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Why natural monazite never becomes amorphous: Experimental evidence for alpha self-healing

Monazite, a common accessory rare-earth orthophosphate mineral in the continental crust widely used in U-Pb geochronology, holds promise for (U-Th)/He thermochronology and for the immobilization of Pu and minor actinides (MA) coming from spent nuclear fuel reprocessing. Previous results obtained on natural and plutonium-doped monazite have demonstrated the ability of this structure to maintain a crystalline state despite high radiation damage levels. However, the low critical temperature (180 °C), above which amorphization cannot be achieved in natural monazite under ion irradiation, does not explain this old and unsolved paradox: why do natural monazites, independent of their geological history, remain crystalline even when they did not experience any thermal event that could heal the defects? This is what the present study aims to address. Synthetic polycrystals of LaPO 4 -monazite were irradiated sequentially and simultaneously with α particles (He) and gold (Au) ions. Here, our results demonstrate experimentally for the first time in monazite, the existence of the defect recovery mechanism, called α-healing, acting in this structure due to electronic energy loss of α particles, which explains the absence of amorphization in natural monazite samples. This mechanism is critically important for monazite geo- and thermochronology and to design and predictively model the long-term behavior of ceramic matrices for nuclear waste conditioning.

36 MATERIALS SCIENCE↗

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↗

Seismic Performance of Dry Casks Storage for Long- Term Exposure

The main goal of this study is to evaluate the long-term seismic performance of freestanding and anchored Dry Storage Casks (DSCs) using experimental tests on a shaking table, as well as comprehensive numerical evaluations that include the cask-pad-soil system. The study focuses on the dynamic performance of vertical DSCs, which can be designed as free-standing structures resting on a reinforced concrete foundation pad, or casks anchored to a foundation pad. The spent nuclear fuel (SNF) at nuclear power plants (NPPs) is initially stored in fuel-storage pools to control the fuel temperature. After several years, the fuel assemblies are transferred to DSCs at sites contiguous to the plant, known as Interim Spent Fuel Storage Installations (ISFSIs). The regulations for these storage systems (10 CFR 72) ensure adequate passive heat removal and radiation shielding during normal operations, off-normal events, and accident scenarios. The integrity of the DSCs is important, even if the overpack does not breach, because eventually the spent fuel-rods need to be shipped either to a reprocessing plant or a repository. DSCs have been considered as a temporary storage solution, and usually are licensed for 20 years, although they can be relicensed for operating periods of up to 60 years. In recent years, DSCs have been reevaluated as a potential mid-term solution, in which the operating period may be extended for up to 300 years. At the same time, recent seismic events have underlined the significant risks DSCs are exposed. The consideration of DCSs for storing spent fuel for hundreds of years has created new challenges. In the case of seismic hazard, longer-term operating periods not only lead to larger horizontal accelerations, but also increase the relative effect of vertical accelerations that usually are disregarded for smaller seismic events. These larger seismic demands could lead to casks sliding and tipping over, impacting the concrete pad or adjacent casks. The casks may also slide and collide with other casks or structural components. Also, the different DSC components may impact each other during these events. This study provides a comprehensive evaluation of DSCs subjected to these extreme demands, including the effect of vertical accelerations, and soilstructure interaction.

36 MATERIALS SCIENCE↗

Improvement of INVS Measurement Uncertainty for Pu and U-Pu Nitrate Solution

In the Tokai Reprocessing Plant (TRP) and the Plutonium Conversion Development Facility (PCDF), a large amount of plutonium nitrate solution which is recovered from light water reactor (LWR) and advanced thermal reactor (ATR), FUGEN are being stored. Since the solution is designated as a direct use material, the periodical inventory verification and flow verification are being conducted by Japan Safeguard Government Office (JSGO) and International Atomic Agency (IAEA).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Performance of a Steel/Oxide Composite Waste Form for Combined Waste Steams from Advanced Electrochemical Processes

The results of electrochemical corrosion tests and modeling activities performed collaboratively by researchers at the University of Illinois at Chicago and Argonne National Laboratory as part of workpackage NU-13-IL-UIC-0203-02 are summarized herein. The overall objective of the project was to develop and demonstrate testing and modeling approaches that could be used to evaluate the use of composite alloy/ceramic materials as high-level durable waste forms. Several prototypical composite waste form materials were made from stainless steels representing fuel cladding, reagent metals representing metallic fuel waste streams, and reagent oxides representing oxide fuel waste streams to study the microstructures and corrosion behaviors of the oxide and alloy phases. Microelectrodes fabricated from small specimens of the composite materials were used in a series of electrochemical tests to assess the corrosion behaviors of the constituent phases and phase boundaries in an aggressive acid brine solution at various imposed surface potentials. The microstructures were characterized in detail before and after the electrochemical tests to relate the electrochemical responses to changes in both the electrode surface and the solution composition. The results of microscopic, electrochemical, and solution analyses were used to develop equivalent circuit and physical models representing the measured corrosion behaviors of the different materials pertinent to long-term corrosion behavior. This report provides details regarding (1) the production of the composite materials, (2) the protocol for the electrochemical measurements and interpretations of the responses of multi-phase alloy and oxide composites, (3) relating corrosion behaviors to microstructures of multi-phase alloys based on 316L stainless steel and HT9 (410 stainless steel was used as a substitute) with added Mo, Ni, and/or Mn, and (4) modeling the corrosion behaviors and rates of several alloy/oxide composite materials made with added lanthanide and uranium oxides. These analyses show the corrosion behaviors of the alloy/ceramic composite materials are very similar to the corrosion behaviors of multi-phase alloy waste forms, and that the presence of oxide inclusions does not impact the corrosion behaviors of the alloy phases. Mixing with metallic waste streams is beneficial to lanthanide and uranium oxides in that they react with Zr in the fuel waste to form highly durable zirconates. The measured corrosion behaviors suggest properly formulated composite materials would be suitable waste forms for combined metallic and oxide waste streams generated during electrometallurgical reprocessing of spent nuclear fuel. Electrochemical methods are suitable for evaluating the durability and modeling long-term behavior of composite waste forms: the degradation model developed for metallic waste forms can be applied to the alloy phases formed in the composite and an affinity-based mineral dissolution model can be applied to the ceramic phases.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

FY-2016 Methyl Iodide Higher NOx Adsorption Test Report

Deep-bed methyl iodide adsorption testing has continued in Fiscal Year 2016 under the Department of Energy (DOE) Fuel Cycle Technology (FCT) Program Offgas Sigma Team to further research and advance the technical maturity of solid sorbents for capturing iodine-129 in off-gas streams during used nuclear fuel reprocessing. Adsorption testing with higher levels of NO (approximately 3,300 ppm) and NO2 (up to about 10,000 ppm) indicate that high efficiency iodine capture by silver aerogel remains possible. Maximum iodine decontamination factors (DFs, or the ratio of iodine flowrate in the sorbent bed inlet gas compared to the iodine flowrate in the outlet gas) exceeded 3,000 until bed breakthrough rapidly decreased the DF levels to as low as about 2, when the adsorption capability was near depletion. After breakthrough, nearly all of the uncaptured iodine that remains in the bed outlet gas stream is no longer in the form of the original methyl iodide. The methyl iodide molecules are cleaved in the sorbent bed, even after iodine adsorption is no longer efficient, so that uncaptured iodine is in the form of iodine species soluble in caustic scrubber solutions, and detected and reported here as diatomic I2. The mass transfer zone depths were estimated at 8 inches, somewhat deeper than the 2-5 inch range estimated for both silver aerogels and silver zeolites in prior deep-bed tests, which had lower NOx levels. The maximum iodine adsorption capacity and silver utilization for these higher NOx tests, at about 5-15% of the original sorbent mass, and about 12-35% of the total silver, respectively, were lower than for trends from prior silver aerogel and silver zeolite tests with lower NOx levels. Additional deep-bed testing and analyses are recommended to expand the database for organic iodide adsorption and increase the technical maturity if iodine adsorption processes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Stability of Tritium and Iodine Sorbents in TPOG Conditions

US regulations could require the removal of both iodine and tritium from the off-gas stream of a used nuclear fuel (UNF) reprocessing facility. Advanced tritium pretreatment is a pretreatment step that uses high concentrations of NOR2R in a gas stream to volatilize tritium and iodine from UNF prior to traditional dissolution. The gaseous effluent from this process would then require abatement to remove tritium and iodine, but high levels of NOR2R could have a detrimental effect on the ability of various solid sorbents to remove the volatile radionuclides. For tritium and iodine, the sorbents of interest are 3Å molecular sieve (3AMS) for tritium and reduced silver mordenite (AgP 0 PZ), silver-functionalized silica-aerogel (AgAerogel), and silver-nitrate-impregnated alumina (AgA) for iodine. Prior research has demonstrated that exposure to high concentrations of NOR2R can reduce the iodine loading capacity of AgP 0 PZ by > 90% when exposed for 1 week. Research in Japan has demonstrated that AgA is more robust to NOR2R exposure than AgZ. The testing described here was intended to assess the effects of high concentrations of NOR2R on the iodine capture capacity of AgA and the water adsorption capacity of 3AMS. To determine the effect of extended exposure of the sorbents to NOR2R, both 3AMS and AgA were aged in a 75% NOR2R environment prior to loading. The 3AMS samples were aged for 1, 4, and 5.5 weeks at 40°C. They were then loaded with water in a 10°C dew point stream (corresponding to a water concentration of ~12,000 ppmv) at 40°C. There was no significant change in the water adsorption capacity of the 3AMS upon exposure to 75% NOR2R. The AgA samples were aged for 1, 2, and 4 weeks at 150°C and were loaded with 50 ppmv IR2R at 150°C. The results show that the iodine capture capacity of AgA is reduced by exposure to high concentrations of NOR2R. The iodine capacity reductions were 16%, 36%, and 76% for 1, 2, and 4 week exposures, respectively. This is less of a capacity loss than that seen in similar testing with the AgP 0 PZ sorbent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

FCRD Advanced Reactor (Transmutation) Fuels Handbook

Transmutation of minor actinides such as Np, Am, and Cm in spent nuclear fuel is of international interest because of its potential for reducing the long-term health and safety hazards caused by the radioactivity of the spent fuel. One important approach to transmutation (currently being pursued by the DOE Fuel Cycle Research & Development Advanced Fuels Campaign) involves incorporating the minor actinides into U-Pu-Zr alloys, which can be used as fuel in fast reactors. U-Pu-Zr alloys are well suited for electrolytic refining, which leads to incorporation rare-earth fission products such as La, Ce, Pr, and Nd. It is, therefore, important to understand not only the properties of U-Pu-Zr alloys but also those of U-Pu-Zr alloys with concentrations of minor actinides (Np, Am) and rare-earth elements (La, Ce, Pr, and Nd) similar to those in reprocessed fuel. In addition to requiring extensive safety precautions, alloys containing U, Pu, and minor actinides (Np and Am) are difficult to study for numerous reasons, including their complex phase transformations, characteristically sluggish phasetransformation kinetics, tendency to produce experimental results that vary depending on the histories of individual samples, rapid oxidation, and sensitivity to contaminants such as oxygen in concentrations below a hundred parts per million. Although less toxic, rare-earth elements such as La, Ce, Pr, and Nd are also difficult to study for similar reasons. Many of the experimental measurements were made before 1980, and the level of documentation for experimental methods and results varies widely. It is, therefore, not surprising that little is known with certainty about U-Pu-Zr alloys, particularly those that also contain minor actinides and rare-earth elements. General acceptance of results commonly indicates that there is only a single measurement for a particular property. This handbook summarizes currently available information about U, Pu, Zr, Np, Am, La, Ce, Pr, and Nd and alloys of two or three of these elements. It contains information about phase diagrams and related information (including phases and phase transformations); heat capacity, entropy, and enthalpy; thermal expansion; and thermal conductivity and diffusivity. In addition to presenting information about materials properties, the handbook attempts to provide information about how well the property is known and how much variation exists between measurements. Although it includes some results from models, its primary focus is experimental data. The Handbook is organized in two sections: one with information about the U-Pu-Zr ternary and one with information about other elements and binary and vi ternary alloys in the U-Np-Pu-Am-La-Ce-Pr-Nd-Zr system. Within each section, information about elements is presented first, followed by information about binary alloys, then information about ternary alloys. The order in which the elements in each alloy are mentioned follows the order in the first sentence of this paragraph. Much of the information on the U-Pu-Zr system repeats information from the FCRD Transmutation Fuels Handbook 2015. Most of the other data has been published elsewhere (although scattered throughout numerous references, some quite obscure); however, some data from Idaho National Laboratory is presented here for the first time. As the FCRD programmatic mission evolves, future editions of this handbook will begin to include other advanced reactor fuel designs and compositions. Hence, the title of the handbook will transition to the Advanced Reactor Fuels Handbook.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Performance evaluation of the ORNL multi-elemental XRF analysis algorithms

Hybrid K-Edge Densitometer (HKED) systems integrate both K-Edge Densitometry (KED) and X-Ray Fluorescence (XRF) analyses to provide accurate rapid, assay results of the uranium and plutonium content of dissolver solution samples from nuclear fuel reprocessing facilities. Introduced for international safeguards applications in the late 1980s, the XRF component of the hybrid analyses is limited to quantification of U and Pu over a narrow range of U:Pu concentration ratios in the vicinity of ≈100. The analysis was further limited regarding the presence of minor actinide components where only a single minor actinide (typically Am) is included in the analysis and then only treated as an interference. The evolving nuclear fuel cycle has created the need to assay more complex dissolver solutions where uranium may no longer be the dominant actinide in the solution and the concentrations of the so called minor actinides (e.g., Th, Np, Am, and Cm) are sufficiently high that they can no longer be treated as impurities and ignored. Extension of the traditional HKED Region of Interest (ROI) based analysis to include these additional actinides is not possible due to the increased complexity of the XRF spectra. Oak Ridge National Laboratory (ORNL) has developed a spectral fitting approach to the HKED XRF measurement with an enhanced algorithm set to accommodate these complex XRF spectra. This report provides a summary of the spectral fitting methodology and examines the performance of these algorithms using data obtained from the ORNL HKED system, as well as data provided by the International Atomic Energy Agency (IAEA) on actual dissolver solutions.

97 MATHEMATICS AND COMPUTING↗

Project Overview: LA07-LAB072-PD02

The goal of this project was to identify and characterize sources of plutonium processing signatures, and understand how fate and transport impact these signatures, with an emphasis on establishing a foundation for the use of aerosolized particle characteristics as indicators of historic and current activities within a facility. Targeted activities included: 1) Pu metal reprocessing via direct oxide reduction, 2) Breakout of α-phase and δ-phase materials, 3) CNC machining of alloyed, δ-phase Pu metal, and 4) Low speed cutting of unalloyed, α-phase metal and alloyed, δ-phase Pu metal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Gamma-ray mirror technology for NDA of spent fuel

Direct measurements of gamma rays emitted by fissile material have been proposed as an alternative to measurements of the gamma rays from fission products. From a safeguards applications perspective, direct detection of uranium (U) and plutonium (Pu) K-shell fluorescence emission lines and specific lines from some of their isotopes could lead to improved shipper-receiver difference or input accountability at the start of Pu reprocessing. However, these measurements are difficult to implement when the spent fuel is in the line-of-sight of the detector, as the detector is exposed to high rates dominated by fission product emissions. To overcome the combination of high rates and high background, grazing incidence multilayer mirrors have been proposed as a solution to selectively reflect U and Pu hard X-ray and soft gamma rays in the 90 to 420 keV energy into a high-purity germanium (HPGe) detector shielded from the direct line-of-sight of spent fuel. Several groups demonstrated that K-shell fluorescence lines of U and Pu in spent fuel could be detected with Ge detectors. In the field of hard X-ray optics the performance of reflective multilayer coated reflective optics was demonstrated up to 645 keV at the European Synchrotron Radiation Facility. Initial measurements conducted at Oak Ridge National Laboratory with sealed sources and scoping experiments conducted at the ORNL Irradiated Fuels Examination Laboratory (IFEL) with spent nuclear fuel further demonstrated the pass-band properties of multilayer mirrors for reflecting specific emission lines into 1D and 2D HPGe detectors, respectively.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Multi-Column Kr/Xe Separation Testing at Representative Superficial Velocities with DGOSPREY Model Validation

Previous testing of AgZ-PAN and HZ-PAN for the separation and removal of xenon and krypton from air have been promising. This report details the results of multi-column testing at superficial velocities chosen to emulate probably velocities in a full-scale used nuclear fuel reprocessing facility. Additionally, results were used to validate the DG-OSPREY model under development at Georgia Institute of Technology.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Materials and Methods for Streamlined Laboratory Analysis of Environmental Samples, FY 2016 Report

The International Atomic Energy Agency (IAEA) relies upon laboratory analysis of environmental samples (typically referred to as “swipes”) collected during on-site inspections of safeguarded facilities to support the detection and deterrence of undeclared activities. Unfortunately, chemical processing and assay of the samples is slow and expensive. A rapid, effective, and simple extraction process and analysis method is needed to provide certified results with improved timeliness at reduced costs (principally in the form of reduced labor), while maintaining or improving sensitivity and efficacy. To address these safeguard needs the Pacific Northwest National Laboratory (PNNL) explored and demonstrated improved methods for environmental sample (ES) analysis. Improvements for both bulk and particle analysis were explored. To facilitate continuity and adoption, the new sampling materials and processing methods will be compatible with existing IAEA protocols for ES analysis. PNNL collaborated with Oak Ridge National Laboratory (ORNL), which performed independent validation of the new bulk analysis methods and compared performance to traditional IAEA’s Network of Analytical Laboratories (NWAL) protocol. ORNL efforts are reported separately. This report describes PNNL’s FY 2016 progress, which was focused on analytical application supporting environmental monitoring of uranium enrichment plants and nuclear fuel processing. In the future the technology could be applied to other safeguard applications and analytes related to fuel manufacturing, reprocessing, etc. PNNL’s FY 2016 efforts were broken into two tasks and a summary of progress, accomplishments and highlights are provided below. Principal progress and accomplishments on Task 1, Optimize Materials and Methods for ICP-MS Environmental Sample Analysis, are listed below. • Completed initial procedure for rapid uranium extraction from ES swipes based upon carbonate-peroxide chemistry (delivered to ORNL for evaluation). • Explored improvements to carbonate-peroxide rapid uranium extraction chemistry. • Evaluated new sampling materials and methods (in collaboration with ORNL). • Demonstrated successful ES extractions from standard and novel swipes for a wide range uranium compounds of interest including UO 2 F 2 and UO 2 (NO 3 ) 2 , U 3 O 8 and uranium ore concentrate. • Completed initial discussions with commercial suppliers of PTFE swipe materials. • Submitted one manuscript for publication. Two additional drafts are being prepared. Principal progress and accomplishments on Task 2, Optimize Materials and Methods for Direct SIMS Environmental Sample Analysis, are listed below. • Designed a SIMS swipe sample holder that retrofits into existing equipment and provides simple, effective, and rapid mounting of ES samples for direct assay while enabling automation and laboratory integration. • Identified preferred conductive sampling materials with better performance characteristics. • Ran samples on the new PNNL NWAL equivalent Cameca 1280 SIMS system. • Obtained excellent agreement between isotopic ratios for certified materials and direct SIMS assay of very low levels of LEU and HEU UO 2 F 2 particles on carbon fiber sampling material. Sample activities range from 1 to 500 CPM (uranium mass on sample is dependent upon specific isotope ratio but is frequently in the subnanogram range). • Found that the presence of the UF molecular ions, as measured by SIMS, provides chemical information about the particle that is separate from the uranium isotopics and strongly suggests that those particles originated from an UF6 enrichment activity. • Submitted one manuscript for publication. Another manuscript is in preparation.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Evaluation of Iodine Remediation Technologies in Subsurface Sediments: Interim Status Report

Isotopes of iodine were generated during plutonium production from nine production reactors at the U.S. Department of Energy Hanford Site. The long half-life 129I generated at the Hanford Site during reactor operations was 1) stored in single-shell and double-shell tanks, 2) discharged to liquid disposal sites (e.g., cribs and trenches), 3) released to the atmosphere during fuel reprocessing operations, or 4) captured by off-gas absorbent devices (silver reactors) at chemical separations plants (PUREX, B-Plant, T-Plant, and REDOX). Releases of 129I to the subsurface have resulted in several large, though dilute, plumes in the groundwater, including the plume in the 200-UP-1 operable unit. There is also 129I remaining in the vadose zone beneath disposal or leak locations. Because 129I is an uncommon contaminant, relevant remediation experience and scientific literature are limited.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Conceptual Model of Iodine Behavior in the Subsurface at the Hanford Site

Isotopes of iodine were generated during plutonium production within the nine production reactors at the U.S. Department of Energy Hanford Site. The short half-life 131I that was released from the fuel into the atmosphere during the dissolution process (when the fuel was dissolved) in the Hanford Site 200 Area is no longer present at concentrations of concern in the environment. The long half-life 129I generated at the Hanford Site during reactor operations was (1) stored in single-shell and double-shell tanks, (2) discharged to liquid disposal sites (e.g., cribs and trenches), (3) released to the atmosphere during fuel reprocessing operations, or (4) captured by off-gas absorbent devices (silver reactors) at chemical separations plants (PUREX, B-Plant, T-Plant, and REDOX). Releases of 129I to the subsurface have resulted in several large, though dilute, plumes in the groundwater. There is also 129I remaining in the vadose zone beneath disposal or leak locations. The fate and transport of 129I in the environment and potential remediation technologies are currently being studied as part of environmental remediation activities at the Hanford Site. A conceptual model describing the nature and extent of subsurface contamination, factors that control plume behavior, and factors relevant to potential remediation processes is needed to support environmental remedy decisions. Because 129I is an uncommon contaminant, relevant remediation experience and scientific literature are limited. In addition, its behavior in subsurface is different from that of other more common and important contaminants (e.g., U, Cr and Tc) in terms of sorption (adsorption and precipitation), and aqueous phase species transformation via redox reactions. Thus, the conceptual model also needs to both describe known contaminant and biogeochemical process information and identify aspects about which additional information is needed to effectively support remedy decisions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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↗

Milestone Report - Data Requirements and Test System Needs for Development of an Integrated Off-Gas Treatment System

In fiscal year 2016 an Engineering Evaluation of an integrated off-gas system was conducted. This study resulted in a report entitled Engineering Evaluation of an Integrated Off-Gas Treatment System for Used Nuclear Fuel Reprocessing Facilities (Jubin et al. 2016a), from here referred to as the “Engineering Evaluation.” This study focused on the capture and retention of the volatile radionuclides ( 3 H, 14 C, 85 Kr, and 129 I), selected semi-volatile radionuclides, specifically 106 Ru, and chemical species like NO and NO 2 generated during the dissolution of the used nuclear fuel. The study examined the design of the combined head-end off-gas streams and the vessel off-gas stream. The study drew upon the available literature to conduct the equipment sizing and sorbent usage. A number of assumptions were required to complete this analysis and major gaps in the available data were identified that, if resolved, could increase the fidelity of the engineering design.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Cross-Calibration of the GPS Constellation CXD Proton Data with GOES EPS [Slides]

The CXD provides good quality proton flux measurements across a range of proton energies. The data within the 1 st and 3 rd quartile range of the ratio of integral flux values is within 20 – 40%. While proton response of the CXD extends down to 6 MeV due to collimator holes in instrument filters, the > 10 MeV integral proton flux is not well captured as shown by the comparisons with EPS. We recommend that users of the data restrict their analysis to proton energies > 20 MeV. Although the full dataset is available now [https://www.ngdc.noaa.gov/stp/spaceweather/satellite-data/satellite-systems/gps/] this updated flux calculation is not present and so a reprocessing will commence soon and the dataset updated. These calibrated datasets will allow a number of exciting multipoint analyses such as more accurate probing of geomagnetic cutoffs as well as providing additional input to radiation belt climatology models such as AE9/AP9/SPM [Ginet et al., 2013].

58 GEOSCIENCES↗