Search NASA⌕ Search

SEARCH · Search NASA

Results for “BOROSILICATE GLASS”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 163 records · Page 9

Waste Management Approach for a Potential Future U.S. Closed Fuel Cycle - 16233

The U.S. Department of Energy, Office of Nuclear Energy has chartered an effort to develop technologies to enable safe and cost effective recycle of commercial used nuclear fuel (UNF) in the U.S. Part of this effort includes the evaluation of exiting waste management technologies for effective treatment of wastes in the context of current U.S. regulations and development of waste forms and processes with significant cost and/or performance benefits over those existing. This study summarizes the results of these ongoing efforts with a focus on the highly radioactive primary waste streams. The primary streams considered and the recommended waste forms include: - Tritium separated from either a low volume gas stream or a high volume water stream. The recommended waste form is low-water cement in high integrity containers. - Iodine-129 separated from off-gas streams in aqueous processing. There are a range of potentially suitable waste forms. As a reference case, a glass composite material (GCM) formed by the encapsulation of the silver Mordenite (AgZ) getter material in a low-temperature glass is assumed. A number of alternatives with distinct advantages are also considered including a fused silica waste form with encapsulated nano-sized AgI crystals. - Carbon-14 separated from LWR fuel treatment off-gases and immobilized as a CaCO{sub 3} in a cement waste form. - Krypton-85 separated from LWR and SFR fuel treatment off-gases and stored as a compressed gas. - An aqueous reprocessing high-level waste (HLW) raffinate waste which is immobilized by the vitrification process in one of three forms: a single phase borosilicate glass, a borosilicate based glass ceramic, or a multi-phased titanate ceramic [e.g., synthetic rock (Synroc)]. - An undissolved solids (UDS) fraction from aqueous reprocessing of LWR fuel that is either included in the borosilicate HLW glass or is immobilized in the form of a metal alloy in the case of glass ceramics or titanate ceramics. - Zirconium-based LWR fuel cladding hulls and stainless steel (SS) fuel assembly hardware that are washed and super-compacted for disposal or as an alternative Zr purification and reuse (or disposal as low-level waste, LLW) by reactive gas separations. - Electrochemical process salt HLW which is immobilized in a glass bonded Sodalite waste form known as the ceramic waste form (CWF). - Electrochemical process UDS and SS cladding hulls which are melted into an iron based alloy waste form. Mass and volume estimates for each of the recommended waste forms based on the source terms from a representative flowsheet are reported. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Optical properties of bimetallic Au-Cu nanocrystals embedded in glass

Highlights: • Bimetallic Au-Cu/Au-Cu sosoloid nanocrystals embedded in glass have been synthesized. • We achieved good size control of the nanocrystals. • The glasses with bimetallic nanoparticles exhibit enhanced for NLO. • The mechanisms on the nonlinear effects of the obtained glasses are discussed. - Abstract: Bimetallic gold-copper and gold-copper solid solutions nanocrystals (NCs) with orthorhombic morphologies were successfully embedded in sodium borosilicate glass; these materials were fabricated via a facile and synthetic sol-gel technique. Microstructural investigations demonstrate that the Au-Cu intermetallic nanostructure is generated in the glass host. Z-scan technique was applied to reveal the third-order nonlinear optical properties of the as-obtained glasses at the wavelength of 800 nm. The as-synthesized glasses exhibit similar nonlinear behaviors with reverse saturation absorption effects and self-focusing performances. The third-order nonlinear susceptibility χ{sup (3)} values were optimized by tuning the sizes of the Au-Cu NCs. The χ{sup (3)} of Au-Cu(1), Au-Cu(2) and Au-Cu(3) measured to be 3.1 × 10{sup −12}, 5.4 × 10{sup −12}, and 4.4 × 10{sup −12} esu for the single-pulse energy of 1 μJ. We have discussed the nonlinear optical mechanism of Au-Cu sodium borosilicate glass that may be due to the quantum confinement effects and surface plasmon resonance effects.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Rhenium Solubility in Borosilicate Nuclear Waste Glass: Implications for the Processing and Immobilization of Technetium-99

The immobilization of 99Tc in a suitable host matrix has proved to be an arduous task for the researchers in nuclear waste community around the world. At the Hanford site in Washington State, the total amount of 99Tc in low-activity waste (LAW) is ~1300 kg and the current strategy is to immobilize the 99Tc in borosilicate glass with vitrification. In this context, the present article reports on the solubility/retention of rhenium, a nonradioactive surrogate for 99Tc, in a LAW borosilicate glass. Due to the radioactive nature of technetium, rhenium was chosen as a simulant because of the similarity between their ionic radii and other chemical aspects. The glasses containing Re (0 – 10,000 ppm by mass) were synthesized in vacuum-sealed quartz ampoules in order to minimize the loss of Re by volatilization during melting at 1000 °C. The rhenium was found to predominantly exist as Re (VII) in all the glasses as observed by X-ray absorption near-edge structure (XANES). The solubility of Re in borosilicate glasses was determined to be ~3000 ppm (by mass) with inductively coupled plasma-optical emission spectroscopy (ICP-OES). At higher rhenium concentrations, some additional material was retained in the glasses in the form of crystalline inclusions that were detected by X-ray diffraction (XRD) and laser ablation-ICP mass spectrometry (LA-ICP-MS). The implications of these results on the immobilization of 99Tc from radioactive wastes in borosilicate glasses have been discussed.

borosilicate glass↗

Vitrification of Inactive Incineration Ash in a Full Industrial Scale In Can Melter - 20502

In the framework of the H2020 THERAMIN project funded by the European Commission, CEA performed a pilot-scale trial consisting of the vitrification of inactive ash (Al, Ca, Si, Zn, Bi, K, Mg, etc.) using the In- Can Melter technology. These ashes were coming from incineration of simulated technological wastes such as cotton, latex, neoprene, polyethylene. The borosilicate glass feasibility was first evaluated at a laboratory scale (10-100 g of glass). The volatile behavior of fly ash was controlled by pelletizing to avoid pipes clogging when performing the pilot scale test. A 10 wt.% inorganic binder was added to obtain cohesive pellets. The glass frit composition was selected and its ratio was fixed at 50 wt.%. After this step, a bench test (1 kg of glass) was done to verify the absence of container corrosion. Finally, it was followed by a pilot scale test (50 kg of glass) with 75,000 ash pellets used. The same glass microstructure and chemical composition were observed at each scale. Typical crystals of apatites (Ca, P), zincochromites (Zn, Cr, Al) and bismuth alloys (Bi, Sb) dispersed into a borosilicate glass matrix were observed. The chemical durability of the wasteform was measured during 28 days in a 90 deg. C water. Although there were durable crystalline phases, the hydrolysis rate of the vitreous part is relatively high because of the B and Na contents. However, leach rate profiles suggest that an alteration layer will form, leading to an alteration rate decrease. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Chemical analysis of simulated high level waste glasses to support stage III sulfate solubility modeling

The U.S. Department of Energy (DOE), Office of Environmental Management (EM) is sponsoring an international, collaborative project to develop a fundamental model for sulfate solubility in nuclear waste glass. The solubility of sulfate has a significant impact on the achievable waste loading for nuclear waste forms within the DOE complex. These wastes can contain relatively high concentrations of sulfate, which has low solubility in borosilicate glass. This is a significant issue for low-activity waste (LAW) glass and is projected to have a major impact on the Hanford Tank Waste Treatment and Immobilization Plant (WTP). Sulfate solubility has also been a limiting factor for recent high level waste (HLW) sludge processed at the Savannah River Site (SRS) Defense Waste Processing Facility (DWPF). The low solubility of sulfate in glass, along with melter and off-gas corrosion constraints, dictate that the waste be blended with lower sulfate concentration waste sources or washed to remove sulfate prior to vitrification. The development of enhanced borosilicate glass compositions with improved sulfate solubility will allow for higher waste loadings and accelerate mission completion.The objective of the current scope being pursued by SHU is to mature the sulfate solubility model to the point where it can be used to guide glass composition development for DWPF and WTP, allowing for enhanced waste loadings and waste throughput at these facilities. A series of targeted glass compositions was selected to resolve data gaps in the model and is identified as Stage III. SHU fabricated these glasses and sent samples to SRNL for chemical composition analysis. SHU will use the resulting data to enhance the sulfate solubility model and resolve any deficiencies. In this report, SRNL provides chemical analyses for the Stage III, simulated HLW glasses fabricated by SHU in support of the sulfate solubility model development.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Indentation cracking behaviour and structures of nanophase separation of glasses

Correlative microscopy is used to compare the performance and nanophase structures of soda–lime–silica, fused silica and borosilicate glasses using Vickers indentation crack analysis and the transmission electron microscopy (TEM) Fresnel contrast method. In this paper, it is found that the observed indentation cracking behaviour is correlated to the nanophase separation structure of these glasses. The so-called "normal" cracking behaviour of soda–lime–silica glass is influenced by its spinodal nanophase separation; while the "anomalous" cracking behaviour of fused silica is due to the uniform single phase structure. Borosilicate glass has a droplet nanophase separation and shows "intermediate" cracking behaviour. Finally, these results indicate that in order to produce low brittleness glasses it is important to control nanophase separation structure of a glass.

36 MATERIALS SCIENCE↗

Iron Phosphate Glass for Vitrifying Hanford AZ102 LAW in Joule Heated and Cold Crucible Induction Melters - 12240

An iron phosphate composition for vitrifying a high sulfate (∼17 wt%) and high alkali (∼80 wt%) Hanford low activity waste (LAW), known as AZ-102 LAW, has been developed for processing in a Joule Heated Melter (JHM) or a Cold Crucible Induction Melter (CCIM). This composition produced a glass waste form, designated as MS26AZ102F-2, with a waste loading of 26 wt% of the AZ-102 which corresponded to a total alkali and sulfate (represented as SO{sub 3}) content of 21 and 4.4 wt%, respectively. A slurry (7 M Na{sup +}) of MS26AZ102F-2 simulant was melted continuously at temperatures between 1030 and 1090 deg. C for 10 days in a small JHM at PNNL and for 70 hours in a CCIM at INL. The as-cast glasses produced in both melters and in trial laboratory experiments along with their canister centerline cooled (CCC) counterparts met the requirements for the Product Consistency Test (PCT) and the Vapor Hydration Test (VHT) responses in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) Contract. These glass waste forms retained up to 77 % of the SO{sub 3} (3.3 wt%), 100% of the Cesium, and 33 to 44% of the rhenium (used as a surrogate for Tc) all of which either exceeded or were comparable to the retention limit for these species in borosilicate glass nuclear waste form. Analyses of commercial K-3 refractory lining and the Inconel 693 metal electrodes used in JHM indicated only minimum corrosion of these components by the iron phosphate glass. This is the first time that an iron phosphate composition was melted continuously in a slurry fed JHM and in the US, thereby, demonstrating that iron phosphate glasses can be used as alternative hosts for vitrifying nuclear waste. The following conclusions are drawn from the results of the present work. (1) An iron phosphate composition, designated as MS26AZ102F-2, containing 26 wt% of the simulated high sulfate (17 wt%), high alkali (80 wt%) Hanford AZ-102 LAW meets all the criteria for processing in a JHM and CCIM. This composition produces a homogeneous glass with a density of 2.80 ± 0.04 g/cm{sup 3} after melting between 1000 and 1050 deg. C for 3 to 5 h. (2) This is the first time that an iron phosphate glass was melted in the JHM continuously for 10 days achieving a specific melting rate of 1010 kg/m2/day and in the CCIM for 70 hrs with a melting rate of 664 kg/m{sup 2}/day. (3) The analyzed (ICP-AES) compositions for all the glasses prepared under several melting conditions are in excellent agreement with the target composition. The variation of melting conditions include: (i) use of small scale/short melting time to large scale/long melting time (300 g to 80 kg, 4 h to 10 days) operations including melting in the JHM and CCIM, (ii) use of dry or wet (slurry) melter feed, (iii) addition of reductant (sugar) in the batch, and (iv) bubbling the melt with air. (4) The chemical durability as measured by PCT and VHT for the quenched and CCC-treated waste forms prepared from laboratory, JHM or CCIM melting exceeds the DOE requirements for LAW. (5) Depending upon the melting time (4 h to 10 days), the average concentration of SO{sub 3} in the MS26AZ102F-2 iron phosphate glass waste form varies from about 1.78 (RSM) to 3.74 (laboratory melt) wt% which corresponds to an SO{sub 3} retention of 41 to 86% when melted between 1030 at 1050 deg. C in air. (6) The retention of SO{sub 3} in the glass was reduced when a reductant (sugar) was added to the slurry. (7) The retention of other problem components like Cesium and Rhenium/Tc-99 is also high; from 92 to 100% for Cs{sub 2}O under different melting conditions, and from 66 to 33% for Re{sub 2}O{sub 7} for melts processed from 3 to 5 hours and up to 10 days. (8) Corrosion tests on Inconel 693 and K-3 refractory at temperatures between 1000 and 1050 deg. C indicate that both materials should be suitable for melting iron phosphate glasses. (9) The viscosity and electrical conductivity of the MS26AZ102F-2 melt are within the acceptable limits for RSM and CCIM processing. (10)This work has shown that iron phosphate compositions are a potential alternative to borosilicate glasses for vitrifying problematic wastes such as Hanford AZ-102 LAW that contains high amounts sulfate and alkali oxides, and that iron phosphate melts such as MS26AZ102F-2 can be processed in the JHM or CCIM. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Production of microchannel plates using nano-scale additive manufacturing

Microchannel plate (MCP) detectors have been the workhorse detector for many applications, including space borne ultra-violet imaging and spectrographic instruments. Recent advances in additive manufacturing (AM) have enabled fabrication of complex structures with nano-scale resolution facilitating the production of highly customizable MCPs. Using AM to produce MCPs potentially has many advantages over traditional fused glass substrates, including better material control (e.g., more robust glasses or ceramics), better control of microscopic features (e.g., unique pore geometries to improve performance), and better control of macroscopic features (e.g., printing precision curved surfaces for focal plane matching). Through a collaboration with industry, national laboratory, and university partners, small format microcapillary array substrates were produced using a standard polymer photoresin. In conclusion, these substrates were functionalized using atomic layer deposition and their performance was compared to current state-of-the-art Pb-glass and borosilicate-glass MCPs.

36 MATERIALS SCIENCE↗

An electromotive force series in a borosilicate glass-forming melt

An electromotive force series for redox couples was defined as a function of oxygen fugacity in a borosilicate melt at 1150 C. The resulting order of relative reduction potentials can be used to estimate the amounts of redox species in glass during processing. The electromotive force series in this melt is comparable to those in other silicate glass-forming melts and in aqueous systems but differs in detail because of interaction of the solvents with individual redox couples.

Schreiber, H. D.↗

RHENIUM SOLUBILITY IN BOROSILICATE NUCLEAR WASTE GLASS IMPLICATIONS FOR THE PROCESSING AND IMMOBILIZATION OF TECHNETIUM-99 (AND SUPPORTING INFORMATION WITH GRAPHICAL ABSTRACT)

The immobilization of 99Tc in a suitable host matrix has proved a challenging task for researchers in the nuclear waste community around the world. At the Hanford site in Washington State in the U.S., the total amount of 99Tc in low-activity waste (LAW) is {approx} 1,300 kg and the current strategy is to immobilize the 99Tc in borosilicate glass with vitrification. In this context, the present article reports on the solubility and retention of rhenium, a nonradioactive surrogate for 99Tc, in a LAW sodium borosilicate glass. Due to the radioactive nature of technetium, rhenium was chosen as a simulant because of previously established similarities in ionic radii and other chemical aspects. The glasses containing target Re concentrations varying from 0 to10,000 ppm by mass were synthesized in vacuum-sealed quartz ampoules to minimize the loss of Re by volatilization during melting at 1000 DC. The rhenium was found to be present predominantly as Re7 + in all the glasses as observed by X-ray absorption near-edge structure (XANES). The solubility of Re in borosilicate glasses was determined to be {approx}3,000 ppm (by mass) using inductively coupled plasma-optical emission spectroscopy (ICP-OES). At higher rhenium concentrations, some additional material was retained in the glasses in the form of alkali perrhenate crystalline inclusions detected by X-ray diffraction (XRD) and laser ablation-ICP mass spectrometry (LA-ICP-MS). Assuming justifiably substantial similarities between Re7 + and Tc 7+ behavior in this glass system, these results implied that the processing and immobilization of 99Tc from radioactive wastes should not be limited by the solubility of 99Tc in borosilicate LAW glasses.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Formic Acid Free Flowsheet Development To Eliminate Catalytic Hydrogen Generation In The Defense Waste Processing

The Defense Waste Processing Facility (DWPF) processes legacy nuclear waste generated at the Savannah River Site (SRS) during production of plutonium and tritium demanded by the Cold War. The nuclear waste is first treated via a complex sequence of controlled chemical reactions and then vitrified into a borosilicate glass form and poured into stainless steel canisters. Converting the nuclear waste into borosilicate glass canisters is a safe, effective way to reduce the volume of the waste and stabilize the radionuclides. Testing was initiated to determine whether the elimination of formic acid from the DWPF's chemical processing flowsheet would eliminate catalytic hydrogen generation. Historically, hydrogen is generated in chemical processing of alkaline High Level Waste sludge in DWPF. In current processing, sludge is combined with nitric and formic acid to neutralize the waste, reduce mercury and manganese, destroy nitrite, and modify (thin) the slurry rheology. The noble metal catalyzed formic acid decomposition produces hydrogen and carbon dioxide. Elimination of formic acid by replacement with glycolic acid has the potential to eliminate the production of catalytic hydrogen. Flowsheet testing was performed to develop the nitric-glycolic acid flowsheet as an alternative to the nitric-formic flowsheet currently being processed at the DWPF. This new flowsheet has shown that mercury can be reduced and removed by steam stripping in DWPF with no catalytic hydrogen generation. All processing objectives were also met, including greatly reducing the Slurry Mix Evaporator (SME) product yield stress as compared to the baseline nitric/formic flowsheet. Ten DWPF tests were performed with nonradioactive simulants designed to cover a broad compositional range. No hydrogen was generated in testing without formic acid.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Closed Fuel Cycle Waste Treatment Strategy

This study is aimed at evaluating the existing waste management approaches for nuclear fuel cycle facilities in comparison to the objectives of implementing an advanced fuel cycle in the U.S. under current legal, regulatory, and logistical constructs. The study begins with the Global Nuclear Energy Partnership (GNEP) Integrated Waste Management Strategy (IWMS) as a general strategy and associated Waste Treatment Baseline Study (WTBS). The tenets of the IWMS are equally valid to the current waste management study. However, the flowsheet details have changed significantly from those considered under GNEP. In addition, significant additional waste management technology development has occurred since the GNEP waste management studies were performed. This study updates the information found in the WTBS, summarizes the results of more recent technology development efforts, and describes waste management approaches as they apply to both a nominal case study and near-term target reprocessing flowsheets. Many of the waste management technologies discussed also apply to other potential flowsheets that involve reprocessing. The report summarizes the waste arising from aqueous reprocessing of a typical light-water reactor (LWR) fuel to separate actinides for use in fabricating metal sodium fast reactor (SFR) fuel and from electrochemical reprocessing of the metal SFR fuel to separate actinides for recycle back into the SFR in the form of metal fuel. The primary streams considered and the recommended waste forms include: • Tritium separated from either a low volume gas stream or a high volume water stream. The recommended waste form is low-water cement in high integrity containers (HICs). • Iodine-129 separated from off-gas streams in aqueous processing. There are a range of potentially suitable waste forms. As a reference case, a glass composite material (GCM) formed by the encapsulation of the silver Mordenite (AgZ) getter material in a low-temperature glass is assumed. A number of alternatives with distinct advantages are also considered including a fused silica waste form with encapsulated nano-sized AgI crystals. • Carbon-14 separated from LWR fuel treatment off-gases and immobilized as a CaCO3 in a cement waste form. • Krypton-85 separated from LWR and SFR fuel treatment off-gases and stored as a compressed gas. • An aqueous reprocessing high-level waste (HLW) raffinate waste which is immobilized by the vitrification process in one of three forms: a single phase borosilicate glass, a borosilicate based glass ceramic, or a multi-phased crystalline synthetic rock (Synroc). • An undissolved solids (UDS) fraction from aqueous reprocessing of LWR fuel that is either included in the borosilicate HLW glass or is immobilized in the form of a metal alloy in the case of glass ceramics or Synroc. • Zirconium-based LWR fuel cladding hulls and stainless steel (SS) fuel assembly hardware that are washed and super-compacted for disposal or as an alternative with high promise the purification and reuse (or disposal as low-level waste, LLW) of Zr by reactive gas separations. • Electrochemical process salt HLW which is incorporated into a glass bonded Sodalite waste form known as the ceramic waste form (CWF). • Electrochemical process UDS and SS cladding hulls which are melted into an iron based alloy waste form. Mass and volume estimates for each of the recommended waste forms based on the source terms from the reference mass balances are reported. In addition to the above listed primary waste streams, a range of secondary process wastes are generated by aqueous reprocessing of LWR fuel, metal SFR fuel fabrication, and electrochemical reprocessing of SFR fuel. These secondary wastes have been summarized and volumes estimated by type and classification. The important waste management data gaps and research needs have been summarized for each primary waste stream and selected waste process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Waste Management Approach for a Potential Future U.S. Closed Fuel Cycle - 16233

The U.S. Department of Energy, Office of Nuclear Energy has chartered an effort to develop technologies to enable safe and cost effective recycle of commercial used nuclear fuel (UNF) in the U.S. Part of this effort includes the evaluation of exiting waste management technologies for effective treatment of wastes in the context of current U.S. regulations and development of waste forms and processes with significant cost and/or performance benefits over those existing. This study summarizes the results of these ongoing efforts with a focus on the highly radioactive primary waste streams. The primary streams considered and the recommended waste forms include: •Tritium separated from either a low volume gas stream or a high volume water stream. The recommended waste form is low-water cement in high integrity containers. •Iodine-129 separated from off-gas streams in aqueous processing. There are a range of potentially suitable waste forms. As a reference case, a glass composite material (GCM) formed by the encapsulation of the silver Mordenite (AgZ) getter material in a low-temperature glass is assumed. A number of alternatives with distinct advantages are also considered including a fused silica waste form with encapsulated nano-sized AgI crystals. •Carbon-14 separated from LWR fuel treatment off-gases and immobilized as a CaCO3 in a cement waste form. •Krypton-85 separated from LWR and SFR fuel treatment off-gases and stored as a compressed gas. •An aqueous reprocessing high-level waste (HLW) raffinate waste which is immobilized by the vitrification process in one of three forms: a single phase borosilicate glass, a borosilicate based glass ceramic, or a multi-phased titanate ceramic [e.g., synthetic rock (Synroc)]. •An undissolved solids (UDS) fraction from aqueous reprocessing of LWR fuel that is either included in the borosilicate HLW glass or is immobilized in the form of a metal alloy in the case of glass ceramics or titanate ceramics. •Zirconium-based LWR fuel cladding hulls and stainless steel (SS) fuel assembly hardware that are washed and super-compacted for disposal or as an alternative Zr purification and reuse (or disposal as low-level waste, LLW) by reactive gas separations. •Electrochemical process salt HLW which is immobilized in a glass bonded Sodalite waste form known as the ceramic waste form (CWF). •Electrochemical process UDS and SS cladding hulls which are melted into an iron based alloy waste form. Mass and volume estimates for each of the recommended waste forms based on the source terms from a representative flowsheet are reported.

Fuel Cycle↗

The effect of Si on the microstructure and mechanical properties of spark plasma sintered boron carbide

Highlights: • Si addition leads to a dense final product at a low sintering temperature. • The added Si preferentially formed SiC and borosilicate glass instead of replacing the chain atoms in boron carbide. • The hardness of our Si-containing boron carbide is 30–35% greater than currently in-use commercial boron carbide plates. - Abstract: Fully dense boron carbide discs were achieved by spark plasma sintering boron carbide powders with 10 wt% silicon. The silicon did not diffuse into boron carbide grains to produce a solid solution of Si-doped boron carbide; instead the silicon reacted with impurities in the starting powder to form β-SiC and borosilicate glass. The resultant new phases facilitated densification of the multiphase ceramic through liquid phase-assisted sintering. The resultant material exhibits improved hardness (34.3 GPa Vikers hardness under 1 kg load) with toughness comparable to both Si-free and commercially available boron carbide.

36 MATERIALS SCIENCE↗

Epsilon Metal Waste Form for Immobilization of Noble Metals from Used Nuclear Fuel

Epsilon metal (ε-metal), an alloy of Mo, Pd, Rh, Ru, and Tc, is being developed as a waste form to treat and immobilize the undissolved solids and dissolved noble metals from aqueous reprocessing of commercial used nuclear fuel. Epsilon metal is an attractive waste form for several reasons: increased durability relative to borosilicate glass, it can be fabricated without additives (100% waste loading), and in addition it also benefits borosilicate glass waste loading by eliminating noble metals from the glass and thus the processing problems related there insolubility in glass. This work focused on the processing aspects of the epsilon metal waste form development. Epsilon metal is comprised of refractory metals resulting in high reaction temperatures to form the alloy, expected to be 1500 - 2000°C making it a non-trivial phase to fabricate by traditional methods. Three commercially available advanced technologies were identified: spark-plasma sintering, microwave sintering, and hot isostatic pressing, and investigated as potential methods to fabricate this waste form. Results of these investigations are reported and compared in terms of bulk density, phase assemblage (X-ray diffraction and elemental analysis), and microstructure (scanning electron microscopy).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Glass-bonded iodosodalite waste form for immobilization of 129I

Immobilization of radioiodine (e.g., 129I, 131I) is an important need for current and future nuclear fuel cycles. For the current work, iodosodalite [Na8(AlSiO4)6I2] was synthesized hydrothermally from metakaolin, NaI, and NaOH. Following hydrothermal treatment, dried unwashed powders were used to make glass-bonded iodosodalite waste forms by heating pressed pellets at 650, 750, or 850 °C with two different types of sodium borosilicate glass binders, i.e., NBS-4 and SA-800. These heat-treated specimens were characterized with X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy, energy dispersive spectroscopy, thermal analysis, porosity and density measurements, neutron activation analysis, and inductively-coupled plasma mass spectrometry. The pellets mixed with 10 mass% of NBS-4 or SA-800 and heat-treated at 750 °C contained relatively high percentage iodine retention (~44-47 % of the maximum iodine loading) with relatively low porosities, while other pellets with higher percentages iodine retention either contained higher porosity or were not completely sintered. ASTM C1308 chemical durability tests of monolithic specimens showed a large initial release of Na, Al, Si, and I on the first day, possibly from water-soluble salt crystals or non-durable amorphous phases. Release rates of Na and Si were higher than for Al and I, probably due to a poorly durable Na-Si-O phase from the glass bonding matrix. The cumulative normalized release of iodine was 12.5 g m-2 for the first 10 1-d exchanges, suggestive of coherent dissolution. The average release rate from 10-24 days during the 7-d exchange intervals was 0.2336 g m-2 d-1.

sodalite, iodosodalite, waste forms, iodine↗