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DOE OSTI2024

Unveiling the effect of composition on nuclear waste immobilization glasses’ durability by nonparametric machine learning

Abstract Ensuring the long-term chemical durability of glasses is critical for nuclear waste immobilization operations. Durable glasses usually undergo qualification for disposal based on their response to standardized tests such as the product consistency test or the vapor hydration test (VHT). The VHT uses elevated temperature and water vapor to accelerate glass alteration and the formation of secondary phases. Understanding the relationship between glass composition and VHT response is of fundamental and practical interest. However, this relationship is complex, non-linear, and sometimes fairly variable, posing challenges in identifying the distinct effect of individual oxides on VHT response. Here, we leverage a dataset comprising 654 Hanford low-activity waste (LAW) glasses across a wide compositional envelope and employ various machine learning techniques to explore this relationship. We find that Gaussian process regression (GPR), a nonparametric regression method, yields the highest predictive accuracy. By utilizing the trained model, we discern the influence of each oxide on the glasses’ VHT response. Moreover, we discuss the trade-off between underfitting and overfitting for extrapolating the material performance in the context of sparse and heterogeneous datasets.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Overview of Upcoming Process Improvement Efforts at the Saltstone Facilities at the Savannah River Site - 20474

The Saltstone Facilities at the Savannah River Site (SRS) process and dispose of low activity salt solution waste generated by other liquid waste facilities. Today in the Liquid Waste System (LWS), approximately 125 million liters of salt waste remain to be processed. The Saltstone Production Facility (SPF) receives the decontaminated salt waste, which is mixed with dry feeds consisting of cement, fly ash and slag to produce the saltstone. The mixed slurry is pumped to the Saltstone Disposal Units (SDUs) for safe disposal in the Saltstone Disposal Facility (SDF). To support continuous Salt Waste Processing Facility (SWPF) operations at annual processing volumes many times higher than present, significant modifications are required to ensure that the SPF has the capacity to support the throughput of salt waste. These changes include several infrastructure upgrades that are being worked through the Enhanced Low Activity Waste Disposal (ELAWD) project. In addition to infrastructure upgrades, Savannah River Remediation (SRR), the Savannah River Site's Liquid Waste Contractor for the U.S. Department of Energy, has identified a flowsheet improvement opportunity of implementing a cement-free saltstone formulation to eliminate cement from the current three component formulation. This two-component formulation would simplify the procurement, transport, off-loading, and storage of the premix materials, and increase the storage capacity for the individual components. This flowsheet, when implemented, will reduce operational risk and improve throughput necessary to achieve disposal rates necessary for SWPF operations. Research has been completed to confirm the feasibility of this formulation, with the new cement-free flowsheet expected to be implemented in the next few years. Improvements have also been identified downstream of the SPF to increase SDU utilization. Specifically, a concentrated effort has taken place to raise the fill height in SDU 6 to the full disposal height, 13 meters, to maximize the usage of each SDU in support of the liquid waste disposal mission. This improvement has been made through additional thermal modeling and improved process understanding to create a SDU flammability model and control strategy more representative of facility operations. This work will allow for the completion of construction and operational readiness for SDU 7 while filling SDU 6 to ensure there is no lapse in available space once SWPF starts up. A summary of these improvements as they relate to increased throughput will be provided along with associated status. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2016

Thermal Analysis of of Near-Isothermal Compressed Gas Energy Storage System

In this paper, alternative system configurations for a novel Ground-Level Integrated Diverse Energy Storage (GLIDES) system, which can store energy via input of electricity and heat and deliver dispatchable electricity, is presented. The proposed system is low-cost and hybridizes compressed air and pumped hydro storage approaches that will allow for the off-peak storage of intermittent renewable energy for use during peak times. This study reveals that implementing direct-contact low grade heat exchange via sprayed falling droplets to cool the gas during charging (compression) and warm the gas during discharging (expansion) can be achieved through a secondary recirculating loop of liquid. This study shows that if the recirculating liquid loop is pre-conditioned with waste-heat prior to spraying during gas expansion and considering all the round trip conversion losses from standard 120 V 60 HZ electricity input and output with utilization of low grade heat at 90 C the alternative system design leads to a 16% boost in round trip efficiency of the electricity storage to elec = 82% with an energy density of ED = 3.59 MJ/m3.

25 ENERGY STORAGE↗

DOE OSTI2019

Closing the Nuclear Fuel Cycle with a Simplified Minor Actinide Lanthanide Separation Process (ALSEP) and Additive Manufacturing

Expanded low-carbon baseload power production through the use of nuclear fission can be enabled by recycling long-lived actinide isotopes within the nuclear fuel cycle. This approach provides the benefits of (a) more completely utilizing the energy potential of mined uranium, (b) reducing the footprint of nuclear geological repositories, and (c) reducing the time required for the radiotoxicity of the disposed waste to decrease to the level of uranium ore from one hundred thousand years to a few hundred years. A key step in achieving this goal is the separation of long-lived isotopes of americium (Am) and curium (Cm) for recycle into fast reactors. To achieve this goal, a novel process was successfully demonstrated on a laboratory scale using a bank of 1.25-cm centrifugal contactors, fabricated by additive manufacturing, and a simulant containing the major fission product elements. Americium and Cm were separated from the lanthanides with over 99.9% completion. The sum of the impurities of the Am/Cm product stream using the simulated raffinate was found to be 3.2 × 10 –3 g/L. The process performance was validated using a genuine high burnup used nuclear fuel raffinate in a batch regime. Separation factors of nearly 100 for 154 Eu over 241 Am were achieved. All these results indicate the process scalability to an engineering scale.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2016

2016 Billion-Ton Report: Advancing Domestic Resources for a Thriving Bioeconomy (Executive Summary)

We report that consumption of renewable energy in the United States is the highest in history, contributing to energy security, greenhouse gas reductions, and other social, economic, and environmental benefits. The largest single source of renewable energy is biomass, representing 3.9 quadrillion of 9.6 quadrillion British thermal units (Btu) in 2015. Biomass includes agricultural and forestry resources, municipal solid waste (MSW), and algae.

09 BIOMASS FUELS↗

DOE OSTI2018

Public Acceptance of Pre-Commercial Thinning and Energy and Soil Amendment Products from Post-Harvest Residues in Western Forests of the United States

Abstract . The goals of the Waste-to-Wisdom project is to produce bioenergy products and biochar from post-harvest forest residues and thus understanding public acceptance of the forest management and utilizing forest residues for biomass-based products is critical. This research explores the public perceptions of producing bioenergy products and biochar from forest thinning activities in the western Pacific Northwest region. A web-based survey was conducted in Washington, Oregon, and Northern California generating 1,202 responses. Multinomial regression techniques and simulation-based approach were applied to analyze how demographic and socio-economic factors influence public perceptions. People living in less populated areas are more likely to support forest thinning. Higher levels of education and household income also lead to higher levels of support for forest thinning. On the other hand, supports for forest thinning results in supports for using forest residuals to produce bioenergy products. These results suggest that different strategies are necessary to effectively communicate the environmental and ecological benefits of using forest residuals derived from forest thinning activities to produce biomass-based products. Keywords: Environmental Perceptions, Multinomial Logistic Regression, Natural Resource Management, Rural vs. Urban, Simulation-Based Approach.

Agriculture↗

DOE OSTI2016

CRADA/NFE-15-05761 Report: Additive Manufacturing of Isotropic NdFeB Bonded Permanent Magnets

The technical objective of this technical collaboration phase I proposal is to fabricate net shape isotropic NdFeB bonded magnets utilizing additive manufacturing technologies at the ORNL MDF. The goal is to form complex shapes of thermoplastic and/or thermoset bonded magnets without expensive tooling and with minimal wasted material. Two additive manufacturing methods; the binder jet process; and big area additive manufacturing (BAAM) were used. Binder jetting produced magnets with the measured density of the magnet of 3.47 g/cm 3 , close to 46% relative to the NdFeB single crystal density of 7.6 g/cm 3 were demonstrated. Magnetic measurements indicate that there is no degradation in the magnetic properties. In addition, BAAM was used to fabricate isotropic near-net-shape NdFeB bonded magnets with magnetic and mechanical properties comparable or better than those of traditional injection molded magnets. The starting polymer magnet composite pellets consist of 65 vol% isotropic NdFeB powder and 35 vol% polyamide (Nylon-12). The density of the final BAAM magnet product reached 4.8 g/cm 3 , and the room temperature magnetic properties are: Intrinsic coercivity Hci = 8.65 kOe, Remanence Br = 5.07 kG, and energy product (BH) max = 5.47 MGOe (43.50 kJ/m 3 ). This study provides a new pathway for preparing near-net shape bonded magnets for various magnetic applications.

36 MATERIALS SCIENCE↗

DOE OSTI2019

High Performance Computing to Enable Next-Generation Low-Temperature Waste Heat Recovery

US manufacturing industry fails to recover an estimated 900 trillion BTUs of low-temperature waste heat from its processes each year. A grand research challenge has been to develop waste heat recovery technology that can be applied to industrial manufacturing processes and vehicle operations. The Oak Ridge National Laboratory (ORNL)/Eaton research team performed computational research and development to design an innovative direct-contact heat exchanger (DCHE) technology to deliver low-cost, compact, longer-lifetime, high-efficiency waste heat recovery that is optimized for a low-temperature organic Rankine cycle. ORNL resources and expertise in high performance computing (HPC) and multiphase flows were utilized to realize this goal while advancing the fundamental understanding of two-phase, two-immiscible-fluid turbulent flow heat transfer for heat exchangers. In the first stage of the project, a computational fluid dynamics (CFD) model of a DCHE was developed. Verification and limited validation of the numerical solution were performed using experimental data from published literature. To support efforts in verification and validation, two-dimensional CFD models were also developed with the objective of investigating different boundary conditions to reach converged, steady-state solutions.Based on benchmarking efforts, a baseline industry-grade design of a DCHE was developed, which consists of two horizontal pipes of different cross-sectional areas – joined by a converging-diverging nozzle in the middle and relies on a three-phase system with co-current flows for operation. Evaporation of the cold liquid (n-pentane or methanol) by the hot liquid water occurs in the first pipe. The first pipe contains two inlets for liquid water and liquid pentane (or liquid methanol). The second pipe with the larger cross-sectional area serves as a gravity-driven phase-separator. It contains two outlets that are staggered to avoid entrainment of the liquid water phase by the gas phase. This baseline design resulted from several trial-and-error evaluations using two-dimensional CFD models. Confirmatory three-dimensional CFD models were also run for different mass flow rates and inlet temperatures (inlet water temperature ranging from 50°C to 90°C), and efficiency plots were produced to fully characterize the proposed industrial-grade design of the DCHE.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2021

Anaerobic Fungal Mevalonate Pathway Genomic Biases Lead to Heterologous Toxicity Underpredicted by Codon Adaptation Indices

Anaerobic fungi are emerging biotechnology platforms with genomes rich in biosynthetic potential. Yet, the heterologous expression of their biosynthetic pathways has had limited success in model hosts like E. coli. We find one reason for this is that the genome composition of anaerobic fungi like P. indianae are extremely AT-biased with a particular preference for rare and semi-rare AT-rich tRNAs in E coli, which are not explicitly predicted by standard codon adaptation indices (CAI). Native P. indianae genes with these extreme biases create drastic growth defects in E. coli (up to 69% reduction in growth), which is not seen in genes from other organisms with similar CAIs. However, codon optimization rescues growth, allowing for gene evaluation. In this manner, we demonstrate that anaerobic fungal homologs such as PI.atoB are more active than S. cerevisiae homologs in a hybrid pathway, increasing the production of mevalonate up to 2.5 g/L (more than two-fold) and reducing waste carbon to acetate by ~90% under the conditions tested. This work demonstrates the bioproduction potential of anaerobic fungal enzyme homologs and how the analysis of codon utilization enables the study of otherwise difficult to express genes that have applications in biocatalysis and natural product discovery.

60 APPLIED LIFE SCIENCES↗

NASA NTRS1974

Carbon wastewater treatment process

A new powdered-carbon treatment process is being developed for the elimination of the present problems, associated with the disposal of biologically active sewage waste solids, and with water reuse. This counter-current flow process produces an activated carbon, which is obtained from the pyrolysis of the sewage solids, and utilizes this material to remove the adulterating materials from the water. Additional advantages of the process are the elimination of odors, the removal of heavy metals, and the potential for energy conservation.

Humphrey, M. F.↗

NASA NTRS1977

High-temperature, high-power-density thermionic energy conversion for space

Theoretic converter outputs and efficiencies indicate the need to consider thermionic energy conversion (TEC) with greater power densities and higher temperatures within reasonable limits for space missions. Converter-output power density, voltage, and efficiency as functions of current density were determined for 1400-to-2000 K emitters with 725-to-1000 K collectors. The results encourage utilization of TEC with hotter-than-1650 K emitters and greater-than-6W sq cm outputs to attain better efficiencies, greater voltages, and higher waste-heat-rejection temperatures for multihundred-kilowatt space-power applications. For example, 1800 K, 30 A sq cm TEC operation for NEP compared with the 1650 K, 5 A/sq cm case should allow much lower radiation weights, substantially fewer and/or smaller emitter heat pipes, significantly reduced reactor and shield-related weights, many fewer converters and associated current-collecting bus bars, less power conditioning, and lower transmission losses. Integration of these effects should yield considerably reduced NEP specific weights.

Morris, J. F.↗

NASA NTRS1987

Regenerative fuel cell study for satellites in GEO orbit

Summarized are the results of a 12-month study to identify high performance regenerative hydrogen-oxygen fuel cell concepts for geosynchronous satellite application. Emphasis was placed on concepts with the potential for high energy density (W-hr/lb) and passive means for water and heat management to maximize system reliability. Both polymer membrane and alkaline electrolyte fuel cells were considered, with emphasis on the alkaline cell because of its high performance, advanced state of development, and proven ability to operate in a launch and space environment. Three alkaline system concepts were studied. The first, the integrated design, utilized a configuration in which the fuel cell and electrolysis cells are alternately stacked inside a pressure vessel. Product water is transferred by diffusion during electrolysis and waste heat is conducted through the pressure wall, thus using completely passive means for transfer and control. The second alkaline system, the dedicated design, uses a separate fuel cell and electrolysis stack so that each unit can be optimized in size and weight based on its orbital operating period. The third design was a dual function stack configuration, in which each cell can operate in both fuel cell and electrolysis mode, thus eliminating the need for two separate stacks and associated equipment. Results indicate that using near term technology energy densities between 46 and 52 W-hr/lb can be achieved at efficiencies of 55 percent. System densities of 115 W-hr/lb are contemplated.

Levy, Alexander↗

NASA NTRS1994

Regenerative life support systems - why do we need them?

Human exploration of the solar system will include missions lasting years at a time. Such missions mandate extensive regeneration of life support consumables with efficient utilization of local planetary resources. As missions durations extend beyond one or two years, regenerable human life support systems which supply food and recycle air, water, and wastes become feasible; resupply of large volumes and masses of food, water, and atmospheric gases become unrealistic. Additionally, reduced dependency on resupply or self sufficiency can be an added benefit to human crews in hostile environments far from the security of Earth. Comparisons of resupply and regeneration will be discussed along with possible scenarios for developing and implementing human life support systems on the Moon and Mars.

D J Barta↗

NASA NTRS2016

Spacecraft Life Support Systems

This is a general presentation on life support systems utilized for human space exploration. It is intended to serve as an overview.

life support↗

DOE OSTI2016

From Banned to Allowed: Pathway to Sub-seabed HLW Repositories - 16279

For many countries the disposal of high-level radioactive waste (HLW) has been delayed due to a number of factors including the Not-In-My-Backyard (NIMBY) syndrome. Sub-seabed disposal has no NIMBY concerns since the disposal facilities utilize sediments underlying approximately 4000 meters of international waters. The technical feasibility of the concept was demonstrated during a 12-year joint effort of over 200 researchers from 10 different countries. Social pressures to keep the oceans off-limits to most disposal activities resulted in termination of the coordinated international effort. However, the treaty banning the concept mandated a 25-year review frequency covering the latest scientific and technical information germane to the activity. An effort is underway to supply information to the signatories of the treaty, in their native languages, so they can make a fully-informed decision -- whether or not to approve an amendment that would allow sub-seabed disposal if determined to be protective of human health and the environment and permitted in accordance with guidelines provided by the International Atomic Energy Agency (IAEA). The information highlights the environmental and safety aspects of the disposal concept within a sensible global stewardship framework. With an amended treaty to allow sub-seabed HLW repositories, the global outlook for nuclear waste disposal would be altered dramatically: the number of potential disposal facilities scattered around the world could be reduced from over sixty land-based to approximately six (three land-based, three sub-seabed). (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Thermal Characterization of Acid Treated Anion Exchange Resins

Anion exchange is a chemical separation and purification technique in which a solid phase ion exchanging material (i.e., anion exchange resin beads) interchanges its anions with the desired anions from a solution phase. Typical anion exchange resins (e.g., Bio-Rad AG 1-X8 strongly basic anion exchange resin) consist of a polymer resin bead of cross-linked polystyrene with quaternary ammonium functional groups (Figure 1). Anion exchange occurs at the resin functional groups by exchange of the counter ion of the quaternary ammonium (typically chloride or nitrate) for the anionic species of interest. Other resin polymers have been developed—such as cross-linked vinylpyridine/divinylbenzene utilized in Reillex HPQ anion exchange resin—to improve the resins’ resistance against degradation by oxidizing agents, strong acids, and radiation. Anion exchange is performed for the separation of transuranic (TRU) elements throughout the Department of Energy complex. At the Los Alamos National Laboratory (LANL), production scale quantities of these resins are handled at the Chemistry and Metallurgy Research Facility, the Plutonium Facility, and the Transuranic Waste Facility. Spent anion exchange resin will eventually be disposed of as TRU waste. This has prompted concerns regarding its safe disposal under potential hazard scenarios, in particular a thermal excursion of a TRU waste drum. There is a concern that a potential thermal excursion of a TRU waste drum containing anion exchange resin previously contacted with nitric acid may result in energetic side reactions and pressure buildup due to resin degradation by nitric acid and heat. Therefore, the objective of the experiments described in this report was to gather qualitative and quantitative data to support decisions regarding the thermal stability and safe disposal strategy of nitric acid treated anion exchange resins utilized in TRU processing operations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Poly(methylene-co-cyanoguanidine) as an Eco-friendly Nitrogen Fertilizer with Prolonged Activity

Poly(methylene-co-cyanoguanidine), PMCG, is an oligomeric polycation that has found its application in the waste-water treatment as well as in preparation of polyelectrolyte complex microcapsules for biomedical purposes. Considering the nitrogen-rich composition of repeating unit, PMCG may be a valuable polycation utilized as a novel slow-release fertilizer. The aim of this study was to evaluate the potential of PMCG as a nitrogen fertilizer during its 6-month incubation in the soil. Monocotyledonous oat (Avena sativa) and dicotyledonous radish (Raphanus sativus L.) were selected as representative model plants for plant growth test. The effect of PMCG on plant growth and development was dependent on both the PMCG concentration and time of incubation. An increase in the nitrogen amount in green parts of plants demonstrated the uptake of the plant-available form of nitrogen released from PMCG incubated in the soil. This resulted in an increased percentage of fresh matter and shoot height of the tested plants during their exposure to PMCG. Ecotoxicological impact of PMCG in the soil during incubation period against bacteria Allivibrio fischeri and crustacean Heterocypris incongruens was also assessed. PMCG was found as the potential polymer fertilizer that does not require special treatment and can be used as it is for the prolonged release of nitrogen in agriculture.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Frit Recommendation For Sludge Batch 9 Coupled Operation With The Salt Waste Processing Facility

Prior to the processing of Sludge Batch 9 (SB9) with Frit 803 at the Defense Waste Processing Facility (DWPF), assessments and experimental glass work were completed to support SB9 coupled processing with streams from the Actinide Removal Process (ARP) and Modular Caustic Side Solvent Extraction Unit (MCU). This previous work did not address coupled processing with streams from the Salt Waste Processing Facility (SWPF) because the Product Composition Control System (PCCS) models limited the TiO2 concentration in glass to 2 weight percent (wt.%). These high activity streams from SWPF include monosodium titanate (MST) and sludge solids from the Sludge Solids Receipt Tank (SSRT) as well as Cscontaining strip effluent (SE). The SWPF streams are expected to reach TiO2 concentrations in glass greater than 2 wt.% based on an MST strike of 0.4 g MST/L of salt solution. Therefore, revisions to the models contained in PCCS were completed to allow the evaluation of glasses containing greater than 2 wt.% TiO2, but less than 6 wt.%. Since the initial SB9 qualification for ARP-MCU coupled operation, additional Tank 40 analyses have been completed, which served as the basis for an updated projection of the SB9 blend composition in Tank 40. This projection will be used to support SB9 coupled operation with SWPF in 2019. Savannah River Remediation (SRR) has requested that the Savannah River National Laboratory (SRNL) select a second frit to optimize SB9 coupled operation with SWPF. The selected frit would provide operational flexibility by allowing an acceptable waste loading (WL) to be targeted while maintaining an operating window of at least ± 4 percentage points around this target. The objective of this study was to select a second frit based on a paper-study utilizing Measurement Acceptance Region (MAR) assessments with DWPF PCCS. To support these assessments, SRNL developed a new method for rigorous and directed optimization of frit compositions, which allowed for rapid screening and an assessment of a large array of candidate frits, and the ability to simultaneously satisfy the following single and double MST strike operating scenarios.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗