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Chong, Saehwa

Publications and source records attributed to Chong, Saehwa.

At least 19 records

Impact of Crystalline Phases on Low-Activity Waste Glass Durability: Insights from PCT and VHT

During vitrification of nuclear wastes, slow cooling along the container centerline promotes crystalline phase formation, which can alter residual glass composition and reduce chemical durability. This study investigates the effects of crystalline phases on the chemical durability of low-activity waste (LAW) borosilicate glasses using the product consistency test (PCT) and vapor hydration test (VHT) on container centerline cooled (CCC) samples. A preliminary model (R2 = 0.88) was developed to predict CCC PCT responses based on glass composition, PCT data from quenched glasses, and measured crystal fractions. Using the latest LAW glass dataset, the feasibility of predictive modeling is evaluated, limitations in current data and methods are identified, and challenges for improving model accuracy are discussed to guide future data collection and model development.

borosilicate glass↗

Low Activity Waste Glass Optimization with Property Models from Machine Learning, Part 2: Experimental Validation and Active Learning

The United States Department of Energy is responsible for managing legacy nuclear waste stored in underground tanks at the Hanford Site. To treat the waste, it is planned as the current baseline to separately vitrify low-activity waste (LAW) and high-level waste fractions. Previously, machine learning (ML) based glass property models (e.g., chemical durability, viscosity, electrical conductivity and SO3 solubility) were developed with prediction uncertainties. A waste glass optimization approach was then established to enable the capability of using these ML models in LAW glass formulation. In this study, the previous ML models were first experimentally validated, and the results were incorporated back into the database to update the ML models. The updated models and formulations showed increased waste loading while reducing the failure rate, demonstrating improved predictive accuracy, reduced uncertainties, and the effectiveness of active learning in guiding high-dimensional, nonlinear LAW glass design. This represents the first experimental validation of ML based LAW glass formulation, with practical benefits such as higher waste loading, shorter mission duration, and lower operational risk.

Lu, Xiaonan (ORCID:0000000179708148)↗

Pelletization with Spark Plasma Sintering and Characterization of Metal Iodides: An Assessment of Long-Term Radioiodine Immobilization Options

Four promising iodine “getter” materials (Ag, Cu, Bi, and Sn) for radioiodine capture were assessed in their pure metal-iodide (MI x ) pelletized forms to compare relative chemical durabilities. To study chemical durability, commercial MI x compounds of AgI, BiI 3 , BiOI, CuI, and SnI 4 were converted to dense monolithic pellets using spark plasma sintering. Semidynamic leach testing in the form of modified ASTM C1308 tests was then performed on the pellets in two different forms including unmounted (as-pressed) specimens (i.e., “U”) and epoxy-mounted specimens (i.e., “M”) with polished surfaces. The chemical durability results and sample characterizations showed that three of the five MI x compounds tested (i.e., AgI, CuI, and BiOI) displayed moderate to high leach resistances. Further, the remaining two MI x compounds (i.e., BiI 3 and SnI 4 ), which are both desirable iodine waste forms due to their high iodine loading capacities, readily decomposed during leach testing, indicated by crystallographic changes in the specimens as well as large amounts of iodine detected in the leachate solutions. The instabilities of BiI 3 and SnI 4 raise uncertainties for using the base metals/cations (i.e., Bi 0 /Bi 3+ and Sn 0 /Sn 4+ , respectively) as viable getters for radioiodine capture due to likely poor waste form chemical durabilities after capture and consolidation into waste forms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Iodine solid sorbent design: a literature review of the critical criteria for consideration

Designing sorbents for iodine capture in different conditions requires selection and optimization of a large and diverse range of variables. These variables fall into general categories (or features) of sorbent activity, sorbent stability, and the fate of the loaded material in terms of the disposal (waste form) options available. To illustrate, silver-loaded, high-porosity sorbents make for maximized iodine capture and less pressure drop in a column-based sorption system approach, however, this high porosity can lead to less mechanically stable sorbents. Additionally, waste forms containing silver must also be compliant with additional criteria for hazardous waste disposal. Thus, all these aspects must be considered simultaneously when selecting a sorbent for utilization under specific conditions. Information is given for different types of sorbent design considerations for different operating conditions and some emphasis is also given on promising alternatives for silver as the active (chemisorption-based) getter metal. Discussion is given around demonstrated options for waste forms for different metal-iodide compounds.

36 MATERIALS SCIENCE↗

Analytical capabilities for iodine detection: Review of possibilities for different applications

This Review summarizes a range of analytical techniques that can be used to detect, quantify, and/or distinguish between isotopes of iodine (e.g., long-lived 129 I, short-lived 131 I, stable 127 I). One reason this is of interest is that understanding potential radioiodine release from nuclear processes is crucial to prevent environmental contamination and to protect human health as it can incorporate into the thyroid leading to cancer. It is also of interest for evaluating iodine retention performances of next-generation iodine off-gas capture materials and long-term waste forms for immobilizing radioiodine for disposal in geologic repositories. Depending upon the form of iodine (e.g., molecules, elemental, and ionic) and the matter state (i.e., solid, liquid, and gaseous), the available options can vary. In addition, several other key parameters vary between the methods discussed herein, including the destructive vs nondestructive nature of the measurement process (including in situ vs ex situ measurement options), the analytical data collection times, and the amount of sample required for analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synthesis and properties of anhydrous rare-earth phosphates, monazite and xenotime: a review

The synthesis methods, crystal structures, and properties of anhydrous monazite and xenotime (REPO 4 ) crystalline materials are summarized within this review. For both monazite and xenotime, currently available Inorganic Crystal Structure Database data were used to study the effects of incorporating different RE cations on the unit cell parameters, cell volumes, densities, and bond lengths. Domains of monazite-type and xenotime-type structures and other AXO4 compounds (A = RE; X = P, As, V) are discussed with respect to cation sizes. Reported chemical and radiation durabilities are summarized. Different synthesis conditions and chemicals used for single crystals and polycrystalline powders, as well as first-principles calculations of the structures and thermophysical properties of these minerals are also provided.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluating Iodine Immobilization Technologies: Cermets, Polycermets, and Polyhalmets

The work in this report documents the efforts conducted to assess the feasibility of some of the ideas documented in Pacific Northwest National Laboratory invention disclosure reports (IDRs) including: 1) Iodine capture in polyacrylonitrile (PAN)-containing composite sorbents (32451-E). In this work, the composites evaluated included Ag0, Bi0, Cu0, Bi2S3, and Cu2S embedded in PAN. 2) Metal iodide removal from these sorbents through dissolution in dimethyl sulfoxide (DMSO) (32729-E). In this work, PAN dissolution was evaluated for multiple types of sorbents including Ag-Pan, Bi-PAN, Cu-PAN, Bi2S3-PAN, and Cu2S-PAN. 3) Using metal-sulfide sorbents for iodine capture (32647-E). In this work, the composites evaluated under this IDR included Ag2S, Bi2S3, and Cu2S embedded in PAN. 4) Using low-melting metals to immobilize (encapsulate) iodine-loaded and polymer-containing sorbents into polymer-ceramic-metal (called polycermet) or polymer-halide-metal (called polyhalmet) composite waste forms (32625-E). In this work, the iodine-loaded PAN composites included AgI-PAN, BiI-PAN, and CuI-PAN. 5) Ceramic-metal composite waste form synthesis of polymer-containing materials using low-melting metals like bismuth, tin, or bismuth-tin alloys (32537-E). In this work, the metals evaluated included Bi, 58Bi-42Sn eutectic. 6) Cermets for immobilizing commercial sorbents loaded with radioiodine (32806-E). In this work, AgIX (iodine-loaded silver faujasite zeolite) was evaluated in cermet form.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Bonding Environments and Radiation Stabilities of Phosphate Glasses

This report is a summary of some key take-aways presented during the Phosphate Round Table Workshop held in 2020, which was led by PNNL and ANL and funded by DOE-NE. Phosphate glasses have a wide range of commercial and industrial uses due to their unique optical, chemical, and physical properties. They are a candidate material for use as an advanced waste form matrix for immobilizing radioactive waste due to their unique ability to immobilize high fractions of alkali- and sulfur-rich streams in chemically durable glasses. This literature review provides an overview of the structure of phosphate glasses, waste-form related properties of interest (e.g., chemical durability and radiation stability), a summary of how specific composition ratios affect chemical durability (e.g., [Fe]/[P] ratio, [O]/[P] ratio, Fe 2+ /Fe 3+ ratio), as well different ways that phosphate glasses can be affected by radiation. All of these are of interest to the waste form community as phosphate glasses, primarily Fe-P-O glasses, are investigated for usage in immobilizing various types of nuclear waste including U.S. legacy wastes as well as a method for treating salt-based high-level wastes from molten salt reactors and pyroprocessing of used nuclear fuels.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Ceramic–Metal (Cermet) Composites: A Review of Key Properties and Synthesis Methods Focused on Nuclear Waste Immobilization

Here this paper reviews key properties, applications, and examples of ceramic-metal composites (cermets), and metal matrix composites (MMC) with emphasis on their applicability as waste forms for immobilizing nuclear waste. While the literature is mature for vitrified and cementitious radioactive waste forms, cermet materials have not received adequate attention as potential candidates for immobilizing nuclear waste. To promulgate this effort, this review connects cermet and MMC design, such as hardened tools, with the chemistry of radioactive waste streams. A discussion on certification and qualification standards for cermet waste forms, literature gaps, and “how-to” sections on cermet processing techniques. Key parameters discussed include thermal conductivity, chemical durability, and waste loading, as well as examples for metal-containing waste forms. As cermet waste forms gain momentum within the community, this review paper aims ensure the end-of-life nuclear fuel cycle is addressed from a materials and waste disposition perspective.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Glass-bonded ceramic waste forms for immobilization of radioiodine from caustic scrubber wastes

Glass-bonded sodalite composite waste forms have been developed for the immobilization of liquid radioactive wastes resulting from off-gas treatment during aqueous reprocessing of used nuclear fuel, with a particular focus on 129I. The proposed composite waste form is comprised of aluminosilicate ceramic phases containing volatile radionuclides bonded with a glassy matrix. In this work, a suite of ten candidate low-temperature glass binders (ZnO-Bi2O3-based glasses and a Na2O-B2O3-SiO2 glass) were examined. Six glasses were mixed with caustic scrubber waste simulant previously converted into a sodalite-rich material (to provide glass fractions of 10 and 20 wt.%), uniaxially pressed into pellets, and sintered at 350 °C or 550 °C for 8 h in air. Iodine retention after heat treatment was assessed by neutron activation analysis, showing retention of 67-100 % of expected iodine. The aqueous durabilities of the resulting materials were then determined, following the ASTM C1308 standard test, showing iodine releases of 1 to 23 g m-2 after 4 d. The cumulative iodine release for the best performing system (a zinc-bismuth-borate glass binder) was <1 g m-2, and its iodine retention from processing was 67 %. The iodine releases compared favorably with other waste forms. In parallel, this best-performing composition was also consolidated via hot isostatic pressing (HIP) in a stainless-steel canister at 550 °C for 2 h under 100 MPa pressure. The HIPed sample was produced at the ~20 g scale and showed improved densification and minimal reaction with the canister.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Compositional effects on the chemical durabilities of aluminophosphate glasses: A review

Phosphate glasses have a range of applications including as hosts for immobilizing radioactive wastes. Studies have shown that addition of iron and/or aluminum oxides can drastically improve the chemical durability of phosphate glasses where the accurate measurement of chemical durability is one of the most important factors for determining the long-term viability of a given waste form. However, due to inconsistencies with the experimental methods used to generate chemical durability data, comparing and interpreting such data is a tedious task. These variables include the temperature of the test, the specimen form (e.g., coupon, particles), the pressure of the test (e.g., atmospheric pressure, elevated pressure in an autoclave), the exposure time, the exposure medium, and how the loss is documented (e.g., total mass lost, normalized elemental release). This review paper summarizes a large collection of chemical durability tests on aluminophosphate glasses in various studies. In addition, the effects of different oxides on the properties of phosphate glasses are summarized.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Crystalline versus Glassy Nature of Iron Phosphate Waste Forms Subjected to Different Slow Cooling Curves

This report provides experimental details and associated results on the elemental distributions (compositions), crystalline/amorphous phase distributions, and microstructures for iron phosphate reference materials (DPF5-336) made with different cooling curves and starting from different temperatures (i.e., 1050°C and 1200°C). The primary goal of this work was to evaluate the properties of the DPF5- 336 reference material after it was melted and cooled at different rates to simulate the cooling profile of different types of canisters. Crystal fractions across the SCC#2, SCC#3, and SCC#5 samples were all similar ranging in crystal content of 35.66–41.14 mass% with amorphous fractions being the balance (64.34–58.86 mass%, respectively). This shows that the heat treatment profile did not seems to greatly affect either the total crystal content or the phase distributions. The quenched sample was almost completely amorphous (99.55 mass%) with very small peaks identified as Li 3 Fe 2 (PO 4 ) 3 whereas the SCC-treated materials showed peaks for what appear to be ten separate phases present in various concentrations. Another goal of these experiments was to see how the phase distribution affected chemical durability of these waste forms, but that information is being collected at Argonne National Laboratory and will be published in a separate report

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Densification and Immobilization of AgI-Containing Iodine Waste Forms Using Spark Plasma Sintering

Here in this study, porous Ag-xerogel (Ag-Xero), Ag-faujasite (Ag-FAU) zeolite, and Ag-mordenite (Ag-MOR) zeolite sorbents were loaded with iodine gas [I 2 (g)] under saturated conditions at 150 °C for 24 h, followed by densification and consolidation into monolithic waste forms using spark plasma sintering (SPS). For Ag-Xero materials, SPS pellets were made with as-loaded samples, while others were made with preheated (PH; 500 °C for 2 h) samples to help with densification. SPS processing was conducted at 50 MPa under different temperatures (T = 200–800 °C) for different times (t = 0.5–30 min), where eleven AgI-Xero samples, five AgI-FAU, and two AgI-MOR separate samples were produced. The primary goal was to look for the optimum processing parameters for each material to yield pellets with high iodine retentions, high densities, and low porosities while preventing AgI decomposition. The Ag-Xero showed the highest iodine loadings (qe = 470 mg g –1 ) compared to Ag-FAU (qe = 368 mg g –1 ) and Ag-MOR (qe = 108 mg g –1 ). Measured iodine concentrations were the highest in AgI-Xero pellets without PH, followed by AgI-Xero with PH, AgI-FAU, and then AgI-MOR. Silver utilization (I/Ag on a mol % basis) values were in the order of AgI-MOR ≈ AgI-Xero (no PH) > AgI-Xero (PH) > AgI-FAU. Chemical durabilities of SPS-densified AgI-Xero (PH) pellets were very favorable, with lower releases than SPS pellets made from AgI-Xero samples without PH. These results show promise for iodine waste form production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗