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All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Waste Stream Treatment and Waste Form Fabrication for Pyroprocessing of Used Nuclear Fuel

This report summarizes treatment and waste form options being evaluated for waste streams resulting from the electrochemical/pyrometallurgical (pyro ) processing of used oxide nuclear fuel. The technologies that are described are South Korean (Republic of Korea – ROK) and United States of America (US) ‘centric’ in the approach to treating pyroprocessing wastes and are based on the decade long collaborations between US and ROK researchers. Some of the general and advanced technologies described in this report will be demonstrated during the Integrated Recycle Test (IRT) to be conducted as a part of the Joint Fuel Cycle Study (JFCS) collaboration between US Department of Energy (DOE) and ROK national laboratories. The JFCS means to specifically address and evaluated the technological, economic, and safe guard issues associated with the treatment of used nuclear fuel by pyroprocessing. The IRT will involve the processing of commercial, used oxide fuel to recover uranium and transuranics. The recovered transuranics will then be fabricated into metallic fuel and irradiated to transmutate, or burn the transuranic elements to shorter lived radionuclides. In addition, the various process streams will be evaluated and tested for fission product removal, electrolytic salt recycle, minimization of actinide loss to waste streams and waste form fabrication and characterization. This report specifically addresses the production and testing of those waste forms to demonstrate their compatibility with treatment options and suitability for disposal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Characterization of crystalline ceramic waste form

The research conducted in this work package is to collect data in support of future development of ceramic waste forms and to help develop the next generation high performance waste management technologies. This work package collaborates closely with the work conducted under “Ceramics - Savannah River National Laboratory (SRNL) - (FT-15SR030702)” and the NEUP project “Alternative High-Performance Ceramic Waste Forms” – Alfred University (AU) – (DE-AC07-05ID14517)”. The Los Alamos National Laboratory (LANL) is focusing on characterization and testing procedure on the reference crystalline ceramics to further develop the crystalline ceramic waste form to incorporate combined HLW raffinate stream and/or TRU stream from fuels fabrication processes. In Fiscal Year 2015, we are mainly working on cold crucible induction melter (CCIM) test multi-phase crystalline ceramic waste form samples and single phase hollandite materials. Various characterization techniques (including X-ray diffraction, transmission electron microscopy, scanning electron microscopy) were used to characterize CCIM samples. For the radiation stability test, in situ radiation techniques were employed to simulate self-radiation in waste form samples.

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

Online Waste Library (OWL) and Waste Forms Characteristics Annual Report

This report represents completion of milestone deliverable M2SF-19SNO10309013 "Online Waste Library (OWL) and Waste Forms Characteristics Annual Report" that reports annual status on fiscal year (FY) 2019 activities for the work package SF-19SN01030901 and is due on August 2, 2019. The online waste library (OWL) has been designed to contain information regarding United States (U.S.) Department of Energy (DOE)-managed (as) high-level waste (DHLW), spent nuclear fuel (SNF), and other wastes that are likely candidates for deep geologic disposal, with links to the current supporting documents for the data (when possible; note that no classified or official-use-only (OUO) data are planned to be included in OWL). There may be up to several hundred different DOE-managed wastes that are likely to require deep geologic disposal. This annual report on FY2019 activities includes evaluations of waste form characteristics and waste form performance models, updates to the OWL development, and descriptions of the management processes for the OWL. Updates to the OWL include an updated user's guide, additions to the OWL database content for wastes and waste forms, results of the beta testing and changes implemented from it. Also added are descriptions of the management/control processes for the OWL development, version control, and archiving. These processes have been implemented as part of the full production release of OWL (i.e., OWL Version 1.0), which has been developed on, and will be hosted and managed on, Sandia National Laboratories (SNL) systems. The version control/update processes will be implemented for updates to the OWL in the future. Additionally, another process covering methods for interfacing with the DOE SNF Database (DOE 2007) at Idaho National Laboratory on the numerous entries for DOE-managed SNF (DSNF) has been pushed forward by defining data exchanges and is planned to be implemented sometime in FY2020. The INL database is also sometimes referred to as the Spent Fuel Database or the SFDB, which is the acronym that will be used in this report. Once fully implemented, this integration effort will serve as a template for interfacing with additional databases throughout the DOE complex.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

Separations and Waste Forms Campaign Implementation Plan

This Separations and Waste Forms Campaign Implementation Plan provides summary level detail describing how the Campaign will achieve the objectives set-forth by the Fuel Cycle Reasearch and Development (FCRD) Program. This implementation plan will be maintained as a living document and will be updated as needed in response to changes or progress in separations and waste forms research and the FCRD Program priorities.

Department of Energy↗
DOE OSTI2013

Fabrication and Properties of Technetium-Bearing Pyrochlores and Perovskites as Potential Waste Forms - 13222

Technetium-99 (t{sub 1/2}= 2.13x10{sup 5} years) is important from a nuclear waste perspective and is one of the most abundant, long-lived radioisotopes in used nuclear fuel (UNF). As such, it is targeted in UNF separation strategies such as UREX+, for isolation and encapsulation in solid waste forms for storage in a nuclear repository. We report here results regarding the incorporation of Tc-99 into ternary oxides of different structure types: pyrochlore (Nd{sub 2}Tc{sub 2}O{sub 7}), perovskite (SrTcO{sub 3}), and layered perovskite (Sr{sub 2}TcO{sub 4}). The goal was to determine synthesis conditions of these potential waste forms to immobilize Tc-99 as tetravalent technetium and to harvest crystallographic, thermophysical and hydrodynamic data. The objective of this research is to provide fundamental crystallographic and thermophysical data on advanced ceramic Tc-99 waste forms such as pyrochlore, perovskite, and layered perovskite in support of our current efforts on the corrosion of technetium-bearing waste forms. The ceramic Tc-99-bearing waste forms exhibit good crystallinity. The lattice parameters and crystal structures of the technetium host phases could be refined with high accuracies of ±3, ±4, and ±7 fm (10{sup -15} m), for Nd{sub 2}Tc{sub 2}O{sub 7}, SrTcO{sub 3}, and Sr{sub 2}TcO{sub 4}, respectively. The associated refinement residuals (R{sub Wp}) for the patterns are 4.1 %, 4.7 % and 6.7 %, and the refinement residuals for the individual phases (R{sub Bragg}) are 2.0 %, 2.4 % and 3.9 %, respectively. Thermophysical properties of the oxides SrTcO{sub 3}, Sr{sub 2}TcO{sub 4}, and Nd{sub 2}Tc{sub 2}O{sub 7} were analyzed using AC magnetic susceptibility measurements to further harvest information on the critical temperature (T{sub c}) for superconductivity. In our experiments the strontium technetates, SrTcO{sub 3} and Sr{sub 2}TcO{sub 4}, show superconductivity at rather high critical temperatures of T{sub c} = 7.8 K and 7 K, respectively. On the other hand Nd{sub 2}Tc{sub 2}O{sub 7} did not show any changes in magnetic properties above 3 K. (authors)

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

The Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD) Energy Frontier Research Center (Final Report)

The DOE Office of Environmental Management is responsible for high level nuclear waste that must be safely isolated from humans and the environment for extremely long periods. The waste forms and containers are made of glass, ceramics, and metals. Verified safe disposal requires understanding the fundamental mechanisms of waste form degradation and the design of new waste forms with improved performance, which comprise the goals of the Energy Frontier Research Center known as the Center for the Performance and Design of Nuclear Waste Forms and Containers, WastePD. WastePD was constructed to develop innovative approaches and solutions to those goals through the synergistic interactions of individuals who are experts in the degradation behavior, modeling, and design of glasses, ceramics and metal alloys. WastePD is the first center ever created to address this diverse group of materials in a comprehensive and coordinated manner. The science goals are grouped into three common topics: corrosion mechanisms via advanced characterization, environmental impacts, and materials design. Synergistic interactions in these areas were a key component of WastePD. The fundamental understanding of the degradation mechanisms of the waste forms and containers as well as the development of new materials with improved properties will allow DOE to prevent environmental contamination and to explore totally new repository concepts. WastePD was operational from August 2016 through July 2022, but the DOE support was drastically reduced for the last two years. This final technical report covers the full period of performance. However, much of what was accomplished in the first four years is nicely summarized in a review paper published in 2021, which is appended to this report. Therefore, this final report focuses on the technical findings from the last two years of WastePD activities. Considerable progress was made in the areas of a) the environmental and compositional impacts on the corrosion of borosilicate and aluminosilicate glasses, b) the mechanism of glass corrosion and the structure and evolution of the surface alteration layer, c) the effects of environment and composition on the corrosion of pyrochlore, perovskite, hollandite, and other oxide ceramics, d) the corrosion mechanism of multi-principal element metallic alloys, and e) a new framework for understanding the pitting corrosion of metals.

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

Bentonite-Clay Waste Form for the Immobilization of Cesium and Strontium from Fuel Processing Waste Streams

The physical properties of a surrogate waste form containing cesium, strontium, rubidium, and barium sintered into bentonite clay were evaluated for several simulant feed streams: chlorinated cobalt dicarbollide/polyethylene glycol (CCD-PEG) strip solution, nitrate salt, and chloride salt feeds. We sintered bentonite clay samples with a loading of 30 mass% of cesium, strontium, rubidium, and barium to a density of approximately 3 g/cm 3 . Sintering temperatures of up to 1000°C did not result in volatility of cesium. Instead, there was an increase in crystallinity of the waste form upon sintering to 1000ºC for chloride- and nitrate-salt loaded clays. The nitrate salt feed produced various cesium pollucite phases, while the chloride salt feed did not produce these familiar phases. In fact, many of the x-ray diffraction peaks could not be matched to known phases. Assemblages of silicates were formed that incorporated the Sr, Rb, and Ba ions. Gas evolution during sintering to 1000°C was significant (35% weight loss for the CCD-PEG waste-loaded clay), with significant water being evolved at approximately 600°C.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Advanced Experimental Technique for Radiation Damage Effects in Nuclear Waste Forms: Neutron Total Scattering Analysis

For the past 30 years, the development of durable materials for radionuclide immobilization has been driven by efforts to dispose of wastes generated by the nuclear fuel cycle [National Research Council, ‘Waste Forms Technology and Performance: Final Report’, the National Academies Press, Washington D.C., 2011]. Many materials have been developed, but there still exist large gaps in the knowledge of fundamental modes of waste form degradation in repository environments. An important aspect of waste form science is the behavior of the materials under intense irradiation from decaying actinides and fission products. This irradiation induces a wide range of defects and disorder, the details of which depend on the specific waste form material. At the present time, it is not fully explained how radiation effects will influence the performance of nuclear waste forms and their long-term retention of fission products and actinides under operational conditions. The complex defect behavior and radiation damage must be understood over a range of length scales, from the initial atomic-scale defect structure to the long-range observable material modification. This is particularly challenging and requires advanced characterization techniques. This contribution describes how pair distribution function (PDF) analysis obtained from neutron total scattering experiments can be applied in the research field of waste form science to uniquely characterize radiation effects in a wide range of materials, including crystalline complex oxides and waste glasses. Neutron scattering strength does not have an explicit Z-dependence; this allows access to many low-Z elements, such as oxygen, that cannot be accurately studied with X-rays. In many cases, this can permit a detailed analysis of both cation (often high-Z) and anion (often low-Z) defect behavior. In contrast to traditional crystallography, which relies on long-range order, PDF analysis probes the local defect structure, including changes in site occupation, coordination, and bond distance. This is particularly important when characterizing aperiodic waste glasses with no long-range order at all. In contrast to X-ray characterization which requires very little sample mass (~0.1 mg), neutron characterization (even at state-of-the-art spallation facilities) requires relatively large sample mass (~50 - 100 mg). In conclusion, obtaining this quantity is challenging for studies of irradiated materials, but by tailoring our experimental approach to use high-energy ions (GeV) with very high penetration depth, we are able to produce the required mass.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Solid Secondary Waste Immobilization in Cementitious Waste Forms at the Hanford Site - 19081

During operations of the Hanford Tank Waste Treatment and Immobilization Plant, solid secondary wastes (SSW) will be generated. These materials include HEPA filters, granular activated carbon (GAC), and silver mordenite (AgM). The planned disposal pathway for SSW is through solidification (blending) or encapsulation in a cementitious waste form and then disposal on site at the Hanford Site's Integrated Disposal Facility. Performance assessment evaluations of SSW forms have been performed; however, limited experimental data on simulated SSW is available as input. This paper will cover efforts to fill this gap in experimental data through testing of simulated SSW materials. Two grout formulations were used in the tests: 1) Hanford grout mix 5, a mix of 25 wt% ordinary Portland cement (OPC) and 75 wt% fly ash (FA); and 2) the Cast Stone dry blend of 47 wt% blast furnace slag, 45 wt% FA, and 8 wt% OPC. The sorption (Kd) of potential contaminants (iodide, iodate, technetium) to the grouts and SSW materials was investigated in simulated grout pore water. Waste forms containing GAC and AgM were prepared using the two grout formulations and characterized using scanning electron microscopy energy dispersive X-ray spectroscopy and X-ray diffraction. Acquiring this information will further support the candidacy of cementitious waste forms to be used for disposal of SSW at Hanford. (authors)

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

Fundamental Aspects of Zeolite Waste Form Production by Hot Isostatic Pressing

The direct conversion of iodine-bearing sorbents into a stable waste form is a research topic of interest to the US Department of Energy. The removal of volatile radioactive 129I from the off-gas of a nuclear fuel reprocessing facility will be necessary in order to comply with the regulatory requirements that apply to facilities sited within the United States (Jubin et al., 2012a), and any iodine-containing media or solid sorbents generated by this process would contain 129 I and would be destined for eventual geological disposal. While recovery of iodine from some sorbents is possible, a method to directly convert iodineloaded sorbents to a durable waste form with little or no additional waste materials being formed and a potentially reduced volume would be beneficial. To this end, recent studies have investigated the conversion of iodine-loaded silver mordenite (I-AgZ) directly to a waste form by hot isostatic pressing (HIPing) (Bruffey and Jubin, 2015). Silver mordenite (AgZ), of the zeolite class of minerals, is under consideration for use in adsorbing iodine from nuclear reprocessing off-gas streams. Direct conversion of I-AgZ by HIPing may provide the following benefits: (1) a waste form of high density that is tolerant to high temperatures, (2) a waste form that is not significantly chemically hazardous, and (3) a robust conversion process that requires no pretreatment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Thermodynamic and Microstructural Mechanisms in the Corrosion of Advanced Ceramic Tc-bearing Waste Forms and Thermophysical Properties

Technetium-99 (Tc, t 1/2 = 2.13x10 5 years) is a challenge from a nuclear waste perspective and is one of the most abundant, long-lived radioisotopes found in used nuclear fuel (UNF). Within the Hanford Tank Waste Treatment and Immobilization Plant, technetium volatilizes at typical glass melting temperature, is captured in the off-gas treatment system and recycled back into the feed to eventually increase Tc-loadings of the glass. The aim of this NEUP project was to provide an alternative strategy to immobilize fission technetium as durable ceramic waste form and also to avoid the accumulation of volatile technetium within the off gas melter system in the course of vitrifying radioactive effluents in a ceramic melter. During this project our major attention was turned to the fabrication of chemical durable mineral phases where technetium is structurally bond entirely as tetravalent cation. These mineral phases will act as the primary waste form with optimal waste loading and superior resistance against leaching and corrosion. We have been very successful in fabricating phase-pure micro-gram amounts of lanthanide-technetium pyrochlores by dry-chemical synthesis. However, upscaling to a gram-size synthesis route using either dry- or wet-chemical processing was not always successful, but progress can be reported on a variety of aspects. During the course of this 5-year NEUP project (including a 2-year no-cost extension) we have significantly enhanced the existing knowledge on the fabrication and properties of ceramic technetium waste forms.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Replacement of Fly Ash with Natural Pozzolans in Cementitious Waste Forms

OBJECTIVE Address long-term and emerging issues for Cementitious Waste forms • Future availability of fly ash from coal fired power plants is uncertain • Improve waste form properties • Regionally available ingredients • Reduce cost and embodied Energy • Increase Salt Solution Waste Loading (water : cementitious reagents) in cement waste forms

Hill, Katie A. [Savannah River National Laboratory↗
DOE OSTI2016

Liquid secondary waste. Waste form formulation and qualification

The Hanford Site Effluent Treatment Facility (ETF) currently treats aqueous waste streams generated during Site cleanup activities. When the Hanford Tank Waste Treatment and Immobilization Plant (WTP) begins operations, a liquid secondary waste (LSW) stream from the WTP will need to be treated. The volume of effluent for treatment at the ETF will increase significantly. Washington River Protection Solutions is implementing a Secondary Liquid Waste Immobilization Technology Development Plan to address the technology needs for a waste form and solidification process to treat the increased volume of waste planned for disposal at the Integrated Disposal Facility IDF). Waste form testing to support this plan is composed of work in the near term to demonstrate the waste form will provide data as input to a performance assessment (PA) for Hanford’s IDF.

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

Secondary Waste Form Development and Data Package for Hanford's Integrated Disposal Facility Performance Assessment - 16479

The Hanford Low-Activity Waste (LAW) Vitrification facility is planned to immobilize Hanford tank waste for on-site, near-surface disposal at Hanford's Integrated Disposal Facility (IDF). During this process, liquid and solid secondary wastes will be generated which are also slated for disposal at the IDF. In order to receive authorization to dispose of the waste in the IDF, a Performance Assessment (PA) must be completed in accordance with DOE Order 435.1, Radioactive Waste Management, and its accompanying Manual. The PA must include calculations of potential doses to a member of the public for a 1,000-year period to provide a reasonable expectation that performance objectives will not be exceeded and that the waste will be managed in a manner that is protective of worker and public health and safety, and the environment. Liquid and solid secondary wastes are planned to be immobilized within cementitious waste forms similar to those used elsewhere in the United States and around the world for permanent disposal of low-level radioactive waste (LLW). Data packages and supporting documents are being developed to provide the technical underpinning for the analyses of contaminant releases to the environment from these waste forms for the IDF PA. Traditionally, releases from cementitious waste forms have utilized a diffusion-limited release model using contaminant-specific diffusivities measured in standard leach tests as inputs. More mechanistic modeling techniques are under development to increase the rigor of the PA analyses. In addition, recent testing has shown diffusivities of key contaminants can be reduced by several orders-of-magnitude through optimized formulation of the waste form and use of additives to bind specific contaminants. (authors)

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

Technetium oxidation in slag-based sodium salt waste forms exposed to water and moist Hanford soil - 15514

Several U.S. DOE sites use or plan to use waste forms and/or concrete containment structures for radioactive waste disposal that are designed to have a chemically reducing environment to immobilize selected contaminants such as Tc(VII)O{sub 4}{sup -} and Cr(VI)O{sub 4}{sup 2-}. These waste forms and containment structures are typically deployed in near surface unsaturated oxidizing environments. Consequently, the effect of exposure to air (oxygen) and water containing dissolved oxygen during production, during the period of institutional control, and over the long term period of performance is important for predicting the speciation and mobility of the redox sensitive radioactive and stable contaminants. Both the SRS and Hanford waste streams contain soluble technetium which may require stabilization to meet disposal requirements. Technetium stabilization is a difficult problem because: 1) Tc is soluble and very mobile in the oxidized form typical of near surface environments, and 2) Tc-99 is a long-lived isotope with a half-life of 2.1 E+05 years which places demanding requirements on the engineered barriers and environment to meet current regulatory disposal requirements. A depth-discrete sampling and leaching method approach for measuring contaminant oxidation rate (effective contaminant specific oxidation rate) was used in this study. The method was modified by coating all sides of a cylindrical sample with an impermeable epoxy and cutting a fresh surface 2 to 2.5 cm from the original top surface eliminates sample inhomogeneity as the result of settling as a reason from observed results and provides 1-D soluble ion transport and gas transport information. Soluble Tc was leached from all of the depth-discrete sub-samples from both Tc2-9 and Tc2-10 which strongly suggests that oxygen was present in the entire length of both samples. About 24 mass percent of the Tc in the original sample, was leached (soluble) from sub-samples between 0.8 and 46 mm below the exposed surface of Tc2-9 (exposed to Hanford sediment). The same percent (24%) was leached from the sub-samples between 0.8 and 11 mm below the exposed surface of Tc2-10 (exposed to DI water). This suggests that the rate of oxygen migration into the sample exposed to soil was faster than the rate of migration into the sample exposed to water which is consistent with the more rapid transport of ions through a gas phase as compared to a liquid phase. It is assumed that moisture in the Hanford sediment was not sufficient to completely block the surface pores with respect to gas transport across the soil-waste form boundary. Based on nitrate leaching results for the depth- discrete sub-samples, regions depleted in nitrates were identified from the top surfaces to 9.5 and 3 mm into samples Tc2-9 (exposed to moist Hanford sediment) and Tc2-10 (DI water). Low mass fractions of nitrate were leached from these depth-discrete samples compared to samples further from the exposed surface presumably because a significant portion of the nitrate had already migrated into the soil or water, respectively. Depth-discrete sub-sample leaching results for Na can be interpreted in the same way over the same regions in the two samples tested. In conclusion, leaching monolithic porous cementitious waste forms in water appears to be conservative for non-redox sensitive contaminants. However, leaching data obtained under saturated exposure conditions do not appear to be conservative for redox sensitive contaminants which are easily oxidized. Leaching crushed samples in water still seems to be a conservative approach to estimating the concentrations of soluble contaminants in a waste form. (authors)

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

Experimental Determination of the Speciation, Partitioning, and Release of Perrhenate as a Chemical Surrogate for Pertechnetate from a Sodalite-Bearing Multiphase Ceramic Waste Form

A key component to closing the nuclear fuel cycle is the storage and disposition of nuclear waste in geologic systems. Multiphase ceramic waste forms have been studied extensively as a potential host matrix for nuclear waste. Understanding the speciation, partitioning, and release behavior of radionuclides immobilized in multiphase ceramic waste forms is a critical aspect of developing the scientific and technical basis for nuclear waste management. In this study, we evaluated a sodalite-bearing multiphase ceramic waste form (i.e., fluidized-bed steam reform sodium aluminosilicate [FBSR NAS] product) as a potential host matrix for long-lived radionuclides, such as technetium (99Tc). The FBSR NAS material consists primarily of nepheline (ideally NaAlSiO4), anion-bearing sodalites (ideally M8[Al6Si6O24]X2, where M refers to alkali and alkaline earth cations and X refers to monovalent anions), and nosean (ideally Na8[AlSiO4]6SO4). Bulk x-ray absorption fine structure analysis of the multiphase ceramic waste form, suggest rhenium (Re) is in the Re(VII) oxidation state and has partitioned to a Re-bearing sodalite phase (most likely a perrhenate sodalite Na8[Al6Si6O24](ReO4)2). Rhenium was added as a chemical surrogate for 99Tc during the FBSR NAS synthesis process. The weathering behavior of the FBSR NAS material was evaluated under hydraulically unsaturated conditions with deionized water at 90 C. The steady-state Al, Na, and Si concentrations suggests the weathering mechanisms are consistent with what has been observed for other aluminosilicate minerals and include a combination of ion exchange, network hydrolysis, and the formation of an enriched-silica surface layer or phase. The steady-state S and Re concentrations are within an order of magnitude of the nosean and perrhenate sodalite solubility, respectively. The order of magnitude difference between the observed and predicted concentration for Re and S may be associated with the fact that the anion-bearing sodalites contained in the multiphase ceramic matrix are present as mixed-anion sodalite phases. These results suggest the multiphase FBSR NAS material may be a viable host matrix for long-lived, highly mobilie radionuclides which is a critical aspect in the management of nuclear waste.

Pierce, Eric M↗
DOE OSTI2013

Experimental determination of the speciation, partitioning, and release of perrhenate as a chemical surrogate for pertechnetate from a sodalite-bearing multiphase ceramic waste form

A key component to closing the nuclear fuel cycle is the storage and disposition of nuclear waste in geologic systems. Multiphase ceramic waste forms have been studied extensively as a potential host matrix for nuclear waste. Understanding the speciation, partitioning, and release behavior of radionuclides immobilized in multiphase ceramic waste forms is a critical aspect of developing the scientific and technical basis for nuclear waste management. In this study, we evaluated a sodalite-bearing multiphase ceramic waste form (i.e., fluidized-bed steam reform sodium aluminosilicate [FBSR NAS] product) as a potential host matrix for long-lived radionuclides, such as technetium (99Tc). The FBSR NAS material consists primarily of nepheline (ideally NaAlSiO4), anion-bearing sodalites (ideally M8[Al6Si6O24]X2, where M refers to alkali and alkaline earth cations and X refers to monovalent anions), and nosean (ideally Na8[AlSiO4]6SO4). Bulk X-ray absorption fine structure analysis of the multiphase ceramic waste form, suggest rhenium (Re) is in the Re(VII) oxidation state and has partitioned to a Re-bearing sodalite phase (most likely a perrhenate sodalite Na8[Al6Si6O24](ReO4)2). Rhenium was added as a chemical surrogate for 99Tc during the FBSR NAS synthesis process. The weathering behavior of the FBSR NAS material was evaluated under hydraulically unsaturated conditions with deionized water at 90 ?C. The steady-state Al, Na, and Si concentrations suggests the weathering mechanisms are consistent with what has been observed for other aluminosilicate minerals and include a combination of ion exchange, network hydrolysis, and the formation of an enriched-silica surface layer or phase. The steady-state S and Re concentrations are within an order of magnitude of the nosean and perrhenate sodalite solubility, respectively. The order of magnitude difference between the observed and predicted concentration for Re and S may be associated with the fact that the anion-bearing sodalites contained in the multiphase ceramic matrix are present as mixed-anion sodalite phases. These results suggest the multiphase FBSR NAS material may be a viable host matrix for long-lived, highly mobilie radionuclides which is a critical aspect in the management of nuclear waste.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Product Consistency Testing of Hot Isostatically Pressed Iodine-containing Waste Forms

Silver-exchanged mordenite (AgZ) is currently under evaluation for the capture of iodine from the off-gas streams that are expected to arise during the reprocessing of used nuclear fuel. A final waste form for AgZ loaded with radioactive iodine has not yet been identified. The applicability of hot isostatic pressing (HIPing) to convert iodine-loaded, reduced silver-exchanged mordenite (I-Ag{sup 0}Z) into a suitable waste form is currently being evaluated at Oak Ridge National Laboratory (ORNL). Because production of such a waste form requires little preprocessing of the I-Ag{sup 0}Z, HIPing could prove very attractive from both safety and economic perspectives. It is desirable to produce a waste form with a distinct iodine-containing mineral phase as the major constituent. Such a mineral phase is thought to increase long-term iodine retention and overall stability. Furthermore, the transformation of the material into a known iodine-containing mineral phase 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. For these reasons, the current work has investigated the possibility of converting I-Ag{sup 0}Z into an iodine-containing sodalite, similar to the efforts documented by Sheppard et al. in which they transformed other silver zeolite structures into sodalite through HIPing. Building on our initial work we are now producing hot isostatically pressed waste forms using mixtures of pure sodium mordenite, AgZ, and silver iodide. The composition of these samples is well known, in contrast with the previously used commercially available, binder-containing AgZ, which has a composition that is proprietary and uncharacterized. It is expected that by controlling the initial sample composition, we might be able to control the mineral phases present in the processed waste form. Transformation of the component material into a well-characterized iodine-containing mineral phase would be desirable; however, this is not an absolute requirement for success. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗