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DOE OSTI2013

Fukushima Daiichi Information Repository FY13 Status

The accident at the Fukushima Daiichi nuclear power station in Japan is one of the most serious in commercial nuclear power plant operating history. Much will be learned that may be applicable to the U.S. reactor fleet, nuclear fuel cycle facilities, and supporting systems, and the international reactor fleet. For example, lessons from Fukushima Daiichi may be applied to emergency response planning, reactor operator training, accident scenario modeling, human factors engineering, radiation protection, and accident mitigation; as well as influence U.S. policies towards the nuclear fuel cycle including power generation, and spent fuel storage, reprocessing, and disposal. This document describes the database used to establish a centralized information repository to store and manage the Fukushima data that has been gathered. The data is stored in a secured (password protected and encrypted) repository that is searchable and available to researchers at diverse locations.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2014

Laboratory Evaporation Testing Of Hanford Waste Treatment Plant Low Activity Waste Off-Gas Condensate Simulant

The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream, LAW Off-Gas Condensate, from the off-gas system. The baseline plan for disposition of this stream is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation and recycled to the LAW vitrification facility again. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable de-coupled operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also decrease the LAW vitrification mission duration and quantity of canistered glass waste forms. This LAW Off-Gas Condensate stream contains components that are volatile at melter temperatures and are problematic for the glass waste form. Because this stream recycles within WTP, these components accumulate in the Condensate stream, exacerbating their impact on the number of LAW glass containers that must be produced. Approximately 32% of the sodium in Supplemental LAW comes from glass formers used to make the extra glass to dilute the halides to be within acceptable concentration ranges in the LAW glass. Diverting the stream reduces the halides in the recycled Condensate and is a key outcome of this work. Additionally, under possible scenarios where the LAW vitrification facility commences operation prior to the WTP Pretreatment facility, identifying a disposition path becomes vitally important. This task examines the impact of potential future disposition of this stream in the Hanford tank farms, and investigates auxiliary evaporation to enable another disposition path. Unless an auxiliary evaporator is used, returning the stream to the tank farms would require evaporation in the 242-A evaporator. This stream is expected to be unusual because it will be very high in corrosive species that are volatile in the melter (chloride, fluoride, sulfur), will have high ammonia, and will contain carryover particulates of glass-former chemicals. These species have potential to cause corrosion of tanks and equipment, precipitation of solids, release of ammonia gas vapors, and scale in the tank farm evaporator. Routing this stream to the tank farms does not permanently divert it from recycling into the WTP, only temporarily stores it prior to reprocessing. Testing is normally performed to demonstrate acceptable conditions and limits for these compounds in wastes sent to the tank farms. The primary parameter of this phase of the test program was measuring the formation of solids during evaporation in order to assess the compatibility of the stream with the evaporator and transfer and storage equipment. The origin of this LAW Off-Gas Condensate stream will be the liquids from the Submerged Bed Scrubber (SBS) and the Wet Electrostatic Precipitator (WESP) from the LAW facility melter offgas system. The stream is expected to be a dilute salt solution with near neutral pH, and will likely contain some insoluble solids from melter carryover. The soluble components are expected to be mostly sodium and ammonium salts of nitrate, chloride, and fluoride. This stream has not been generated yet, and, thus, the composition will not be available until the WTP begins operation, but a simulant has been produced based on models, calculations, and comparison with pilot-scale tests. This report discusses results of evaporation testing of the simulant. Two conditions were tested, one with the simulant at near neutral pH, and a second at alkaline pH. The neutral pH test is comparable to the conditions in the Hanford Effluent Treatment Facility (ETF) evaporator, although that evaporator operates at near atmospheric pressure and tests were done under vacuum. For the alkaline test, the target pH was based on the tank farm corrosion control program requirements, and the test protocol and equipment was comparable to that used for routine evaluation of feed compatibility studies for the 242-A evaporator. One of the radionuclides that is volatile in the melter and expected to be in high concentration in this LAW Off-Gas Condensate stream is Technetium-99 (99Tc). Technetium will not be removed from the aqueous waste in the Hanford WTP, and will primarily end up immobilized in the LAW glass by repeated recycle of the off-gas condensate into the LAW melter. Other radionuclides that are also expected to be in appreciable concentrations in the LAW Off-Gas Condensate are 129I, 90Sr, 137Cs, and 241Am. The concentrations of these radionuclides in this stream will be much lower than in the LAW, but they will still be higher than limits for some of the other disposition pathways currently available. At this time, these scoping tests did not evaluate the partitioning of the radionuclides to the evaporator condensate, since ample data are available separately from other experience in the DOE complex. Results from the evaporation testing show that the neutral SBS simulant first forms turbidity at ~7.5X concentration, while the alkaline-adjusted simulant became turbid at ~3X concentration. The major solid in both cases was Kogarkoite, Na3FSO4. Sodium and lithium fluorides were also detected. Minimal solids were formed in the evaporator bottoms until a substantial fraction of liquid was removed, indicating that evaporation could minimize storage volume issues. Achievable concentration factors without significant insoluble solids were 17X at alkaline pH, and 23X at neutral pH. In both runs, significant ammonia carried over and was captured in the condenser with the water condensate. Results also indicate that with low insoluble solids formation in the initial testing at neutral pH, the use of Reverse Osmosis is a potential alternate method for concentrating the solution, although an evaluation is needed to identify equipment that can tolerate insoluble solids. Most of the ammonia remains in the evaporator bottoms during the neutral pH evaporation, but partitions to the condensate during alkaline evaporation. Disposition of both streams needs to consider the management of ammonia vapor and its release. Since this is an initial phase of testing, additional tasks related to evaporation methods are expected to be identified for development. These tasks likely include evaluation and testing of composition variability testing and evaluations, corrosion and erosion testing, slurry storage and immobilization investigations, and evaporator condensate disposition.

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

Informal Preliminary Report on Comparisons of Prototype SPN-1 Radiometer to PARSL Measurements

The prototype SPN-1 has been taking measurements for several months collocated with our PNNL Atmospheric Remote Sensing Laboratory (PARSL) solar tracker mounted instruments at the Pacific Northwest National Laboratory (PNNL) located in Richland, Washington, USA. The PARSL radiometers used in the following comparisons consist of an Eppley Normal Incident Pyrheliometer (NIP) and a shaded Eppley model 8-48 “Black and White” pyrgeometer (B&W) to measure the direct and diffuse shortwave irradiance (SW), respectively. These instruments were calibrated in mid-September by comparison to an absolute cavity radiometer directly traceable to the world standard group in Davos, Switzerland. The NIP calibration was determined by direct comparison, while the B&W was calibrated using the shade/unshade technique. All PARSL data prior to mid-September have been reprocessed using the new calibration factors. The PARSL data are logged as 1-minute averages from 1-second samples. Data used in this report span the time period from June 22 through December 1, 2006. All data have been processed through the QCRad code (Long and Shi, 2006), which itself is a more elaborately developed methodology along the lines of that applied by the Baseline Surface Radiation Network (BSRN) Archive (Long and Dutton, 2004), for quality control. The SPN-1 data are the standard total and diffuse SW values obtained from the analog data port of the instrument. The comparisons use only times when both the PARSL and SPN-1 data passed all QC testing. The data were further processed and analyzed by application of the SW Flux Analysis methodology (Long and Ackerman, 2000; Long and Gaustad, 2004, Long et al., 2006) to detect periods of clear skies, calculate continuous estimates of clear-sky SW irradiance and the effect of clouds on the downwelling SW, and estimate fractional sky cover.

Long, Charles N.↗
DOE OSTI2014

Silicate Based Glass Formulations for Immobilization of U.S. Defense Wastes Using Cold Crucible Induction Melters

The cold crucible induction melter (CCIM) is an alternative technology to the currently deployed liquid-fed, ceramic-lined, Joule-heated melter for immobilizing of U.S. tank waste generated from defense related reprocessing. In order to accurately evaluate the potential benefits of deploying a CCIM, glasses must be developed specifically for that melting technology. Related glass formulation efforts have been conducted since the 1990s including a recent study that is first documented in this report. The purpose of this report is to summarize the silicate base glass formulation efforts for CCIM testing of U.S. tank wastes. Summaries of phosphate based glass formulation and phosphate and silicate based CCIM demonstration tests are reported separately (Day and Ray 2013 and Marra 2013, respectively). Combined these three reports summarize the current state of knowledge related to waste form development and process testing of CCIM technology for U.S. tank wastes.

Cold crucible induction melter↗
DOE OSTI2013

Land and Water Use, CO2 Emissions, and Worker Radiological Exposure Factors for the Nuclear Fuel Cycle

The Department of Energy Office of Nuclear Energy’s Fuel Cycle Technologies program is preparing to evaluate several proposed nuclear fuel cycle options to help guide and prioritize Fuel Cycle Technology research and development. Metrics are being developed to assess performance against nine evaluation criteria that will be used to assess relevant impacts resulting from all phases of the fuel cycle. This report focuses on four specific environmental metrics. • land use • water use • CO2 emissions • radiological Dose to workers Impacts associated with the processes in the front-end of the nuclear fuel cycle, mining through enrichment and deconversion of DUF6 are summarized from FCRD-FCO-2012-000124, Revision 1. Impact estimates are developed within this report for the remaining phases of the nuclear fuel cycle. These phases include fuel fabrication, reactor construction and operations, fuel reprocessing, and storage, transport, and disposal of associated used fuel and radioactive wastes. Impact estimates for each of the phases of the nuclear fuel cycle are given as impact factors normalized per unit process throughput or output. These impact factors can then be re-scaled against the appropriate mass flows to provide estimates for a wide range of potential fuel cycles. A companion report, FCRD-FCO-2013-000213, applies the impact factors to estimate and provide a comparative evaluation of 40 fuel cycles under consideration relative to these four environmental metrics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

NO2 Aging and Iodine Loading of Silver-Functionalized Aerogels

Off-gas treatment systems in used fuel reprocessing which use fixed-bed adsorbers are typically designed to operate for an extended period of time before replacement or regeneration of the adsorbent. During this time, the sorbent material will be exposed to the off-gas stream. Exposure could last for months, depending on the replacement cycle time. The gas stream will be at elevated temperature and will possibly contain a mixture of water vapor, NOx, nitric acid vapors, and a variety of other constituents in addition to the radionuclides of capture interest. A series of studies were undertaken to evaluate the effects of long-term exposure, or aging, on proposed iodine sorbent materials under increasingly harsh off-gas conditions. Previous studies have evaluated the effects of up to 6 months of aging under dry air and under humid air conditions on the iodine loading behavior of Ag0-functionalized aerogels. This study examines the effects of extended exposure (up to 6 months) to NO2 on the iodine loading capacity of Ag0- functionalized aerogels. Material aged for 1 and 2 months appeared to have a similar total loading capacity to fresh material. Over an aging period of 4 months, a loss of approximately 15% of the total iodine capacity was seen. The iodine capacity loss on silver-functionalized aerogels due to NO2 was smaller than the iodine capacity loss due to humid or dry air aging.

Patton, K K↗
DOE OSTI2014

Complete Phase I Tests As Described in the Multi-lab Test Plan for the Evaluation of CH3I Adsorption on AgZ

Silver-exchanged mordenite (AgZ) has been identified as a potential sorbent for iodine present in the off-gas streams of a used nuclear fuel reprocessing facility. In such a facility, both elemental and organic forms of iodine are released from the dissolver in gaseous form. These species of iodine must be captured with high efficiency for a facility to avoid radioactive iodine release above regulatory limits in the gaseous effluent of the plant. Studies completed at Idaho National Laboratory (INL) examined the adsorption of organic iodine in the form of CH3I by AgZ. Upon breakthrough of the feed gas through the sorbent bed, elemental iodine was observed in the effluent stream, despite the fact that the only source of iodine in the system was the CH3I in the feed gas.1 This behavior does not appear to have been reported previously nor has it been independently confirmed. Thus, as a result of these prior studies, multiple knowledge gaps relating to the adsorption of CH3I by AgZ were identified, and a multi-lab test plan, including Oak Ridge National Laboratory (ORNL), INL, Pacific Northwest National Laboratory (PNNL), and Sandia National Laboratories, was formulated to address each in a systematic way.2 For this report, the scope of work for ORNL was further narrowed to three thin-bed experiments that would characterize CH3I adsorption onto AgZ in the presence of water, NO, and NO2. Completion of these three-thin bed experiments demonstrated that organic iodine in the form of CH3I was adsorbed by reduced silver mordenite (Ag0Z) to a 50% higher loading than that of I2 when adsorbed from a dry air stream. Adsorption curves suggest different adsorption mechanisms for I2 and CH3I. In the presence of NO and NO2 gas, the loading of CH3I onto Ag0Z is suppressed and may be reversible. Further, the presence of NO and NO2 gas appears to oxidize CH3I to I2; this is indicated by an adsorption curve similar to that of I2 on Ag0Z. Finally, the loss of organic iodine loading capacity by Ag0Z in the presence of NOx is unaffected by the addition of water vapor to the gas stream; no marked additional loss in capacity or retention was observed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Expanded Analysis of Hot Isostatic Pressed Iodine-Loaded Silver-Exchanged Mordenite

Reduced silver-exchanged mordenite (Ag0Z) is being evaluated as a potential material to control the release of radioactive iodine that is released during the reprocessing of used nuclear fuel into the plant off-gas streams. The purpose of this study was to determine if hot pressing could directly convert this iodine loaded sorbent into a waste form suitable for long-term disposition. The minimal pretreatment required for production of pressed pellets makes hot pressing a technically and economically desirable process. Initial scoping studies utilized hot uniaxial pressing (HUPing) to prepare samples of non-iodine-loaded reduced silver exchanged mordenite (Ag0Z). The resulting samples were very fragile due to the low pressure (~ 28 MPa) used. It was recommended that hot isostatic pressing (HIPing), performed at higher temperatures and pressures, be investigated. HIPing was carried out in two phases, with a third and final phase currently underway. Phase I evaluated the effects of pressure and temperature conditions on the manufacture of a pressed sample. The base material was an engineered form of silver zeolite. Six samples of Ag0Z and two samples of I-Ag0Z were pressed. It was found that HIPing produced a pressed pellet of high density. Analysis of each pressed pellet by scanning electron microscopy-energy dispersive spectrophotometry (SEM-EDS) and X-ray diffraction (XRD) demonstrated that under the conditions used for pressing, the majority of the material transforms into an amorphous structure. The only crystalline phase observed in the pressed Ag0Z material was SiO2. For the samples loaded with iodine (I-Ag0Z) iodine was present as AgI clusters at low temperatures, and transformed into AgIO4 at high temperatures. Surface mapping and EDS demonstrate segregation between silver iodide phases and silicon dioxide phases. Based on the results of the Phase I study, an expanded test matrix was developed to examine the effects of multiple source materials, compositional variations, and an expanded temperature range. Each sample was analyzed with the approach used in Phase I. In all cases, there is nothing in the SEM or XRD analyses that indicates creation of any AgI-containing silicon phase, with the samples being found to be largely amorphous. Phase III of this study has been initiated and is the final phase of scoping tests. It will expand upon the test matrix completed in Phase II and will examine the durability of the pressed pellets through product consistency testing (PCT) studies. Transformation of the component material into a well-characterized iodine-containing mineral phase would be desirable. This would limit the additional experimental testing and modeling required to determine the long-term stability of the pressed pellet, as much of that information has already been learned for several common iodine-containing minerals. However, this is not an absolute requirement, especially if pellets produced by hot isostatic pressing can be demonstrated through initial PCT studies to retain iodine well despite their amorphous composition.

hot isostatic pressing↗
DOE OSTI2014

Overview of different aspects of climate change effects on soils

Climate change [i.e., high atmospheric carbon dioxide (CO 2 ) concentrations (≥400 ppm); increasing air temperatures (2-4°C or greater); significant and/or abrupt changes in daily, seasonal, and inter-annual temperature; changes in the wet/dry cycles; intensive rainfall and/or heavy storms; extended periods of drought; extreme frost; heat waves and increased fire frequency] is and will significantly affect soil properties and fertility, water resources, food quantity and quality, and environmental quality. Biotic processes that consume atmospheric CO 2 and create organic carbon (C) that is either reprocessed to CO 2 or stored in soils, are the subject of active current investigations with great concern over the influence of climate change. In addition, abiotic C cycling and its influence on the inorganic C pool in soils is a fundamental global process in which acidic atmospheric CO 2 participates in the weathering of carbonate and silicate minerals, ultimately delivering bicarbonate and Ca 2 + or other cations that precipitate in the form of carbonates in soils or are transported to the rivers, lakes, and oceans. Soil responses to climate change will be complex, and there are many uncertainties and unresolved issues. The objective of the review is to initiate and further stimulate a discussion about some important and challenging aspects of climate-change effects on soils, such as accelerated weathering of soil minerals and resulting C and elemental fluxes in and out of soils, soil/geo-engineering methods used to increase C sequestration in soils, soil organic matter (SOM) protection, transformation and mineralization, and SOM temperature sensitivity. This review reports recent discoveries and identifies key research needs required to understand the effects of climate change on soils.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Viscosity Meaurement Technique for Metal Fuels

Metallic fuels have exceptional transient behavior, excellent thermal conductivity, and a more straightforward reprocessing path, which does not separate out pure plutonium from the process stream. Fabrication of fuel containing minor actinides and rare earth (RE) elements for irradiation tests, for instance, U-20Pu-3Am-2Np-1.0RE-15Zr samples at the Idaho National Laboratory, is generally done by melt casting in an inert atmosphere. For the design of a casting system and further scale up development, computational modeling of the casting process is needed to provide information on melt flow and solidification for process optimization. Therefore, there is a need for melt viscosity data, the most important melt property that controls the melt flow. The goal of the project was to develop a measurement technique that uses fully sealed melt sample with no Americium vapor loss to determine the viscosity of metallic melts and at temperatures relevant to the casting process. The specific objectives of the project were to: develop mathematical models to establish the principle of the measurement method, design and build a viscosity measurement prototype system based on the established principle, and calibrate the system and quantify the uncertainty range. The result of the project indicates that the oscillation cup technique is applicable for melt viscosity measurement. Detailed mathematical models of innovative sample ampoule designs were developed to not only determine melt viscosity, but also melt density under certain designs. Measurement uncertainties were analyzed and quantified. The result of this project can be used as the initial step toward the eventual goal of establishing a viscosity measurement system for radioactive melts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Adsorption Isotherms for Xenon and Krypton using INL HZ-PAN and AgZ-PAN Sorbents

The generation of adsorption isotherms compliments the scale-up of off-gas processes used to control the emission of encapsulated radioactive volatile fission and activation products released during Used Nuclear Fuel (UNF) reprocessing activities. A series of experiments were conducted to obtain capacity results for varying Kr and Xe gas concentrations using HZ-PAN and AgZ-PAN engineered form sorbents. Gas compositions for Kr ranged from 150-40,000 ppmv and 250-5020 ppmv for Xe in a helium balance. The experiments were all performed at 220 K at a flowrate of 50 sccm. Acquired capacities were then respectively fit to the Langmuir equation using the Langmuir linear regression method to obtain the equilibrium parameters Qmax and Keq. Generated experimental adsorption isotherms were then plotted with the Langmuir predicted isotherms to illustrate agreement between the two. The Langmuir parameters were provided for input into the OSPREY model to predict breakthrough of single component adsorption of Kr and Xe on HZ-PAN and AgZ-PAN sorbents at the experimental conditions tested. Kr and Xe capacities resulting from model breakthrough predictions were then compared to experimental capacities for model validation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Delayed Gamma-ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

This project addresses the need for improved non-destructive assay techniques for quantifying the actinide composition of spent nuclear fuel and for the independent verification of declared quantities of special nuclear materials at key stages of the fuel cycle. High-energy delayed gamma-ray spectroscopy following neutron irradiation is a potential technique for directly assaying spent fuel assemblies and achieving the safeguards goal of quantifying nuclear material inventories for spent fuel handling, interim storage, reprocessing facilities, repository sites, and final disposal. Other potential applications include determination of MOX fuel composition, characterization of nuclear waste packages, and challenges in homeland security and arms control verification.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2015

Cold Crucible Induction Melter (CCIM) Testing on Glass Ceramic and Ceramic Waste Forms

The U.S. Department of Energy Office of Nuclear Energy’s Fuel Cycle Research and Development (FCR&D) program is developing advanced high level waste (HLW) forms for the immobilization of the long-lived radionuclides resulting from future potential reprocessing of the used nuclear fuel from commercial reactors. One of the program’s goals is to have orders of magnitude improvements in durability (compared to the reference borosilicate glass waste form for HLW), to facilitate lower costs including less expensive and complex processing, to lower storage costs and to provide for final disposal of the waste in a deep geological repository. Both glass ceramic and ceramic waste forms are being developed and evaluated as possible improvements to borosilicate glass to achieve these objectives.

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

Geothermal Exploration of Newberry Volcano, Oregon

Davenport Newberry (Davenport) has completed 8 years of exploration for geothermal energy on Newberry Volcano in central Oregon. Two deep exploration test wells were drilled by Davenport on the west flank of the volcano, one intersected a hydrothermal system; the other intersected isolated fractures with no hydrothermal interconnection. Both holes have bottom-hole temperatures near or above 315°C (600°F). Subsequent to deep test drilling an expanded exploration and evaluation program was initiated. These efforts have included reprocessing existing data, executing multiple geological, geophysical, geochemical programs, deep exploration test well drilling and shallow well drilling. The efforts over the last three years have been made possible through a DOE Innovative Exploration Technology (IET) Grant 109, designed to facilitate innovative geothermal exploration techniques. The combined results of the last 8 years have led to a better understanding of the history and complexity of Newberry Volcano and improved the design and interpretation of geophysical exploration techniques with regard to blind geothermal resources in volcanic terrain.

15 GEOTHERMAL ENERGY↗
DOE OSTI2015

Hydroxylamine Nitrate Decomposition under Non-radiological Conditions

Hydroxylamine nitrate (HAN) is used to reduce Pu(IV) to Pu(III) in the separation of plutonium from uranium. HAN becomes unstable under certain conditions and has been known to explode, causing injury to humans including death. Hence, it is necessary to deactivate HAN once the reduction of plutonium is finished. This report reviews what is known about the chemistry of HAN and various methods to achieve a safe decomposition. However, there are areas where more information is needed to make a decision about the handling of HAN in reprocessing of nuclear fuel. Experiments have demonstrated a number of non-radiolytic ways to safely decompose HAN, including heating in HNO 3 , photolytic oxidation in the presence of H 2 O 2 , and the addition of a metal such as Fe(III) that will oxidize the HAN.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2014

Evaluation of Tritium Content and Release from Surry-2 Fuel Cladding (Milestone Report)

To design and operate future reprocessing plants in a safe and environmentally compliant manner, the amount and form of tritium in the used nuclear fuel (UNF) must be understood and quantified. To gain a better understanding of how tritium in cladding will behave during processing, scoping tests are being performed to determine the tritium content in the cladding pre- and post-tritium pretreatment. A sample of Surry-2 pressurized water reactor (PWR) cladding was heated to 1100–1200°C to oxidize the zirconium and release all of the tritium in the cladding sample. The tritium content was measured to be ~240 µCi/g. Cladding samples were heated to 500ºC, which is within the temperature range (480 - 600ºC) expected for standard air tritium pretreatment systems, and to a slightly higher temperature (700ºC) to determine the impact of tritium pretreatment on tritium release from the cladding. Heating at 500°C for 24 hr removes ~0.2% of the tritium from the cladding, and heating at 700°C for 24 hr removes ~9%. Thus, a significant fraction of the tritium remains bound in the cladding and must be considered in operations involving cladding recycle.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Complete NO and NO 2 Aging Study for AgZ (Milestone Report)

In an off-gas system within a nuclear fuel reprocessing plant, any capture material will be exposed to a gas stream for months at a time. This gas stream may be at elevated temperature and could contain water, NO x gas, or a variety of other constituents that comprise the off-gas stream. For this reason, it is important to understand the effects of long-term exposure, or aging, on proposed capture materials. One material under consideration is silver-exchanged mordenite (AgZ). The aim of this study was to determine the effect of extended exposure at 150°C to an air stream containing NO on the iodine capture capacity of the hydrogen reduced form of AgZ designated as Ag 0 Z. The study was originally also intended to expand on the static NO 2 aging studies by exposing Ag 0 Z to a flowing stream of NO 2 for an extended period of time, but those tests were delayed due to NO 2 production schedules by the gas vendor. Unreduced silver mordenite has a loading capacity of approximately 25 mg I/g AgZ and that capacity is increased to 100 mg I/g Ag 0 Z upon reduction. It appears that extended exposure of AgZ to 1% NO at 150°C may not only neutralize the increased capacity gained by reduction, but perhaps degrade the sorbent even further. Loss of 80% of sorbent capacity and surface area was observed after 8 weeks of exposure to a 1% NO stream at 150°C. Investigations continue into the effects of aging by off-gas components on iodine sorbents. Future work will age silver mordenite with streams containing NO 2 . As the simulated off-gas streams become more complex and more corrosive, the ability of AgZ to withstand conditions present in off-gas streams will be more fully known.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Complete Iodine Loading of NO-Aged Ag 0 -Functionalized Silica Aerogel (Milestone Report)

In off-gas treatment systems within a nuclear fuel reprocessing plant, capture materials will be exposed to a gas stream for extended periods during their lifetime. This gas stream may be at elevated temperature and could contain water, NO x gas, or a variety of other constituents. For this reason, it is important to understand the effects of long-term exposure, or aging, on proposed capture materials. One material under consideration for iodine sequestration is silver-functionalized silica aerogel (Ag 0 -aerogel). The aim of this study was to determine the effect of extended exposure at 150°C to an air stream containing NO on the iodine capture capacity of Ag 0 -aerogel. Ag 0 -aerogel was provided by the Pacific Northwest National Laboratory (PNNL), which manufactures the material at a lab scale. Prior to aging, the material has an iodine loading capacity of approximately 290 mg I/g Ag 0 -aerogel. Previous studies have aged the material in a dry air stream or in a moist air stream for up to 6 months. Both tests resulted in a 22% loss in iodine capacity. Aging the material in a static 2% NO 2 environment for up to 2 months results in a 15% loss of iodine capacity.3 In this study, exposure of Ag 0 -aerogel to 1% NO at 150°C for 2 months produced a loss of 43% in iodine loading capacity. This is largest loss observed for aerogel aging studies to date. The performance of Ag 0 -aerogel in this study was compared to the performance of reduced silver mordenite (Ag 0 Z) in similar studies. Ag 0 Z is a zeolite mineral considered to be the current standard technology for iodine removal from off-gas streams of a potential US used fuel processing plant. In an aging study exposing Ag 0 Z to 1% NO for 2 months, an iodine capacity loss of over 80% was observed. This corresponds to a silver utilization of 13.5% for 2 month NO-aged Ag 0 Z, compared to 57% silver utilization for 2 month NO-aged aerogel. While iodine loading capacity and silver utilization are critical parameters in evaluating these materials, other properties must also be considered when selecting the appropriate material (e.g., relative material densities and potential waste form production technology). The resistance of Ag 0 -aerogel to NO is promising, and investigations of this material for use in iodine capture should continue to be pursued.

36 MATERIALS SCIENCE↗