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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

DEM and MELT In-Can Vitrification Process for Fukushima Daiichi Water Treatment Secondary Waste - 20034

Fukushima Daiichi Nuclear Power Station was severely damaged by a tsunami induced by the earthquake on March 11, 2011. A large amount of water treatment secondary waste has been generated from the purification work of contaminated water that consists of the water flowing into the reactor building. The Mid and Long-Term Road map specifies that solid waste at Fukushima Daiichi Nuclear Power Station should be stored safely and reasonably according to its characteristics. In order to meet this goal, a versatile treatment solution is needed, and the In-Can vitrification seems to be a suitable solution. The DEM and MELT In-Can vitrification process is being developed and qualified in France to treat waste arising from decommissioning and dismantling operations. This qualification is carried out through the consortium of the DEM and MELT project coordinated by CEA which gathers Orano, ECM technologies and Andra. The DEM and MELT In-Can vitrification process is a robust, simple and versatile in situ vitrification process. It is designed for high or intermediate level waste and is compact enough to be implemented in an existing facility or close to the waste to be treated. It is developed to treat liquid and solid waste, to produce a small amount of secondary waste and to minimize investment and operating costs. The DEM and MELT In-Can vitrification process is also developed with a modular design in order to be adapted to nuclear operators needs and requirements. The In-Can melting process has already been developed and fully qualified by the CEA for Alpha liquid waste and can be rated TRL 7 for this scope. The In-Can vitrification technology is considered as a qualified solution that could be applied for the treatment of waste resulting from the D and D work in Fukushima Daiichi Nuclear Power Station. The feasibility evaluation of the DEM and MELT In-Can vitrification process for Fukushima Daiichi water treatment secondary waste is a project led by Orano, CEA and ANADEC. This R and D project is performed by the funds from the Ministry of Economy, Trade and Industry as The Subsidy Program 'Project of Decommissioning and Contaminated Water Management'. This paper presents the first results of this feasibility evaluation, from the scenarios and glass formulation definition to the industrial implementation feasibility. (authors)

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NASA NTRS1973

Vitrification darkening of rock powders - Implications for optical properties of the lunar surface

Laboratory experiments show that albedoes as low as those on the moon can be produced by vacuum vitrification and associated chemical fractionation of ordinary terrestrial basaltic material. Vitrification is established as an unequivocal process that can account for the low albedo and apparent local darkening with age of the lunar surface. The spectral reflectance curves of glass powders are significantly different than those of the parent rock mineralogy; thus, the presence of ubiquitous glass in lunar surface material complicates compositional determinations by interpretation of spectral reflectance curves. Vitrification of rocks on the moon may highly modify the chemical composition of the resulting glass; thus, glass fragments found in lunar fines cannot be assumed to represent bulk parent rock material. Progressive impact vitrification of lunar surface material throughout the moon's history may have led to a fine-grain, opaque, refractory-rich material we call 'ultimate glass.' This unidentified and, at this point, hypothetical component may exist in dark regolith material; if found, it may be a useful indicator of regolith maturity.

Nash, D. B.↗
DOE OSTI2025

Advanced Computational Modeling of High-Level Waste Vitrification at the Hanford Site

The U.S. Department of Energy (DOE) has selected vitrification for stabilizing legacy tank waste at the Hanford site, where radioactive waste from plutonium production was historically stored in underground tanks. This waste will be separated into low-activity waste (LAW) and high-level waste (HLW) fractions and processed at the Waste Treatment and Immobilization Plant (WTP). At WTP, glass melters are used for the vitrification of radioactive tank waste, transforming it into a stable borosilicate glass form for safe long-term storage. The melter vessel is constructed from highly durable and heat-resistant materials, where the vitrification process occurs. The main regions that are modeled are the melt pool, plenum, cold cap, riser/discharge chamber, and surrounding structure with insulation layers. Forced convection induced by air bubblers at the base of the melter ensure uniform temperature distribution and provide heat to the cold cap layer. The cold cap is a region of reacting batch feed that floats on top of the molten glass and is where the batch-to-glass reactions occur. Joule heating provided by electrodes mounted along the vertical walls of the melter and immersed directly in the glass, generates the necessary heat for the net endothermic conversion processes that occur in the cold cap. The high temperatures, radioactivity, and opaque nature of the glass prevent direct observation inside the melters. Therefore, computational models are essential for providing insight into factors that affect melter throughput. Thermocouples in the plenum provide operators with plenum temperature measurements. Operational adjustments include bubbling rate, voltage supplied to the electrodes, feed adjustments, and glass removal rate. Different computational fluid dynamics (CFD) models have been developed, each serving a specific purpose. There are CFD models of different scale melters, as well as models that capture the two-phase flow interfaces of rising bubbles in the molten glass or models with a simplified molten glass region so that the surrounding structure and plenum can be feasibly incorporated. Pilot-scale melter models have been developed to serve as validation of the methods employed in the simulation of the full-scale WTP melters. Models incorporating resolved bubbling are used to develop momentum source terms to implement into a single phase, multi-region, steady-state flow model that is being validated by measured process parameters such as glass production rate, voltage, input power, plenum temperatures, etc. The resolved bubbling model uses the multiphase volume of fluid approach to model the system with a high-resolution interface capturing scheme to maintain sharp interfaces between the molten glass and the air phase. The suite of CFD models is continually being improved to incorporate more realistic physics and achieve faster turnaround time. For example, an incremental controller is implemented to automatically adjust electrode voltage within the simulation to a molten glass set point temperature of 1150°C. Newer models feature improved meshes to ensure conformal meshes between regions and eliminate unnecessary mesh refinement in areas that are not of interest (such as boundary layers in offgas ports). Instead of explicitly modeling the structural, refractory, and insulation layers of the melter, a thermal resistance approach is used with published correlations used for boundary conditions. The development of robust and efficient CFD models will be instrumental in enabling the WTP to successfully fulfill its mission of safely stabilizing legacy nuclear waste.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
DOE OSTI2020

GeoMelt{sup R} In-Container Vitrification (ICV){sup TM} for Fukushima Daiichi Water Treatment Secondary Wastes - 20212

The Japanese government is supporting development work implemented jointly by Veolia subsidiaries Kurion Japan, K.K., Veolia Nuclear Solutions (VNS), Inc., and Veolia Nuclear Solutions Federal Services, LLC for treating radioactive waste generated from Fukushima Daiichi Nuclear Power Station (NPS) water treatment using the GeoMelt{sup TM} In-Container Vitrification (ICV){sup TM} technology. The initial work consisted of glass formulation and engineering-scale testing which was completed in 2018, in the frame of an IRID (International Research Institute for Nuclear Decommissioning) program as part of a project subsidized by Japan's Ministry of Economy, Trade and Industry (METI). The Fukushima Daiichi NPS Mid- and Long-Term Road-map requires investigation of methods to stabilize solid wastes (and to immobilize radioisotopes in the wastes) generated as a result of emergency response and decommissioning activities. Cooling water treatment has resulted in a significant amount of solid and slurry secondary wastes (mostly adsorbents and ion-exchange materials) which will require processing at some point. GeoMelt{sup R} ICV{sup TM} is a joule-heated melter technology which uses a refractory-lined single-use container combining the melter and disposal container. There is no pouring required nor concerns with refractory corrosion which allows the process to accommodate a wide range of waste chemistries and high waste loadings. The testing described here consisted of three engineering-scale melts, each processing between 212 kg and 240 kg of waste simulants, glass formers, and non-radioactive cesium (Cs) and strontium (Sr) tracers. Continuous isokinetic stack sampling of off-gas emissions was performed for each test in order to calculate Cs and Sr retention in the glass wasteform. Single-pass retention of Cs in the final glass wasteform ranged from 91.46 to 99.30%, and single-pass retention of Sr ranged from 99.76 to 100%. Planned particulate recycle will increase these retention levels. Melt 1 processed a mixture of KUR-EH (a zeolite-based ion-exchange material), simulated Advanced Liquid Processing System (ALPS) Carbonate and Iron Slurries, and glass additives. Melt 2 processed a mixture of KUR-EH, KUR-TSG (a titanate-based adsorbent), and glass additives. Melt 3 processed a mixture of KUR-EH, simulated barium sulfate/iron ferrocyanide sludge (AREVA sludge), and glass additives. Waste loadings for these melts ranged from 70 weight percent (wt%) to 82 wt%. Vitrification produces a waste form much denser than the stored water treatment secondary waste wastes, resulting in significant volume reduction. Volume reductions for the three tests ranged from 74 to 79 vol%. Vitrification produces a chemically durable wasteform. Pacific Northwest National Laboratory (PNNL) tested three glass samples from each engineering-scale melt) by the Materials Characterization Center 1 (MCC-1) test, an international standard leach test of the chemical durability of nuclear waste glasses. PNNL also obtained one U.S. reference glass (EA Glass) and two Japan reference glasses P0798) and tested these under the same MCC-1 conditions (90 deg. C, 10 m-1, DIW, and 7, 14, 28-day) as the GeoMelt{sup R} ICV{sup TM} glasses. The GeoMelt{sup R} ICV{sup TM} glasses exhibited lower total normalized releases and 14- to 28-day normalized release rates than the three reference glasses. These results suggest that the GeoMelt{sup R} ICV{sup TM} glasses have durabilities on par with high-level waste glasses under standard test conditions. Post-melt process sampling and analysis indicated no Cs migration into the melter refractory materials and very little deposition of Cs or Sr onto the melter hood or off-gas piping internals. The results of the testing indicated good Cs retention in the glass, high volume reduction and waste loadings, and excellent chemical durability. These factors are important to minimize treatment costs and to protect workers and the environment. (authors)

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DOE OSTI2023

Alternative reductants for foam control during vitrification of high-iron High Level Waste (HLW) feeds

Foaming during vitrification of radioactive waste in Joule-Heated Ceramic Melters (JHCM) is exacerbated by trapping of evolving gases, such as CO 2 , NO x and O 2 , beneath a viscous reaction layer. Foaming restricts heat transfer during melting. Sucrose is employed as the baseline additive at the Hanford site in Washington State, USA to reduce foaming. Alternative carbon-based reductant additives were explored in simulated, inactive Hanford high-iron HLW-NG-Fe2 feeds, for both their effect on foaming and to give insight to the behaviour of multivalent species in glass melts under different redox conditions. Graphite, coke (93% C), formic acid and HEDTA additives were compared with sucrose, and a feed with no additive. Graphite and coke additions proved most effective in reducing the maximum foam volume by 51 ± 3% and 54 ± 2%, respectively, compared with 24 ± 5% for sucrose. Lower foaming could result in more efficient vitrification in JHCMs. Reductants also affected redox ratios in the multivalent species present in the feed. The order of reduction, Mn 3+ /Mn 2+ > Cr 6+ /Cr 3+ > Ce 3+ /Ce 4+ > Fe 3+ /Fe 2+ was as predicted on the basis of their redox potentials. There is less reduction overall, particularly in the Fe 3+ → Fe 2+ , than predicted by the calculations, attributed to the oxygenated atmosphere of the experiments.

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

Effect of feed composition on the production of off-gases during vitrification of simulated low-activity nuclear waste

During the vitrification of nuclear waste, hazardous and radioactive emissions are generated from the feed-to-glass conversion reactions, in addition to discharges from forced air bubbling and air inleakage. Although the major gaseous emissions are water vapor, nitrogen, and carbon dioxide, various monitored environmental pollutants are also released, such as nitrogen oxides or sulfur dioxide. In addition, reactions between organics and nitrates in the feed may also form products of incomplete combustion such as carbon monoxide and acetonitrile. Although off-gas emissions are commonly measured during both laboratory- and pilot-scale melter testing, no predictive tool is currently available to a priori estimate the composition of gaseous emissions during nuclear waste vitrification. This work forms a basis for the development of such predictive tool by measuring gas evolution from a broad range of simulated low-activity waste melter feeds using evolved gas analysis data and developing correlations between the feed and off-gas compositions. Using reaction stoichiometry and regression analysis, we demonstrate that next to the content of nitrogen and organic carbon in the feed, the gaseous emissions are affected by the feed reduction-oxidation conditions – the more the feed is reduced, the less nitrogen monoxide, and more carbon monoxide and acetonitrile evolves. In conclusion, the results presented in this work provide a first step towards reducing the amount of expensive physical melter testing and the regression analysis provides a simple tool for rapid optimization of feed composition with respect to off-gas composition.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Boron nitride: Novel ceramic reductant for low‐activity waste vitrification

Abstract During vitrification of radioactive wastes, excessive foaming reduces processing rates within melters by hindering heat transfer from the molten glass pool to the reacting melter feed. Formulations of low‐activity waste (LAW) melter feeds, for vitrification at the Waste Treatment and Immobilization Plant at the Hanford Site, conventionally include the addition of sucrose to mitigate excessive foaming by hastening the denitration process. However, incomplete combustion of sucrose produces organics such as acetonitrile (C 2 H 3 N) that may exceed bounding limits of downstream effluent treatment facilities. Using boron nitride (BN) as an alternate reductant to sucrose, in a representative LAW melter feed reduced C 2 H 3 N production by 90% by preventing the low‐temperature sucrose–nitrate reactions. Furthermore, foaming was suppressed due to the higher decomposition temperature of BN than H 3 BO 3 meaning a delayed reaction of a large fraction of boron with the transient glass‐forming melt until above the foam onset temperature, thus reducing the quantity and viscosity of the connected melt and trapping less gas in the foam layer.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

In-Can Incineration and Vitrification Process for the Treatment of Transuranic Wastes - 20035

Technological alpha contaminated wastes are produced by the nuclear fuel cycle management industry, essentially from MOX fuel production units. These Plutonium Contaminated Materials (PCM) contain a mixture of organic, metal and mineral materials, contaminated with uranium, plutonium and americium. One treatment scenario under study is to incinerate the organic materials, melt the metallic fraction and incorporate the mineral fraction (including ashes from organics incineration) into a glass matrix without sorting or pretreatment (grinding for instance). A scale 1 pilot of this PIVIC process (Process for Incineration and Vitrification In Can) has been commissioned in 2018 at the CEA R and D vitrification facility in Marcoule site. A R and D program aiming to demonstrate the feasibility of this process is currently on going. This paper starts with a description of PIVIC process with explanation of the technologies involved. Then, main results of the first year of operation with the technological demonstration goal are presented. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Assessment of the reason for the vitrification of a wall at a hillfort. The example of Broborg in Sweden

It was discovered around 250 years ago that some of the rock material in the walls of some hillforts had been subjected to such high temperature that it had vitrified. This prompted a debate as to the reason for it that is still going on today: did the vitrification come about as a result of hostile action, by accident, or for the purpose of constructing the fort? The present paper is based on the prerequisite that hillforts are different, and therefore should be evaluated individually. All identifiable factors of interest should be included, and especially those that might disprove any alternative. Thus, incentives, competence and petrographic aspects were evaluated for the hillfort Broborg (dated Migration Period, in Sweden A.D. 400 - 550), and it is concluded that the vitrification came about for the purpose of constructing the fort. This capability was lost when mortar was introduced half a millennium later.

42 ENGINEERING↗
DOE OSTI2020

Vitrification of Hanford Tank 241-AP-107 with Recycled Condensate

During the vitrification of nuclear waste at the Hanford Waste Treatment and Immobilization Plant (WTP) – the primary mission of the U.S. Department of Energy Office of River Protection – the offgas condensate generated from the waste-to-glass conversion is currently planned to be concentrated by evaporation in the Effluent Management Facility (EMF). This concentrated condensate can then be recycled back to the incoming waste and vitrified. To test the recycle process, a test apparatus was designed to mimic the EMF evaporator and used to concentrate a volume of condensate that had been previously produced during the vitrification of Hanford tank 241-AP-107 (referred to herein as AP-107) waste in a continuous laboratory-scale melter (CLSM). The test apparatus successfully concentrated the AP-107 condensate by a factor of 10 while retaining over 90 % of the technetium-99 ( 99 Tc), Cs, and I inventory. A second portion of AP-107 waste was retrieved by Washington River Protection Solutions, LLC, given to Pacific Northwest National Laboratory, and combined with the AP-107 condensate concentrate after undergoing solids filtration and cesium removal by ion exchange. This combination served to approximate the recycling action to be performed at the WTP. After the addition of glass-forming chemicals (GFCs), the combined AP-107 waste and AP-107 condensate concentrate were processed in the CLSM to produce a glass, called AP-107-1R, that was designed to satisfy the WTP baseline requirements (Kim et al. 2012). During the 8.87 hours of processing, 7.27 kg of AP-107-1R glass were produced for an average glass production rate of 1739 kg m 2 d -1 . Compared to the previous run in the CLSM without recycled condensate, the run with the recycle had a greater average glass production rate, but the rate was within the potential range of variability when processing melter feeds with similar composition in the CLSM. The glass produced from the AP-107 recycle run in the CLSM was within 10 % of the target AP-107-1R glass composition with respect to the primary glass components. Analysis of the minor component impurities revealed that their content in the glass product had approached their nominal target after 2 turnovers of the glass inventory in the CLSM while the activity of the minor radionuclides was retained in the glass product. The 99 Tc and total cesium content in the combined AP-107 waste and recycled condensate were maintained at concentrations expected to be experienced at the WTP. During processing in the CLSM, at discrete sampling time periods, the target 99 Tc/Cs mass ratio in the glass formulation varied from 0.9 to 62.9. Across this range, the Cs retention in the glass ranged from 53 to 60 %, while the retention from the entire runtime totaled 68 %, values which align with Cs retention in other scaled melter systems while processing LAW melter feeds at 99 Tc/Cs mass ratios ranging from 1 to 100. The 99 Tc retention in the glass ranged from 22 to 32 %, primarily due to the cold-cap coverage on the glass melt surface, the area covered by reacting melter feed, varying from ~80 % to ~95 % during processing, demonstrating greater volatility of 99 Tc from the glass while more surface was exposed, as expected based on previous 99 Tc volatility studies.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Vitrification of Hanford Tank Wastes for Condensate Recycle and Feed Composition Changeover Testing

During the vitrification of Hanford Site nuclear waste at the Waste Treatment and Immobilization Plant (WTP), which is a part of the safe and efficient retrieval, treatment, and disposal mission of the U.S. Department of Energy Office of River Protection, the offgas condensate generated from the waste-to-glass conversion is currently planned to be concentrated by evaporation in the Effluent Management Facility (EMF). This concentrated condensate can then be recycled back to the incoming waste and vitrified. To test the recycle process, an apparatus was designed and built to mimic the EMF evaporator and was then used to concentrate a volume of condensate produced during the vitrification of a sample of Hanford tank 241-AP-107 (referred to herein as AP-107) waste in a continuous laboratory-scale melter (CLSM). The concentrated condensate was added to an additional sample of AP-107 waste, to mimic one round of the recycle process, and the combined solution was vitrified, producing a second round of recycle condensate. In the current study, the EMF test apparatus was used to concentrate the second-round recycle condensate under evaporation conditions (at 45 °C and 1.4 psia) designed to emulate EMF operation. The condensate was successfully concentrated by a factor of ~10 while retaining over 95 % of the technetium-99 ( 99 Tc), Cs, and I inventories in the concentrate. Another portion of AP-107 waste was retrieved by Washington River Protection Solutions, LLC (WRPS) and transferred to Pacific Northwest National Laboratory (PNNL), where it was pretreated and then combined with the second-round recycle AP-107 condensate concentrate and glass-forming chemicals (GFCs) to form the two-time recycle AP-107 melter feed, approximating a second round to the recycling action to be performed at the WTP. A portion of AP-105 waste was also retrieved by WRPS and provided to PNNL for pretreatment and combining with GFCs to form AP-105 melter feed. The two-time recycle AP-107 and AP-105 melter feeds were processed consecutively in the CLSM. The CLSM run proceeded for 13.63 hours, producing 9.70 kg of glass for an average glass production rate of 1464 kg m 2 d -1 during the two-time recycle AP-107 feed charging and 1568 kg m 2 d -1 during the AP-105 feed charging. The rate during AP-107 charging was essentially equivalent to the rate when processing no-recycle AP-107 feed and lower than that achieved when processing one-time recycle AP-107 feed. However, all rates were within the potential range of variability when processing melter feeds with similar composition in the CLSM. Likewise, the rate during AP-105 charging was higher than the previous rate processing AP-105, but within the potential CLSM range. The cold-cap characteristics changed from the typically thin AP-107 cold cap to a foamy-edged cold cap as previously seen with AP-105 shortly after transitioning to the AP-105 melter feed. The glass produced during the CLSM run was within 10 % of its target composition for the primary glass components. The CaO and Li 2 O targets varied by more than 1 wt% between the two-time recycle AP-107 and AP-105 glass targets and it took about 2 turnovers of the CLSM glass inventory to reach a relative chemical steady state in the glass for CaO and Li 2 O after the melter feed inputs were switched. The 99 Tc and total cesium content in the melter feeds were maintained at concentrations expected to be experienced at the WTP. During the CLSM run, while processing the two-time recycle AP-107 melter feed at a relative chemical steady state, the 99 Tc/Cs ratio was 10, and 34% of 99 Tc and 74% of Cs were retained in the glass. These values were higher than those measured in the CLSM run with one-time recycle AP-107 melter feed. After the transition to processing the AP-105 melter feed, when the production reached a relative chemical steady state, the 99 Tc/Cs ratio was 77 while 44% of 99 Tc was retained in the glass. The C's retention during this time frame reached 200% due to the excess C's in the glass after the target content decreased to 15% of its initial level in the two-time recycle AP-107 melter feed to the lower target in the Ap-105 melter feed. While iodine was below inductively coupled plasma mass spectrometry analytical reporting limits in the melter feed and glass samples, it was detected in quantities above the analytical reporting limits in the liquid and filter samples collected from the CLSM offgas treatment system. The behavior of iodine in the CLSM offgas treatment system followed a similar pattern to those of 99 Tc and Cs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Vitrification of Hanford Tank Wastes for Condensate Recycle and Feed Composition Changeover Testing (Rev. 1)

During the vitrification of Hanford Site nuclear waste at the Waste Treatment and Immobilization Plant (WTP), which is a part of the safe and efficient retrieval, treatment, and disposal mission of the U.S. Department of Energy Office of River Protection, the offgas condensate generated from the waste-to-glass conversion is currently planned to be concentrated by evaporation in the Effluent Management Facility (EMF). This concentrated condensate can then be recycled back to the incoming waste and vitrified. To test the recycle process, an apparatus was designed and built to mimic the EMF evaporator and was then used to concentrate a volume of condensate produced during the vitrification of a sample of Hanford tank 241-AP-107 (referred to herein as AP-107) waste in a continuous laboratory-scale melter (CLSM). The concentrated condensate was added to an additional sample of AP-107 waste, to mimic one round of the recycle process, and the combined solution was vitrified, producing a second round of recycle condensate. In the current study, the EMF test apparatus was used to concentrate the second-round recycle condensate under evaporation conditions (at 45 °C and 1.4 psia) designed to emulate EMF operation. The condensate was successfully concentrated by a factor of ~10 while retaining over 95 % of the technetium-99 (99Tc), Cs, and I inventories in the concentrate. Another portion of AP-107 waste was retrieved by Washington River Protection Solutions, LLC (WRPS) and transferred to Pacific Northwest National Laboratory (PNNL), where it was pretreated and then combined with the second-round recycle AP-107 condensate concentrate and glass-forming chemicals (GFCs) to form the two-time recycle AP-107 melter feed, approximating a second round to the recycling action to be performed at the WTP. A portion of AP-105 waste was also retrieved by WRPS and provided to PNNL for pretreatment and combining with GFCs to form AP-105 melter feed. The two-time recycle AP-107 and AP-105 melter feeds were processed consecutively in the CLSM. The CLSM run proceeded for 13.63 hours, producing 9.70 kg of glass for an average glass production rate of 1464 kg m 2 d -1 during the two-time recycle AP-107 feed charging and 1568 kg m 2 d -1 during the AP-105 feed charging. The rate during AP-107 charging was essentially equivalent to the rate when processing no-recycle AP-107 feed and lower than that achieved when processing one-time recycle AP-107 feed. However, all rates were within the potential range of variability when processing melter feeds with similar composition in the CLSM. Likewise, the rate during AP-105 charging was higher than the previous rate processing AP-105, but within the potential CLSM range. The cold-cap characteristics changed from the typically thin AP-107 cold cap to a foamy-edged cold cap as previously seen with AP-105 shortly after transitioning to the AP-105 melter feed. The glass produced during the CLSM run was within 10 % of its target composition for the primary glass components. The CaO and Li 2 O targets varied by more than 1 wt% between the two-time recycle AP-107 and AP-105 glass targets and it took about 2 turnovers of the CLSM glass inventory to reach a relative chemical steady state in the glass for CaO and Li 2 O after the melter feed inputs were switched.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2026

Direct vitrification of HLW: evaluation of candidate source tanks

The initial objective of the present work was to review Hanford HLW compositions to identify HLW streams that are good candidates for the HLW direct feed vitrification option. Another objective was to develop and identify HLW glass compositions and glass forming additive blends for vitrification of two HLW streams identified from the review that could be treated with little or no washing or other pretreatment and would be, therefore, good direct feed candidates. The HLW glass compositions and additive blends were developed to maintain high waste loadings, high processing rates, and acceptable product glass properties. This was accomplished through a combination of crucible-scale and DM100 melter system tests.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Nanoscopic structure of borosilicate glass with additives for nuclear waste vitrification

In this report we investigated the nanoscopic structure of borosilicate glasses as a host for high-level radioactive liquid waste (HLLW) in the presence of the additives Na 2 O and CaO/ZnO with and without Li 2 O. These additives have been used to lower the glass melting point, suppress the macroscopic phase separation, and increase the chemical durability of glasses. Small-angle neutron scattering was used to elucidate the effect of the additives on the nanoscopic structure along with macro- and atomic-scale observations obtained using neutron imaging and X-ray diffraction, respectively. The borosilicate glass made without Na 2 O formed a microphase-separated structure of SiO 2 - and B 2 O 3 -rich domains approximately 100 nm in size, and the material was homogeneous at length scales up to millimeters. With the addition of increasing amounts of Na 2 O, the domain spacing decreased. Introducing CaO/ZnO additives induced inhomogeneities in the glass, such as void structures several nanometers in size, although the inhomogeneity was suppressed by the coaddition of Li 2 O. These results provide insights into the performance of host glasses for HLLW vitrification. Incorporating HLLW into glasses is likely to cause changes in the nanoscopic structure of host glasses similar to those revealed here.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Effect of sucrose on the oxidation-reduction conditions and retention of rhenium during vitrification of low-activity waste

Technetium speciation and solubility during nuclear waste vitrification are affected by oxygen partial pressure in the melt. Thus, reducing agents such as sucrose, which are routinely added to nuclear waste feeds to repress foaming, can significantly affect the volatilization of Tc and increase its retention in glass. Using Re as a surrogate for Tc, we measured the effect of sucrose addition to two low-activity waste melter feeds on the Re retention, oxygen partial pressure, and iron redox as functions of temperature. As expected, Re retention in glass increased as the sucrose content increased. Furthermore, this is attributed to sucrose reaction with nitrates and nitrites in the feed. Destruction of nitrates and nitrites reduces the salt phase fraction and thus likely promotes Re diffusion into the glass-forming melt. In agreement with available literature, we discuss that a modest increase in the sucrose content (compared to current practice) can significantly improve the Tc retention without reducing Fe 2+ to metal.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Glass formulation and lab-scale testing of glasses designed for in-can Melter and in-container Vitrification of high-assay low-enriched uranium aqueous polishing Raffinate waste

Glasses were designed for processing a nuclear waste from aqueous polishing of high-assay low-enriched uranium using either In-Can Melter (ICM) or GeoMelt® In-Container Vitrification™ (ICV) technologies, which operate at temperatures of T p ≤ 1100 °C and T p ≤ 1450 °C, respectively. Due to the different operating conditions, the melt and glass properties were optimized differently for each technology. Each glass was designed to optimize for maximum waste loading while simultaneously satisfying processing (e.g., crystallization, viscosity, and conductivity) and product quality (e.g., durability, hazard characteristic, and crystal content) constraints. Here, the raffinate waste contains high nitric acid (4 M) and low total solids (9 g·L -1 ) concentrations. Feed preparation processes were tested to facilitate concentration and nitrate destruction/removal while controlling redox of the melter feed. A successful feed process including sugar addition and spray-drying was performed to generate an adequate melter feed for ICV processing.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Effect of cold cap coverage and emissivity on the plenum temperature in a pilot-scale waste vitrification melter

Integrated computational fluid dynamics (CFD) models are being developed to model the complex physics occurring within the high-level waste melter for vitrification of legacy tank waste at the Hanford site. Here, we present a validation of the integrated CFD model by using data from two experimental runs in a pilot-scale melter. While the model uses several simplifying assumptions (such as constant heat sinks from a cooling jacket and inleakage of ambient air, steady state feed-to-batch conversion heat, and a cold cap model with a simplified shape), it closely predicts the molten glass (1150°C and 1175°C) and plenum temperatures (550°C) obtained from thermocouples during two pilot-scale tests, with an average cold cap coverage of 80%. Additional simulations were performed to explore the sensitivity of the predicted plenum temperatures to variations in cold cap coverage (fraction of melt surface covered by the glass batch) and batch emissivity. The plenum temperature was found to be in the range of 606°C when cold cap coverage decreased from 95% to 70%. Cold cap emissivity had a smaller effect, increasing the plenum temperature by as much as 179°C when cold cap emissivity increased from 0.2 to 0.8. Maintaining a high cold cap coverage without overfeeding is important for a sustained melter operation with high glass throughput. This work provides a tool for achieving that goal in terms of correlating the plenum temperature with the cold cap coverage.

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

Uncertainty propagation and sensitivity analysis for constrained optimization of nuclear waste vitrification

Abstract The vitrification of high‐level waste (HLW) by heating a mixture of glass‐forming chemicals (GFCs) with the waste can be improved using a constrained optimization problem. This study explores how different uncertainty propagation (UP) methods implemented with the optimization process can affect the glass formulation of nuclear waste glasses. UP is the effort of propagating uncertain inputs through a system to understand and quantify output distributions. Uncertainty intervals are crafted from output distributions to inform the optimization algorithm. UP is often implemented with Monte Carlo (MC) sampling for large nonlinear systems, which can be difficult to implement within a constrained optimization algorithm that requires derivative information. Other UP methods often used for optimization under uncertainty (OUU) can be designed to work within an established constrained optimization framework. Methods of UP are evaluated in this study including iterative sampling approaches, first‐order approximations, and surrogate modeling with machine learning (ML). A method of dimensional reduction based on global sensitivity analysis is introduced to support the UP methods for the large dimensionality of the problem. Analytical UP methods able to achieve similar optimums 10 times faster than the baseline MC approach, and produce 93.9% similar output distributions are reported.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗