, and high-level waste. Since its inception, this report has been periodically updated. The last such internal document was published in August 2015 while the last external edition was published in December of 2009 as INL/EXT-07-12107 and is available on the Web at URL: www.inl.gov/technicalpublications/Documents/4536700.pdf. This current report (Sept 2017) is planned to be reviewed for external release, at which time it will replace the 2009 report as an external publication. This information is used in the ongoing evaluation of nuclear fuel cycles by the NE NTRD program.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2013

Risk-Based Remediation Approach for Cs-137 Contaminated Sediment/Soils at the Savannah River Site (SRS) Lower Three Runs Tail (U) - 13348 - SRNS-RP-2012-00546

Lower Three Runs is a large blackwater stream that runs through the eastern and southern portion of the Savannah River Site. The Lower Three Runs watershed includes two SRS facility areas: P Area (P Reactor) and R Area (R Reactor) that provided effluent discharges to Lower Three Runs. During reactor operations, effluent discharges were well above natural (pre-industrial) or present day stream discharges. The watershed contains a 2,500-acre mainstream impoundment (PAR Pond), several smaller pre-cooler ponds, and a canal system that connects the pre-cooler ponds and discharges surface water to PAR Pond. From the PAR Pond dam, Lower Three Runs flows approximately 36 kilometers braiding through bottom-land/flood-plain forests before it enters the Savannah River. About eight kilometers downstream from the PAR Pond dam, the SRS boundary narrows (termed the Lower Three Runs tail) providing a limited buffer of DOE property for the Lower Three Runs stream and associated flood-plain. Previous screening characterization efforts revealed Cs-137 contamination in the sediment/soils of the flood-plain. As a part of the American Recovery and Reinvestment Act stimulus package, a comprehensive characterization effort was executed on the sediment/soils of the Lower Three Runs tail flood-plain providing a comprehensive look at the contaminant signature of the area. As a follow-up to that characterization, a regulatory decision Core Team, comprised of members of the South Carolina Department of Health and Environmental Control, Environmental Protection Agency - Region IV, and DOE, conducted negotiations on a risk-based approach to address the level of contamination found in the tail flood-plain as an early action that provided a long-term solution to exposure scenarios. For evaluation purposes, the adolescent trespasser was selected as the most likely human receptor for the Lower Three Runs tail portion because of the natural attractiveness of the area for recreational activities (i.e., hunting, fishing, hiking etc.) and access from public property. Exposure of the adolescent trespasser to Cs-137 contaminated sediment/soil at concentrations greater than 23.7 pico curies per gram have been calculated to result in an unacceptable cancer risk (> 1 x 10{sup -4}). Comparing the characterization sampling results conducted in 2009 with the benchmark concentration of 23.7 pCi/g, identified elevated risk levels along three sampling areas in the Lower Three Runs tail portion. On January 5, 2012, it was agreed by the core team that a Removal Action in the Lower Three Runs tail was to be conducted for the identified soil/sediment locations in the three identified areas that exceed the 1 x 10{sup -4} risk (23.7 pCi/g) for the adolescent trespasser receptor. The addition of Land Use Controls following the Removal Action was appropriate to protect human health and the environment. A systematic screening matrix was initiated at the identified hot spots (i.e., sampling points with Cs-137 activities greater than 23.7 pCi/g) to identify the limits of the excavation area. Sediment/soil within the defined removal areas would be excavated to the depth necessary to achieve the cleanup goal and disposed of in a CERCLA Off-Site Rule approved disposal facility. It was agreed that this removal action would adequately reduce the volume of available Cs-137 in the Lower Three Runs tail and consequently residual activities of the Cs-137 would decay over time reducing the amount of Cs-137 available in the tail which would curtail risk. The Land Use Controls consist of installation of an additional seven miles of fencing at major road crossings, utility easements, and at areas that showed a higher probability of access. In addition, signs were placed along the entire SRS perimeter of the Lower Three Runs tail approximately every 200 feet. Sign posts included both a No Trespassing sign and a Contaminant Warning sign. The project initiated a subcontract for both the removal action and the installation of fencing and signs on May 1, 2012. All field activities were completed by July 26, 2012. The project excavated and disposed of over 2700 cubic yards of contaminated sediment/soil, erected approximately seven miles of fence and placed over 2,000 signs demonstrating DOE's commitment to protect human health and act as a good neighbor to residents in the area. (authors)

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

Modeling and Analysis of Coupled Flow Through Packed Beds as a Diagnostic Tool for Packed Bed Reactor Health - 17172

The US Department of Energy, Office of River Protection, is building the Waste Treatment and Immobilization Plant (WTP) in Richland, Washington, to immobilize the hundreds of millions of liters of radioactive waste stored at the Hanford Site in Washington state. The offgas generated during vitrification of these wastes requires treatment to remove and/or destroy chemical and radioactive hazardous components before release to the atmosphere. In particular, volatile and semi-volatile hydrocarbon components are to be catalytically oxidized to carbon dioxide and water, whereas nitrogen oxides (NOx) are to be catalytically reduced to nitrogen and water. These tasks are accomplished in a series of packed bed reactors. Achieving the requisite Destruction/Removal Efficiency (DRE) for each of the tracked components is highly dependent on the flow characteristics of the offgas through the packed beds. The flow kinetics may be monitored and characterized during the initial warm-up of the system. The gases, initially at 76 deg. C (169 deg. F), (a) flow through one side of a countercurrent heat exchanger to recover heat from the exiting gases (which have already passed through the catalytic beds), (b) are then further heated electrically to approximately 400 deg. C (750 deg. F; the preferred operating temperature of the Thermo Catalytic Oxidizer (TCO)), (c) pass through the TCO where the reduced components of the offgas are oxidized over a supported Pt catalyst bed, (d) are partially cooled to approximately 315 deg. C (600 deg. F) by addition of approximately 25% (by weight) diluted ammonia/air mixture, (e) pass through the Selective Catalytic Reducer (SCR) where the NOx components are converted to N{sub 2} and H{sub 2}O over a supported V2O{sub 5}/TiO{sub 2} catalyst bed, and (f) exit through the hot side of the countercurrent heat exchanger. The electrical heater is not powerful enough to raise the temperature of the offgas to the desired 400 deg. C without the contribution of the heat recovered in the heat exchanger. Moreover, the thermal mass of the beds and housings of the TCO and SCR require a significant input of thermal energy to reach the desired operating temperatures; the better part of a day is required to bring the unit from ambient temperatures to operating temperatures. Therefore, the temperature of the stream during the initial warm-up of the system at each point in the system is dependent upon the thermal mass, flow dispersion, and permeability of the components, quantified as characteristic/representative volumes and residence times. By monitoring the temperature of the offgas as it enters and exits each portion of the system during this warm-up period one may model the system as a series of small Continuously Stirred Tank Reactors (CSTR)s (referred to as 'CSTRlets') to explain the flow kinetics through the catalyst beds. These component CSTRlets are adjustable in size and number, that one may model the flow profile of the gases through the catalyst beds. For example, a single large CSTR will present an effluent temperature profile with a simple exponential decay shape. Concatenating more CSTRlets generate more complex sigmoidal responses. Concatenating one CSTRlet significantly larger than the others in the train also alters the shape of the effluent temperature profile, in a fashion not replicable by a train of equal-sized CSTRlets. The ultimate goal is to accurately emulate the entire system as a representative CSTRlet train. Once accomplished, this characterization may be used in subsequent warm-ups (following shutdown for catalyst maintenance, for example) or by an intentional step change in inlet offgas temperature to detect/diagnose anomalies in flow through the beds (e.g., channeling or partial blockage.) This work presents development of this model through analytical, calculational, and empirical means. - The analytic model is accomplished by Laplace transform analysis of each component to recover component process transfer functions. - The calculational portion is performed via brute force finite element calculation. - Fitting empirical data from the warm-up of the TCO skid allows one to select the hypothetical CSTRlet trains which best fit the TCO and SCR beds for the analytical and finite element calculations. The first portion of this paper presents the development of the analytical (Laplace space) model of the coupled system. Estimated values for the initial temperature, mass, specific heat, electrical heat, and relative quantities of the offgas, catalyst beds, stainless steel housings, and ammonia dilution stream are used to generate expected temperature profiles at several selected junctures of the system. The number and size of the component hypothetical CSTRlets are calculated from the analytical model and are used to predict temperature profiles at the exit of the system and at intermediate junctions between system components (where thermocouples are present in the actual unit.) The finite element calculations employ a series of CSTRlet volumes to produce a similar suite of temperature profiles, for comparison with the analytical model results. Finally, empirical data from the Factory Acceptance Test system warm-up are used to select and compare the results from each modeling strategy to select the CSTRlet train(s) which best model the behavior of the actual system. This work presents a novel method of system component characterization, of value to the WTP plant and similar vitrification facilities as well as chemical process industries unrelated to waste management. (authors)

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DOE OSTI2016

PGSFR General Arrangement

The Nuclear Island of the PGSFR is constructed upon the seismic isolation structure bearing a common basemat of the Reactor Building and the Auxiliary Building. The Reactor Building is divided into two different functional structures: 1) containment structure comprised of a operating floor, head access area (HAA), annulus area and etc., 2) the other areas accessible to reactor vault area outside of the containment structure via the Auxiliary Building. The arrangement of the Auxiliary Building is composed of symmetric divisional areas where there are two steam generators, heat exchangers of the Decay Heat Removal System (DHRS), facilities of the Intermediate Sodium Purification System (ISPS), the Primary Inert Gas Processing System (PIGPS), a main control room (MCR), electric equipment rooms, and main steam valve houses (MSVH), and etc. The general arrangement of the Reactor Building and the Auxiliary Building of the PGSFR is currently in development. Not only NSSS but supporting systems have not been finalized yet. Moreover, the other facility buildings such as a Turbine Generator Building, a fuel cycle facility, radwaste treatment facilities, and etc. have to be designed with relevant interfaces to the Reactor Building and the Auxiliary Building. We can expect additional modifications to optimize the general arrangement. However, the basic principles such as sodium and non-sodium segregation, convenient accessibility and maintenance, economics of architectural volume would be kept in the design. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2023

Second Report of the Nuclear Data Subcommittee of the Nuclear Science Advisory Committee

The central importance of the nuclear data curated by the US Nuclear Data Program (USNDP) for clean energy generation, national security, nonproliferation, medical applications, and space exploration as well as basic science was described in a prior report issued by the DOE/NSF Nuclear Science Advisory Committee subcommittee on Nuclear Data (NSAC-ND) in September 2022. In this report, we present a set of fourteen (14) recommendations that will enhance and advance DOE-NP's stewardship of nuclear data. The first three recommendations focus on the existing core USNDP capabilities, namely: 1) Support the nuclear structure evaluation workforce to improve the currency, consistency, and accessibility of the Evaluated Nuclear Structure Data File (ENSDF); 2) Enhance nuclear reaction evaluation within the USNDP in support of the Evaluated Nuclear Data File (ENDF) through expansion of the workforce and integration of high-performance computing, automation, and machine learning and; 3) Continue atomic mass evaluation in support AME and NUBASE databases. This is followed by eight (8) recommendations representing new cross-cutting initiatives involving both measurement and evaluation to address outstanding nuclear data needs. These new initiatives require a highly trained, diverse workforce that includes personnel with expertise from both inside and outside the nuclear physics community from which evaluators have traditionally been recruited. As such, many of these initiatives are accomplished via a Topical Nuclear Data Collaborations (TNDC). A TNDC is made up of domestic and international stakeholders, subject matter and nuclear data experts, and nuclear data evaluators and features a workforce development plan to ensure that nuclear data evaluators maintain currency in the relevant applications and are seen as equity partners in the endeavor. These include: 1) Establish a coordinated effort to improve evaluation and modeling in nuclear astrophysics for stellar dynamics, multi-messenger astronomy and nucleosynthesis; 2) Initiate a TNDC to develop and maintain nuclear structure evaluation beyond discrete states, including nuclear level densities, photon strength functions and photonuclear data for improved reaction modeling, and exploring nuclear structure at finite temperature; 3) Create a TNDC to perform correlated fission data evaluation, including cross sections, fragment yields, v(A), v(E n ) for nuclear energy, national security, nonproliferation and basic science; 4) From a panel of subject matter experts to establish and annually update a roster of key decay data to nurture its accelerated dissemination including both measurement and evaluation for targeted high-value nuclides for national security, nonproliferation and medical applications; 5) Comprehensive, consistent neutron-induced structure and reaction data for nuclear energy, national security, nonproliferation and planetary nuclear spectroscopy; 6) Charged-particle stopping powers for detector design, space effects and ion beam therapy; 7) High-energy reactions for space exploration and medical nuclide production, and; 8) The creation of an infrastructure for open data and data preservation for use by the entire nuclear physics community. All told, these initiatives require approximately $6.5M increase in NP support of the USNDP in fiscal year 2023 dollars and would require at least 3-5 years to carry out due to the length of time needed to recruit and train new nuclear data researchers. This relatively modest investment would help ensure that the fruits of the nuclear data research carried out by DOE-NP and its collaborators would be brought to bear to address some of the most important needs of our nation and the world. To ensure effective execution of this plan, we present an overview of recruitment, training, and retention goals for the USNDP, the centerpiece of which is a mutually agreed upon code of conduct. Finally, we identify the facility and instrumentation needed to perform the recommended experimental activities. This includes a short review of target fabrication capabilities, reactors, neutron beam, light- and heavy-stable ion, gamma-ray, high-energy and radioactive ion beam facilities. Lastly, a more complete appendix of experimental facilities previously compiled is included with new input provided for 6 facilities.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Induction Heating for Tritium Storage Beds

Metal hydride beds used for storing hydrogen isotopes accumulate helium due to beta-decay of tritium. Helium alters the hydrogen capacity and plateau pressures of these storage beds and ultimately results in the beds being disqualified for use in tritium facilities. Removal of helium and hydrogen isotopes for disposal or storage bed regeneration can be achieved with sufficient heating; however, existing Gen 1 and Gen 2 storage beds are not designed to reach helium removal temperatures and face disposal challenges. In this report, we describe experiments and Multiphysics models that were used to develop a method to achieve induction heating of existing tritium storage beds using induction coils placed on the outside of the beds. The heating method involves low-frequency (< 100 Hz) induction heating through flexible solenoid coils that wrap tightly around the outer jacket of a tritium storage bed. This method of heating offers a pragmatic path to heat existing storage beds for metal hydride regeneration, helium removal for disposal, and possibly routine gas cycling operations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Engineering Scale Drying of Aluminum-Clad Spent Nuclear Fuel: Experiment Report

Engineering-scale tests were performed to evaluate the relative effectiveness of forced gas and vacuum-drying processes on aluminum-clad spent nuclear fuel (ASNF) in preparation for extended dry storage. Drying models were developed to improve confidence in the likely range of conditions at the start of dry storage and to understand the factors most significant to each process. Testing was performed at the Holtec International Forced Helium Dehydration training facility in Camden, New Jersey, by students from the University of South Carolina in collaboration with Idaho National Laboratory. A full-size Type 1a basket, with a full-diameter vessel configuration (based on the Department of Energy standardized canister design), was used in combination with a 10 assembly surrogate ASNF arrangement to provide a proxy for geometry. A resistance heater incorporated in one assembly simulated the influence of 100 W decay heat. This instrumented chamber allowed testing of the removal of bulk water, physisorbed water, and chemisorbed water over a range of operating parameters with either drying process. Thick oxide films were grown on aluminum test plates to mimic the ASNF surface chemistry. These one-use test plates were housed within select assemblies during drying. Post-test analysis of these plates gave a measure of the moisture removed during each test, which was compared to a control. Instrumentation provided detailed thermal, humidity, and gas or pressure data relevant to each test. Model simulations generally compared favorably to instrument data for the tests. While both processes were able to remove bulk water, removal of chemisorbed water was shown to depend heavily on local temperature. To the disadvantage of vacuum drying, operations approaching or exceeding 220°C achieved consistently more dehydroxylation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Decontamination and Melting of Reactor Upper Internals - 18536

In a BWR, the upper reactor internals, i.e. the steam separators and the steam dryer converts the hot water to a dry steam for the turbines. These components have due to the distance to the reactor core low to very low levels of neutron activation, if any. The contamination of these components is usually significant and consists of both loose contamination and contamination bound in oxide layers. The upper reactor internals on a BWR are quite voluminous in relation to their weight, has a complex geometry and are therefore time consuming to cut in pieces that allows high density packing in waste containers for ILW. The incentives for decontamination of the components down to levels that allow melting for volume reduction are therefore high. A performed full-scale treatment project on a steam dryer confirms the significant volume reduction. The steam dryer was decayed prior to segmentation and melting for volume reduction. Cyclife/EDF has, since significant volume reduction is within reach if the inventory of gamma emitting nuclides and by then the dose rate can be reduced, taken benefit of chemical decontamination studies and an analyze of potential treatment results. The analyze confirm that high decontamination factors can be achieved and that the acceptance criteria for melting can be met, with margin. Full scale decontamination results achieved by AREVA NP and others do align fairly well with the test results. Even without the option of clearance/recycling of the metals, due to high residual activity, a high or very high volume reduction factors can be achieved by melting as well as a potential reclassification of the metal in a disposal perspective. One key aspect for success is to keep the volume of the secondary waste from the decontamination down and to make sure that the waste form fulfils the requirements for disposal. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS2011

U.S. Space Radioisotope Power Systems and Applications: Past, Present and Future

Radioisotope power systems (RPS) have been essential to the U.S. exploration of outer space. RPS have two primary uses: electrical power and thermal power. To provide electrical power, the RPS uses the heat produced by the natural decay of a radioisotope (e.g., plutonium-238 in U.S. RPS) to drive a converter (e.g., thermoelectric elements or Stirling linear alternator). As a thermal power source the heat is conducted to whatever component on the spacecraft needs to be kept warm; this heat can be produced by a radioisotope heater unit (RHU) or by using the excess heat of a radioisotope thermoelectric generator (RTG). As of 2010, the U.S. has launched 41 RTGs on 26 space systems. These space systems have ranged from navigational satellites to challenging outer planet missions such as Pioneer 10/11, Voyager 1/2, Galileo, Ulysses, Cassini and the New Horizons mission to Pluto. In the fall of 2011, NASA plans to launch the Mars Science Laboratory (MSL) that will employ the new Multi-Mission Radioisotope Thermoelectric Generator (MMRTG) as the principal power source. Hundreds of radioisotope heater units (RHUs) have been launched to provide warmth to Apollo 11, used to provide heating of critical components in a seismic experiment package, Pioneer 10/11, Voyager 1/2, Galileo, Cassini, Mars Pathfinder, MER rovers, etc. to provide temperature control to critical spacecraft electronics and other mechanical devices such as propulsion system propellant valves. A radioisotope (electrical) power source or system (RPS) consists of three basic elements: (1) the radioisotope heat source that provides the thermal power, (2) the converter that transforms the thermal power into electrical power and (3) the heat rejection radiator. Figure 1 illustrates the basic features of an RPS. The idea of a radioisotope power source follows closely after the early investigations of radioactivity by researchers such as Henri Becquerel (1852-1908), Marie Curie (1867-1935), Pierre Curie (1859-1906) and R. J. Strut. Almost 100 years ago, in 1913, English physicist H. G. J. Moseley (1887-1915) constructed the first nuclear battery using a vacuum flask and 20 mCi of radium (Corliss and Harvey, 1964, Proceedings of the Royal Society, 1913). After World War II, serious interest in radioisotope power systems in the U.S. was sparked by studies of space satellites such as North American Aviation s 1947 report on nuclear space power and the RAND Corporation s 1949 report on radioisotope power. (Greenfield, 1947, Gendler and Kock, 1949). Radioisotopes were also considered in early studies of nuclear-powered aircraft (Corliss and Harvey, 1964). In 1951, the U.S. Atomic Energy Commission (AEC) signed several contracts to study a 1-kWe space power plant using reactors or radioisotopes. Several of these studies, which were completed in 1952, recommended the use of RPS. (Corliss and Harvey, 1964). In 1954, the RAND Corporation issued the summary report of the Project Feedback military satellite study in which radioisotope power was considered (Lipp and Salter, 1954, RAND). Paralleling these studies, in 1954, K. C. Jordan and J. H. Birden of the AEC s Mound Laboratory conceived and built the first RTG using chromel-constantan thermocouples and a polonium-210 (210Po or Po-210) radioisotope heat source (see Figure 2). While the power produced (1.8 mWe) was low by today s standards, this first RTG showed the feasibility of RPS. A second thermal battery was built with more Po-210, producing 9.4 mWe. Jordan and Birden concluded that the Po-210 thermal battery would have about ten times the energy of ordinary dry cells of the same mass (Jordan and Birden, 1954). The heat source consisted of a 1-cm-diameter sphere of 57 Ci (1.8 Wt) of Po-210 inside a capsule of nickel-coated cold-rolled steel all inside a container of Lucite. The thermocouples were silver-soldered chromel-constantan. The thermal battery produced 1.8 mWe.

Cataldo, Robert L.↗
DOE OSTI2024

DECOVALEX-2023: Task F1 Final Report

DECOVALEX-2023 Task F is a comparison of models and methods for post-closure performance assessment (PA) of a deep geologic repository for radioactive waste. The general aims of Task F are to build confidence in the models, methods, and software used for PA and to stimulate additional research and development in PA methodologies. The task objectives are to motivate development of PA modelling skills and capabilities, to examine the influence of model choices on calculated repository performance, and to compare the uncertainties introduced by model choices to other sources of uncertainty. Task F involves no actual experiment or site. It is a PA modelling exercise that requires the conceptual development of hypothetical repository designs and geologic settings. Because three of the teams were interested in salt and the rest of the teams were interested in crystalline rock, Task F was split into two branches: Task F1 for crystalline rock and Task F2 for salt. This report is for Task F1, crystalline rock. Teams from seven countries (Canada, Czech Republic, Germany, Korea, Sweden, Taiwan, and United States) participated in Task F1. The teams worked together to define the features, events, and processes of the reference case repository and established a set of performance measures. In addition, they defined a set of benchmark problems designed to test and compare modelling capabilities for fracture flow and transport at different scales. The repository design and benchmark problems are documented in a Task Specification that evolved over time as the group honed the specifications. The benchmark problems verified that each team can aptly model flow and transport in fractured media in 1-, 2-, and 3-dimensions. Two general approaches were used for the 3-dimensional benchmarks: discrete fracture network (DFN) and equivalent continuous porous medium (ECPM). DFN modelling involves explicit meshing of each fracture while ECPM modelling aims to capture the effective porosity and directional permeability of each cell in a space-filling mesh as affected by intersecting fractures. In some models, a combination of the two is used, i.e., DFN for large known fractures and ECPM for the rest of the domain. Transport is solved by using either the advection-dispersion equation or particle tracking. Although some variation is observed among model breakthrough curves in the benchmark problems, there is strong agreement in breakthrough behaviour up to at least the 75 th percentile for all benchmarks. At the 90 th percentile, breakthrough results show larger differences, suggesting several models retain substantially higher fractions of tracer in regions of slower moving water. In addition to the flow and transport benchmarks, several teams completed the source term benchmark, verifying capabilities for modelling radionuclide decay and ingrowth, waste package breach, instant release fractions, fuel matrix degradation rates, and radionuclide solubility limitations. The reference case is conceptualized as a generic spent fuel repository at a depth of 450 m in fractured crystalline rock. The repository has 50 parallel backfilled drifts, each with 50 deposition holes 6 m apart. Each deposition hole contains a 4-PWR waste package and bentonite buffer. The rock domain is 5 km in length, 2 km in width, and 1 km in depth. It has 6 deterministic fractured deformation zones and a multitude of stochastic fractures. Teams generally used the ECPM approach for the entire rock or a hybrid approach in which the deterministic fracture zones are modelled with a DFN and the rest of the rock is modelled by ECPM. Of the reference case problems specified, only the results of the initial reference case problem are compared in this report. The initial problem focuses on transport from the deposition holes to the surface, i.e., it neglects waste package performance. Tracers are released at all waste package locations at time zero and tracked for their releases to the near field and ground surface. The water fluxes calculated at the ground surface entry and exit regions of the domain are similar for all models except for two that have considerably lower fluxes. For tracer transport, large differences are observed among models in the magnitude of tracer transported. Much of the difference appears to be due to how the repository is implemented and hence the different degrees of repository simplification. Models that exclude the drifts, buffer, and backfill from the domain tend to show greater release of tracers and radionuclides from the repository. The initial study presented here indicates that major differences in modelling important processes within the repository (e.g., diffusion through buffer and backfill) can produce broadly different release and transport results, especially when those processes are excluded. Even for the models that included all specified features, events, and processes, the results show significant differences and demonstrate the importance of examining multiple modelling approaches in performance assessment. The differences in results observed in this study are expected to motivate teams to either increase complexity in future versions of the reference case models or to improve methods to account for the effects of simplified features and processes. Either way, future improvements in these models are expected to produce results that more closely agree.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Invariant-mass spectroscopy of Ne 18 , O 16 , and C 10 excited states formed in neutron-transfer reactions

Neutron-transfer reactions with fast secondary beams of 17 Ne, 15 O, and 9 C have been studied with the HiRA and CAESAR arrays. Excited states of 18 Ne, 16 O, and 10 C in the continuum have been identified using invariant-mass spectroscopy. The best experimental resolution of these states is achieved by selecting events where the decay fragments are emitted transverse to the beam direction. We have confirmed a number of spin assignments made in previous works for the negative-parity states of 18 Ne. In addition we have found new higher-lying excited states in 16 O and 18 Ne, some of which fission into two ground-state 8 Be fragments. Finally for 10 C, a new excited state was observed. Furthermore, these transfer reactions were found to leave the remnant of the 9 Be target nuclei at very high excitation energies and may be associated with the pickup of a deeply bound 9 Be neutron.

6 ≤ A ≤ 19↗
DOE OSTI2024

Oxygen Limit for Flammability of a Gas Mixture of Helium – Hydrogen – Oxygen in the U.S. Department of Energy Standard Canister

The radiolytic breakdown of residual free, physisorbed, and chemisorbed waters is anticipated in the sealed dry storage of spent nuclear fuel (SNF), releasing H 2 gas into the initial cover gas of helium. For aluminum-clad SNF (ASNF) in particular, the expected total hydrogen in the canister is enough to dominate the cover gas mixture if fully released, and based on experimental rates of H 2 generation, H 2 percentages exceeding the lower flammability limit appear likely. However, no evidence of radiolytic generation of O 2 has been observed to date, so the potential for flammability is averted due to the lack O 2 . Lack of oxygen has been credited for avoiding flammability in some existing storage and transportation approaches for SNF and other waste. This report reviews literature on flammability limits with a focus on the limiting oxygen concentration to provide technical underpinnings to refine a flammability criterion for gas mixtures of helium, hydrogen, and oxygen where the oxygen is expected to be the limiting species. While there is general consensus on H 2 flammability limits at standard temperature and pressure, the decay heat and gas generation within ASNF sealed dry storage canisters could push them to elevated temperatures and pressures, so the goal is to identify an oxygen threshold that will bound the behavior over the temperature and pressure range of the U.S. Department of Energy (DOE) Standard Canister. The information reviewed in this document supports the criterion that the oxygen concentration in a He-H 2 -O 2 mixture should be less than 1.5% to avoid flammability at temperatures and pressures relevant to sealed dry storage of ASNF in the DOE Standard Canister, i.e., up to 343°C (650°F) and 500 psig, respectively. Note that while data covering the full range of temperature at atmospheric pressure and nearly the full range of pressure at room temperature were available, data for the combined effects was available only at moderate temperatures and pressures; the recommended 1.5% O 2 threshold is based on the breadth of available data reported here and apparent trends therein.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Simulation of radon-222 with the GEOS-Chem global model: Emissions, seasonality, and convective transport

Radon-222 (222Rn) is a short-lived radioactive gas naturally emitted from land surface, and has long been used to assess convective transport in atmospheric models. In this study, we simulate 222Rn using the GEOS-Chem chemical transport model with aims to improve our understanding of 222Rn emissions and surface concentration seasonality, and to characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, MERRA and GEOS-FP. We evaluate four available 222Rn emission scenarios by comparing model results with surface observations at 51 global surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with global surface observations (< 70% data within a factor of 2) and a large underestimate of wintertime surface 222Rn concentrations at Northern Hemisphere mid- and high-latitudes due to an oversimplified formulation of 222Rn emission fluxes (1 atom cm-2 s-1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global 222Rn emission scenario based on Zhang et al. (2011) and show its potential to improve simulated surface 222Rn concentrations and seasonality. The regional components of this emission scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors to 222Rn emission flux rates. However, large model underestimates of surface 222Rn concentrations still exist in Asia, suggesting unusually high regional 222Rn emissions. We propose a conservative up-scaling factor of 1.2 for 222Rn emission fluxes in China, as also constrained by the observed deposition fluxes of 210Pb (decay daughter of 222Rn). With this modification, the model shows better agreement with the observations in Europe and North America (>80% data within a factor of 2), and reasonable agreement in Asia (close to 70%). Further constraints on 222Rn emissions would require additional observations of surface 222Rn concentrations and emission fluxes in central U.S., Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed 222Rn vertical profiles during northern mid-latitude summertime and from two short-term airborne campaigns. While the simulations with both GEOS products are able to capture the observed vertical gradient of 222Rn concentrations in the lower troposphere (0-4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared to GEOS-FP, MERRA leads to stronger convective transport of 222Rn, which is partially compensated by its weaker large-scale vertical advection, resulting in similar global vertical distributions of 222Rn concentrations between the two simulations.

Zhang, Bo↗
DOE OSTI2015

The nonlinear light output of NaI(Tl) detectors in the Modular Total Absorption Spectrometer

New detector array, the Modular Total Absorption Spectrometer (MTAS),was commissioned at the Holifield Radioactive Ion Beam Facility (HRIBF) at Oak Ridge National Lab(ORNL).Total absorption gamma spectra measured with MTAS are expected to improve beta-feeding patterns and beta strength functions in fission products.MTAS is constructed out of hexagonal NaI(Tl) detectors with a unique central module surrounded by 18 identical crystals assembled in three rings. The total NaI(Tl) mass of MTAS is over1000 kg.The response of the central and other 18 MTAS modules to -radiation was simulated using the GEANT4 tool kit modified to analyze the nonlinear light output of NaI(Tl).A detailed description oftheGEANT4modifications madeisdiscussed.SimulatedenergyresolutionofMTAS modules is found to agree well with the measurements for single transitions of 662keV (137Cs) with 8.2% full width half maximum (FWHM),835keV (54Mn) with FWHM of 7.5% FWHM, and 1115keV (65Zn) with FWHM of 6.5%.Simulations of single and multiple -rays from 60Co are also discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Electrochemical hydrogen isotope fractionation - fundamental insights leading to process scale up

Introduction Deuterium and tritium, the two isotopes of hydrogen besides protium, are utilized in many industries. Deuterium is routinely used as a nuclear reactor moderator and molecular labeling agent, while tritium is used as an autoradiography label in medical imaging, and in an emerging market for self-powered lighting for watches, exit signs, firearm night-sights and future fusion fuel. Tritium is produced naturally at very low steady-state levels due to cosmic rays, natural nuclear decay reactions, as well as commercial nuclear fission reactors, and terrestrial nuclear testing conducted primarily in the mid-twentieth century. Tritium often accumulates in the heavy water used in nuclear fission reactors and sometimes appears in groundwater near nuclear reactors due to slight leakage from water sources in the reactor. Because of the health and environmental impacts from tritium leaking into the water sources, as well as the value of this precious material, it is desirable to remove and recover as much tritium as reasonably possible from contaminated water.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

The Recovery of Medical Isotope 188 W from Irradiated W Metal Target - A New Approach

Tungsten-188 is in widespread use in 188 W(t 1/2 = 69 d )/ 188 Re(t 1/2 = 16.9 h ) biomedical generators. Oak Ridge National Laboratory has been providing this product to the world since 1999. At ORNL, 188 W is produced via irradiation in ORNL’s High Flux Isotope Reactor (HFIR). Enriched 186 W targets in the form of sintered metallic pellets or rings achieve a compact loading in the irradiation vessel, providing a high yield per unit target. The enrichment of the target is >90% 186 W, and this isotope undergoes double neutron capture to produce the desired 188 W product. While 188 W is produced by neutron bombardment, 191 Os(t 1/2 = 15.4 d ) is simultaneously produced as a by-product and expected to be separated from 188 W by postirradiation treatment.In the current processing pathway, the irradiated W metal rings are first converted into an oxide form of WO 3 by heating the irradiated W metal target at 750°C in a quartz reaction vessel inside a vertical furnace under a constant flow of air. During heating, W metal reacts with oxygen in the air to produce WO 3 , which is soluble in 6 M NaOH for preparation of 188 W product. This oxidation process also converts 188 Os (the decay daughter of 188 W) and 191 Os (15.4 d , the irradiation produced byproduct) into OsO 4 , a highly volatile and toxic gas. The gaseous effluents driven from the quartz reaction vessel are passed through a scrubbing array to remove OsO 4 before the air is discharged from the process. This heterogeneous oxidation method simultaneously achieves goals of (1) converting metal target to a soluble oxide form and (2) removing volatile OsO 4 away from the solid WO 3 product by air flow and absorbing the harmful Os species by the scrubbing array. But this method has two potential problems as well: (1) O 2 reacts with only W metal at high temperatures, not with W alloyed with other elements. The O 2 –W reaction will be retarded when formation of WRe or WC occurs, or even when a layer of non-W materials on the surface of the irradiated W rings.; (2) 100% absorption of OsO 4 of high yield (>90%) from the reaction of Os + O 2 is a strict requirement to the OsO 4 scrubbing system--so NaOH scrubbers of a redundant size (2x 1.5 L) are in use for safety reasons.To resolve above two potential problems, direct dissolution of the irradiated W metal target by a selected reagent is a preferred pathway to avoid heating step with generation of tremendous amount of volatile OsO 4 . Hydrogen peroxide (H 2 O 2 ) is such a candidate to dissolve W in forms of either metal or alloys, although literature lacks information of solubilities of Re or Os in H 2 O 2 . With experimental results of dissolving non-radioactive W, Re and Os in H 2 O 2 under various conditions, this report illustrates a method of H 2 O 2 dissolution for irradiated W target, with a complete dissolution of W and Re, but ≤10% dissolution of Os (converted into gaseous OsO 4 and carried out into a scrubbing for absorption) during processing irradiated W target. The portion of undissolved Os can be separated from W solution by a follow up filtration step. Solubilities of W, Re and Os in H 2 O 2 at a temperature range from 14° to 50°C are presented. And a dissolution rate of W metal per surface area of W metal in H 2 O 2 is calculated based on results of dissolving a W metal cylinder of known surface area in H 2 O 2 at room temperature without stirring.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2013

Measurement and Analysis of Gamma-Rays Emitted From Spent Nuclear Fuel Above 3 MeV

The gamma-ray spectrum of spent nuclear fuel in the 3- to 6-MeV energy range is important for active interrogation since emitted gamma rays emitted from nuclear decay are not expected to interfere with measurements in this energy region. There is, unfortunately, a dearth of empirical measurements from spent nuclear fuel in this region. This work is an initial attempt to partially ll this gap by presenting an analysis of gamma-ray spectra collected from a set of spent nuclear fuel sources using a high-purity germanium detector array. This multi-crystal array possesses a large collection volume, providing high energy resolution up to 16 MeV. The results of these measurements establish the continuum count-rate in the energy region between 3- and 6-MeV. Also assessed is the potential for peaks from passive emissions to interfere with peak measurements resulting from active interrogation delayed emissions. As one of the first documented empirical measurements of passive emissions from spent fuel for energies above 3 MeV, this work provides a foundation for active interrogation model validation and detector development.

delayed gamma rays↗
DOE OSTI2018

Rock-welding materials development for deep borehole nuclear waste disposal

We report that various versions of deep borehole nuclear waste disposal have been proposed in the past in which effective sealing of a borehole after waste emplacement is generally required. In a high temperature disposal mode, the sealing function will be fulfilled by melting the ambient granitic rock with waste decay heat or an external heating source, creating a melt that will encapsulate waste containers or plug a portion of the borehole above a stack of the containers. However, there are certain drawbacks associated with natural materials, such as high melting temperatures, inefficient consolidation, slow crystallization kinetics, the resulting sealing materials generally being porous with low mechanical strength, insufficient adhesion to waste container surface, and lack of flexibility for engineering controls. In this study, we showed that natural granitic materials can be purposefully engineered through chemical modifications to enhance the sealing capability of the materials for deep borehole disposal. The present work systematically explores the effect of chemical modification and crystallinity (amorphous vs. crystalline) on the melting and crystallization processes of a granitic rock system. The approach can be applied to modify granites excavated from different geological sites. Several engineered granitic materials have been explored which possess significantly lower processing and densification temperatures than natural granites. Finally, those new materials consolidate more efficiently by viscous flow and accelerated recrystallization without compromising their mechanical integrity and properties.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗