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Chong, Saehwa

Publications and source records attributed to Chong, Saehwa.

At least 55 records · Page 3

Iodine Vapor Reactions with Pure Metal Wires at Temperatures of 100–139 °C in Air

In this work, I 2(g) reactions with 11 metal wires (i.e., Al, Ag, Cu, In, Mo, Nb, Ni, Pd, Pt, Sn, Ta) were evaluated at three temperatures (i.e., 100 ± 3°C, 123 ± 4°C, 139 ± 5°C) with exposure times of 24 hours at each temperature. Over these temperatures, some of the metals showed increased mass gain with higher temperatures (i.e., In, Ag, Cu), Sn showed decreased iodine capture at increased temperatures, and most metals (i.e., Mo, Nb, Ni, Pd, Pt, and Ta) showed little to no mass gain at all temperatures. Silver mordenite (AgZ) was used as a standard during these studies and showed a consistent mass gain (m% I ) of 10.6 → 12.8% over this temperature range. The values of mass of iodine captured per mass of starting metal (g g -1 ) ranged widely across the study with the highest values achieved for (in descending order) Sn-T 100°C (4.37), In-T 139°C (3.34), Sn-T 123°C (1.98), In-T 123°C (1.57), Ag-T 139°C (1.19), In-T 100°C (0.97), and Cu-T 139°C (0.71). In some cases, the metal-iodide complex was not stable at the experimental temperature and it was clear some volatility had occurred during the experiment based on discoloration in the vials. These results show that some metals can have extensive reactions with I 2(g) without showing metal-iodide preferences over metal-oxide formation based on thermodynamic predictions. It is possible that materials such as these could be implemented near nuclear facilities to getter I 2(g) in the event of a nuclear accident.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluation of the Generation-2 Dechlorination Apparatus for Treating Salt Wastes

This document satisfies the requirements for two milestones, i.e., M2FT-21PN030103021 and M3FT-21PN030103026, which are described in detail below. Also, details for the work package at the Pacific Northwest National Laboratory (PNNL) are provided below. The goal of this milestone was to demonstrate the generation-2 dechlorination apparatus (G2DA) for removing Cl from chloride-based electrochemical salt simulants. The two salts chosen for this initial study were KCl to simulate a component from the eutectic salt (LiCl is harder to detect with analytical instruments) and CsCl to simulate a fission product chloride that might be present in these types of waste streams. The overall scope of this work included receiving, installing, and testing the G2DA. This new system was designed to address several shortcomings identified with the generation-1 apparatus (G1DA), which are described in detail within this document. The G2DA was designed to address all of these shortcomings. The studies presented in here show that the G2DA worked as intended and will help provide scaled-up batches for additional testing at Argonne National Laboratory.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Polyacrylonitrile Composites of Ag–Al–Si–O Aerogels and Xerogels as Iodine and Iodide Sorbents

Mechanically robust engineered sorbents were constructed by embedding Ag-loaded aerogels or xerogels in a polyacrylonitrile (PAN) matrix at 30 or 50 mass% loadings of gel in PAN. Here, the process for making the base gels as well as the composite materials is described herein, a technology that is very flexible for making hybrid sorbents using various inorganic or organic active sorbents. The PAN-gel composite materials were evaluated for iodine uptake in the form of gaseous iodine [I 2(g) ] at room temperature and at 150°C as well as iodide (I – ) at room temperature from simulated liquid nuclear wastes. The composites show high I 2(g) uptake and high I – uptake (= 93 mass%) in simulated liquid secondary waste spiked with 5 mg L -1 I – . These results demonstrate the utility of such a composite form for iodine removal from contaminated gas and liquid streams.

36 MATERIALS SCIENCE↗

Iodine capture with mechanically robust heat-treated Ag-Al-Si-O xerogel sorbents

Silver-loaded heat-treated aluminosilicate xerogels (Ag-HTX) were evaluated as sorbents for iodine [I2(g)] capture. The heat treatment step was performed to help increase the mechanical integrity of the gels. The synthesized xerogels were characterized using powder X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, Brunauer-Emmett-Teller analysis, gravimetric iodine loading, nanoindentation, and dynamic mechanical analysis. The structural and chemical analyses of Ag-HTX showed uniform distribution of Ag throughout the gel network after Ag-exchange. After I2(g) capture, the AgI crystallites were observed in the sorbent verifying chemisorption as the iodine capture mechanism. Iodine loading of this xerogel was 0.43 g g-1 at 150°C over 1 d and 0.52 g g-1 at 22°C over 33 d. The specific surface area of Ag-HTX was 202 m2 g-1 and decreased to 87 m2 g-1 after iodine loading. The hardness of the heat-treated xerogel was 160 times higher than heat-treated aerogel of the same composition. The heat-treatment process increased the modulus value to 40.77 MPa from 6.99 MPa of as-made xerogel, demonstrating the need for this added step in the synthesis process. These results show that Ag-HTX is a promising sorbent for I2(g) capture with good loading capacity and mechanical stability.

xerogels, aerogels, iodine capture, hardness testi↗

Molecular Iodine Interactions with Metal Substrates: Towards the Understanding of Iodine Interactions in the Environment Following a Nuclear Accident

In order to evaluate the potential impacts to the public from radioiodine in a nuclear event, it is vital to expand our understanding of the interaction of molecular iodine with various surfaces. There are many potential surfaces that iodine could interact with in and around a nuclear facility, including stainless steel. This study, carried out at ambient temperature, pressure and humidity, demonstrates the highly adsorptive nature of molecular iodine on two types of austenitic stainless steel, 304L and 316L. In the authors review of available literature, Fe is the only metal in stainless steel that is assumed to react with gas-phase molecular iodine. By using a novel approach which combines Inductively Coupled Plasma-Optical Emission Spectroscopy (ICP-OES) with surface Energy Dispersive X-ray Spectroscopy (EDS) there is evidence of the formation of metal iodides that have not previously been verified or quantified. Samples exposed to gaseous molecular iodine formed an iodine containing corrosion product visible by scanning electron microcopy (SEM). Evaluation of the metals in the corrosion region using EDS was compared to a water leach of the same samples analyzed using ICP-OES. A comparison of the results provide evidence that the water leachate is representative of the corrosion layer and not the base material. Furthermore, it provides confirmation of metal iodide formation with minor stainless-steel constituents including: FeI2, NiI2, MnI2 and CrI2.

Beck, Chelsie L.↗

Molecular Iodine Interactions with Fe, Ni, Cr, and Stainless Steel Alloys

The adsorption behavior of molecular iodine is important for understanding the spread of radioiodine in a nuclear accident. Prior experiments indicate that, in addition to the interaction with Fe, molecular iodine [i.e., I 2(g) ] also interacts with the next most abundant components of austenitic stainless steel (i.e., Ni, and Cr) at room temperature. Here, we investigate iodine adsorption on Fe, Ni, and Cr while focusing on understanding the variables affecting adsorption as well as the iodine compounds that are formed during adsorption. Scanning electron microscopy and energy-dispersive X-ray spectroscopy were used to characterize the surfaces of exposed metal particles and aid in the understanding of the morphology and chemistry of iodine interactions with the substrates. Inductively coupled plasma optical emission spectroscopy was used to detect low levels of metal iodides and X-ray photoelectron spectroscopy was used to confirm the formation of the metal iodides. The role of environmental factors (e.g., humidity and oxygen content) for iodine adsorption on metal substrates is addressed. The individual metals demonstrated formation of metal iodides for Fe and Ni particles from interaction with I 2(g) . The formation of metal iodides may indicate the affinity of iodine for the respective metal. In this study, the iodine affinities ranked Fe > Ni > Cr as determined by the quantity of chemisorbed iodine. This trend is also supported by the distributions and proportions of metals in the corrosion product of the stainless steels. The exposures without oxygen and humidity indicate the potential of a multistep iodine adsorption process where iodine first attacks the oxide layer and then chemisorbs to the exposed metal.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of ion site occupancies on the unit cell parameters, specific volumes, and densities of M 8 (AlSiO 4 ) 6 X 2 sodalites where M = Li, Na, K, Rb, and Ag and X = Cl, Br, and I

Here, this paper discusses the effects of composition on the unit cell parameter (a), unit cell volume (V), specific volume (v), and density (ρ) of various sodalite compositions including $M^+_8$(AlSiO 4 ) 6 Cl 2 (M = Li, Na, K, Rb, and/or Ag) and Na8(AlSiO 4 ) 6 $X^-_2$(X = Cl, Br, and/or I). Compositional models were developed, and the results show that the models are successful at predicting a, V, and v (and thus ρ) within the compositional range available in the literature. Discussion is included on the correlation between the ionic radii of the alkali metals and halides in the sodalite β-cages and the measured values of a, V, v, and ρ. The data show linear increases in a and ρ with increases in the average ionic radii of the M + and X - constituents (data for v show a linear decrease).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Crystal structures and comparisons of potassium rare-earth molybdates KRE(MoO 4 ) 2 (RE = Tb, Dy, Ho, Er, Yb, and Lu)

Six potassium rare-earth molybdates KRE(MoO 4 ) 2 (RE = Tb, Dy, Ho, Er, Yb, and Lu) were synthesized by flux-assisted growth in K 2 Mo 3 O 10 . The crystal structures were determined using single-crystal X-ray diffraction data. The synthesized molybdates crystallize with the orthorhombic Pbcn space group (No. 60). Trendlines for unit-cell parameters were calculated using data from the current study. The unit-cell parameters a and c increase linearly whereas b decreases with larger RE cations, based on crystal radii. The unit-cell volumes increase linearly and the densities decrease linearly with larger RE cations. The average distances between the RE cations and the nearest O atoms increase with larger cations whereas the average distances of Mo—O and K—O do not show specific trends.

36 MATERIALS SCIENCE↗

Glass waste form options for rare-earth fission products from electrochemical reprocessing

Herein, we describe a first-of-a-kind study where lead tellurite (Pb-Te-O), iron phosphate (Fe-P-O), and lanthanide aluminoborosilicate (LABS) waste forms are evaluated for treating and/or immobilizing waste streams containing high rare-earth (RE) content, e.g., RECl 3 , REOCl, and/or REO x . Results from this study show that NdOCl can be immobilized in 78TeO 2 -22PbO glass at up to 10 mass%. Higher loadings of up to 15 mass% were demonstrated, but with a small fraction of crystallization. Two Fe-P-O glasses produced from either RECl 3 (RE = Nd,Ce) or NdOCl revealed products with very similar properties, demonstrating that the phosphate process can be used to chlorinate a variety of RE-containing waste streams. Two LABS glasses produced from Nd 2 O 3 or NdOCl showed similar properties, but the LABS-NdOCl glass did have some residual Cl present. Characterization is provided for all waste forms including chemical analysis, X-ray diffraction, and bulk density.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Metal–Organic Framework–Polyacrylonitrile Composite Beads for Xenon Capture

Mechanically robust forms of HKUST-1 metal-organic frameworks (MOFs) were fabricated by embedding the MOF in a passive polyacrylonitrile (PAN) matrix at different MOF loadings of 10–90 mass%. Here, the PAN is highly porous and acts as a scaffold that holds the active MOF adsorbent in place for Xe capture. Data presented herein show that the PAN matrix does not notably interfere with the Xe capture process where the Xe capacities scale somewhat linearly with the increase in MOF loading in the composites. Radiation testing of the composites under a gamma flux revealed that they are highly tolerant to these types of radiation fields.

36 MATERIALS SCIENCE↗

Syntheses and Crystal Structures of Rare-Earth Oxyapatites Ca 2 RE 8 (SiO 4 ) 6 O 2 (RE = Pr, Tb, Ho, Tm)

Four different rare-earth oxyapatites of Ca 2 RE 8 (SiO 4 ) 6 O 2 (RE = Pr, Tb, Ho, Tm) were synthesized using a solution-based method followed by drying, calcination, and high-temperature sintering in air. X-ray powder diffraction and Raman spectroscopy were performed on the synthesized oxyapatites. Here, the RE oxyapatites crystallize in the hexagonal space group P6 3 /m with similar unit cell parameters, increasing linearly with larger RE cations. The unit cell volumes increase linearly whereas the densities decrease nonlinearly with larger RE cations. Raman spectra showed intense bands of the symmetric bending and stretching modes of SiO 4 at ~ 400 and 860 cm -1 regions, respectively. The bands generally shifted to higher frequencies with smaller RE cations in the structures.

36 MATERIALS SCIENCE↗

Environmental remediation with functional aerogels and xerogels

Several different types of aerogel and/or xerogel scaffolds have been demonstrated as effective sorbents for the capture and immobilization of radionuclides in gaseous form [e.g., iodine gas or I2(g), Xe] as well as ionic form (e.g., Ce4+, Cs+, I–, IO3-, Rb+, Sr2+, 99Tc7+, and U6+). These scaffolds have unique properties, which include high specific surface areas, high pore volumes, varieties of pore sizes, and functionalities that provide methods for binding radionuclides through physisorption, chemisorption, or a combination thereof. This combination of properties and functionalities make these types of materials ideal scaffolds for use as sorbents for capturing radionuclides. The primary base materials that will be discussed in this chapter include Ag0-functionalized silica aerogels, Ag+-impregnated aluminosilicate aerogels, Ag0-functionalized aluminosilicate aerogels, metal-impregnated (non-Ag) aluminosilicate aerogels and xerogels, sulfide-based aerogels, and carbon-based aerogel composites. For the capture of I2(g), the materials reported herein show some of the highest iodine loadings ever reported for inorganic sorbents. For the capture of ionic species, these materials also show promise to be some of the next generations of materials for active radionuclide remediation. This progress report will describe how these materials are fabricated, the general properties of these materials, as well as an overview of how they have been used for different applications in environmental remediation of radionuclides.

aerogel, xerogel, iodine, radionuclide remediation↗

Gaseous Iodine Sorbents: A Comparison between Ag-Loaded Aerogel and Xerogel Scaffolds

The general properties of aluminosilicate aerogels and xerogels with silver nanoparticles as sorbents for capturing iodine gas [I2(g)] were investigated. The structures, morphologies, compositions, and pore structures of aerogel and xerogel were compared using powder X-ray diffraction (PXRD), scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, as well as specific surface area (SSA) and pore size analyses. The as-made aerogels, xerogels, and heat-treated aerogels were impregnated with Ag by aqueous ion exchange using AgNO3 solutions, and PXRD patterns showed the presence of nanocrystalline Ag0 after Ag-impregnation. Iodine loadings of aerogels and xerogels were 0.33–0.41 g g-1. The Ag-impregnated aerogels without heat-treatment showed an 8 mass% higher iodine loading than Ag-impregnated xerogels and 3 mass% higher than heat-treated Ag-impregnated aerogels. All gels after iodine uptake showed the presence of AgI, indicating chemisorption of iodine to silver. The SSA values of the as-made gels were 419–598 m2 g-1 but decreased significantly to 34–120 m2 g-1 after Ag-impregnation and iodine uptake processes. Overall, changes in physical and chemical properties of aerogels and xerogels after iodine uptake were similar, and the difference in iodine loading capacities of the aerogels and xerogels was not significant while the synthesis process of xerogel is more practical because it does not require supercritical drying.

aerogel, xerogel, iodine capture↗

Iodosodalite synthesis with hot isostatic pressing of precursors produced from aqueous and hydrothermal processes

Iodosodalite powders were synthesized using aqueous and hydrothermal methods, with or without sodium borosilicate glass binders, and then hot isostatically pressed (HIP) at 900 ? and 175 MPa for 3 h to convert into waste forms. After HIPing, the structures, compositions, morphologies, porosities, and leach rates of the aqueous and hydrothermally produced iodosodalite samples were compared. X-ray diffraction patterns of HIPed samples showed that iodosodalite remained as the dominant phase. However, the fraction of the iodosodalite phase decreased after HIPing, indicating decomposition of the iodosodalite structure during the HIP process. Scanning electron microscopy and chemical imaging on the cross sections of HIPed samples showed homogeneous elemental distribution for aqueous-grown iodosodalite, whereas hydrothermally grown iodosodalite samples had more heterogeneity and porosity. The densities of HIPed samples with more glass binder were generally higher than sampled HIPed without binder. The leach tests on samples containing 20 mass% glass binder showed that the iodine dissolution rate of HIPed hydrothermally grown iodosodalite was about 4 times higher than iodosodalite by aqueous method. This study provides alternative techniques for immobilizing iodine-streams in iodosodalite waste forms.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Dehydration synthesis and crystal structure of terbium oxychloride, TbOCl

Terbium oxychloride, TbOCl, was synthesized via a simple heat-treatment of TbCl3·6H2O. The structure was determined using X-ray powder diffraction (XRD) data. The TbOCl compound crystallizes within the tetragonal P4/nmm space group, and its crystal structure is composed of alternating layers of (TbO)n and n Cl- anions. The unit cell parameters, volume, and density were compared to the literature data of other isostructural rare-earth oxychlorides in the P4/nmm space group and showed a good agreement when fitted to the calculated trendlines.

oxychloride, rare-earth oxyhalide, powder diffract↗

Evaluation of Getter Metals in Na–Al–Si–O Aerogels and Xerogels for the Capture of Iodine Gas

In this paper, sodium aluminosilicate aerogels and xerogels were evaluated as scaffolds for a variety of different getters including: Ag + , Cs + , Cu 2+ , Fe 3+ , K + , Li + , Rb + , Sb 3+ , Sn 2+ , and Sn 4+ . The exchange capacities varied widely from a near complete exchange in the case of Ag + to much lower exchange levels for some of the Sn compounds [i.e., colloidal SnO 2 , Sn(II) acetate, Sn(IV) acetate]. Several of the additives showed great promise at allowing for high iodine loadings in the base materials including the following: AgNO 3 , colloidal SnO 2 , Sn(II) acetate, Sn(IV) acetate, Cu(NO 3 ) 2 , and CuSO 4 . From the standpoint of iodine uptake as a function of getter loading, the Sn4+ showed the most promise with a getter utilization (mass of iodine divided by mass of Sn, in atomic%) of 8.4, a chemical uptake of 60.7 mass% (oxygen excluded), and an mI $m_s^{-1}$ value of 0.881; these are some of the highest values reported to date for inorganic iodine sorbents.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗