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DOE OSTI2017

Preparation, Performance and Mechanism of Tc and I Getters in Cementitious Waste Forms - 17124

Cementitious waste forms offer a low temperature, cost effective technology for the solidification of liquid wastes. At the Department of Energy Hanford Site, 99-Tc and 129-I are radionuclides contained within low activity waste (LAW) which contribute significantly to environmental impacts associated with clean-up of the site. Cast Stone, a cementitious waste form comprised of 47 wt% blast furnace slag, 45 wt% fly ash and 8 wt% ordinary Portland cement, has undergone investigation as a possible candidate technology for the solidification of LAW. In screening tests using EPA Method 1315 leach testing of various mixes of Cast Stone with simulated LAW, Tc observed effective diffusivities (Dobs) had an average of 5.3 x 10-11 cm{sup 2}/s and I Dobs had an average of 5.7 x 10-9 cm{sup 2}/s. From these measurements, an opportunity exists to improve retention of Tc and I by Cast Stone. One approach to accomplish this is through the incorporation of Tc and I getters to selectively sequester Tc and I in the waste stream and eventual waste form. Initial testing conducted at PNNL identified potassium metal sulfide (KMS-2) and Sn(II)-apatite (Sn-A) as the strongest performing Tc getters and silver exchanged zeolite (Ag-Z) as the top performing I getter. This research also demonstrated that the Tc and I getters, when added to solution simultaneously, can have deleterious interactions with one another and lower the Tc and I removal levels. However, these interactions can be overcome through sequential treatment of solution with the getters. Cast Stone samples were fabricated using a 6.5 M Na average LAW simulant spiked with Tc and I with the addition of various combinations of Tc and I getters. Through EPA Method 1315 and Method 1313 testing it was found that the KMS-2 Tc getter was most successful at lowering Tc Dobs. The I getters were not effective, as apparent interference from sulfide components of the waste form may have led to dissociation of the AgI formed by the Ag-Z getter in sequestering the I from solution. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

Decay spectroscopy in the neutron-rich Mo–Ru–Pd region

A leading challenge of nuclear-structure research is to understand the properties of nuclides of extreme isospin. Experiments at radioactive-ion-beam facilities, such as the Facility for Rare Isotope Beams in the US, may answer key questions that address diverse topics including fundamental nuclear physics, stellar nucleosynthesis and nuclear applications. The neutron-rich Mo–Ru–Pd (Z = 42 – 46) nuclides are hypothesised to exhibit triaxial-oblate deformation. We performed an experiment with the Facility for Rare Isotope Beams Decay Station initiator (FDSi) to study the structure and decay properties of nuclides in this region. Over 100 different nuclides have been identified in a preliminary analysis of the data. This work presents a first look at several examples between Rb (Z = 37) and Ag (Z = 47). Performance of the FDSi and methods developed to measure ground-state and excited-state lifetimes are presented, and plans for future work are also discussed.

Allmond, James [ORNL] (ORCID:0000000165338721)↗

DOE OSTI2016

Getter Incorporation into Cast Stone and Solid State Characterizations

Washington River Protection Solutions (WRPS) is collecting relevant available data on waste forms for use as a supplemental immobilization technology, to provide the additional capacity needed to treat low-activity waste (LAW) in Hanford Site tanks and complete the tank waste cleanup mission in a timely and cost-effective manner. One candidate supplemental waste form, fabricated using a low-temperature process, is a cementitious grout called Cast Stone. Cast Stone has been under investigation for this application at Pacific Northwest National Laboratory (PNNL) since initial screening tests in FY13. This report is the culmination of work to lower the diffusivities of Tc and I from Cast Stone using getters. Getters are compounds added to a system designed to selectively sequester a species of interest to provide increased stability to the species. The work contained within this report is related to waste form development and testing, and does not directly support the 2017 integrated disposal facility (IDF) performance assessment. However, this work contains valuable information which may be used in performance assessment maintenance past FY17, and in future waste form development. This report on performance characterization of Tc and I getters in Cast Stone fabricated with simulated LAW covers several areas of interest and major findings to WRPS: investigating performance of potassium metal sulfide (KMS-2-SS) and tin (II) apatite (Sn-A) as Tc getters when incorporated into Cast Stone; investigating performance of silver exchanged zeolite (Ag-Z) and argentite (Arg) as I getters when incorporated into Cast Stone; utilizing sequential addition of Tc and I getters to overcome any deleterious interactions between the getters in solution; determining, for the first time, Tc distribution within the cured Cast Stone and its evolution during leaching; and performing solid state characterization of getters and Cast Stone samples to support leach test findings and develop a mechanistic understanding of the processes that control Tc and I release into solution.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Comparison of Extended and Accelerated VOG Tests

The reprocessing of used nuclear fuel would release volatile radionuclides into the off-gas streams of a processing plant, including ¹²⁹I. The dissolver off-gas and more dilute vessel off-gas streams (VOG) must both be targeted when mitigating ¹²⁹I environmental release because each contains some amount of iodine. Iodine-129 will likely be found as elemental iodine (I₂) and methyl iodide (CH₃I) in these off-gas streams. Reduced silver-exchanged mordenite (AgZ or Ag⁰Z) has been investigated as a potential sorbent for iodine abatement and is studied here under prototypic VOG conditions. Because of the relatively low iodine abundance and high flow rates of the VOG, total iodine concentrations are expected to be in the parts per billion range. Thus, VOG experiments need to run for extended durations at low concentrations to reach sorbent saturation. Because the sorbent will be exposed to oxidizing gas streams for extended periods of time, aging effects and sorbent degradation need to be considered when designing a sorbent-based abatement system. Three sets of experiments were performed with the aim of determining how the adsorption of iodine by AgZ is affected by differing test durations and gas compositions. The first tested the capacity of sorbent aged for 8 months under a humid air stream. The second tested differences in sorbent capacity and mass transfer zone (MTZ) length during high-concentration (1200 ppb v ) CH₃I loading in a humid nitrogen gas (N₂) stream and a humid air gas stream over 28 days. The third tested sorbent capacity and MTZ length during low concentration (< 200 ppb v ) CH₃I and I₂ loading in a humid air stream over 9 months. The results of these tests suggest that AgZ capacity drops by ~50% after 1 month of aging, by ~60% after 2 months of aging, and then does not continue to decrease significantly at up to 8 months of aging. One-month aging tests that compared N₂ and air as the gas stream diluent resulted in similar maximum loading capacities and overall loading curves, indicating that the effects of aging cannot be mitigated by avoiding air as the balance gas. The 9-month extended VOG tests did not result in clear sorbent saturation at the inlet, but it can be inferred using an assumption of a maximum capacity of 45 mg I/g AgZ. Applying this assumption, then the MTZ of CH₃I is 12.8 cm, and the MTZ of I₂ is 12.4 cm. These results are similar to previous tests. Comparisons to tests completed at Idaho National Laboratory suggest that the CH₃I MTZ may be dependent on concentration. Future work should re-evaluate the design of the VOG iodine capture system with this updated data and should seek to understand fundamental characteristics of CH₃I adsorption by AgZ, such as the effect of concentration, gas velocity, and gas composition.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Solid Sorbent Cost Sensitivity Analysis: A Framework for UNF Reprocessing Sorbent Cost Comparison

Solid sorbents have been the subject of research and development across the U.S. Department of Energy national laboratory complex for many years. They are generally accepted as a safer alternative to cryogenic distillation for noble gas capture, and they present an easier pathway in development of long-term waste forms after iodine capture. As more types of sorbents have been proposed for capture of volatile radionuclides, it has become necessary to compare them based on performance and cost criteria. This report details cost and performance information for three promising sorbents and provides a cost sensitivity analysis. The goal of this analysis is to establish a framework which can be utilized to directly compare future sorbents, with differing properties, to the sorbents discussed in this report. Direct comparison is instrumental to making informed decisions to efficiently guide research and minimize laborious detours. In all cases, sorbent capacity is a major cost driver as it influences the mass of sorbent, operational footprint, and disposal cost requirements., However, sorbent price can greatly increase the cost of a capture technology. For sorbents used in krypton capture, the purity of krypton released to storage is the highest cost driver.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗