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DOE OSTI2015

Controlled crystallization of salts from nuclear waste solutions - 15235

Crystallization has been proposed as a potential method for removing low-activity salt from nuclear waste solutions. The viability of such a process hinges on the ability to partition formed salt crystals from the waste solution. Good solid-liquid separation is expected if the crystals are large and uniform, thus is important to control the crystallization operation to produce such crystals. This work examines a closed-loop control strategy for producing large salt crystals from a model electrolytic solution. (authors)

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NASA NTRS1975

Energy recovery from solid waste. Volume 1: Summary report

A systems analysis of energy recovery from solid waste which demonstrates the feasibility of several processes for converting solid waste to an energy form is presented. The social, legal, environmental, and political factors are considered and recommendations made in regard to legislation and policy. A technical and economic evaluation of available and developing energy-recovery processes is given with emphasis on thermal decomposition and biodegradation. A pyrolysis process is suggested. The use of prepared solid waste as a fuel supplemental to coal is considered to be the most economic process for recovery of energy from solid waste. Markets are discussed with suggestions for improving market conditions and for developing market stability. A decision procedure is given to aid a community in deciding on its options in dealing with solid waste.

Source record↗

DOE OSTI2016

WTP Waste Feed Qualification: Glass Fabrication Unit Operation Testing Report

The waste feed qualification program is being developed to protect the Hanford Tank Waste Treatment and Immobilization Plant (WTP) design, safety basis, and technical basis by assuring waste acceptance requirements are met for each staged waste feed campaign prior to transfer from the Tank Operations Contractor to the feed receipt vessels inside the Pretreatment Facility. The Waste Feed Qualification Program Plan describes the three components of waste feed qualification: 1. Demonstrate compliance with the waste acceptance criteria 2. Determine waste processability 3. Test unit operations at laboratory scale. The glass fabrication unit operation is the final step in the process demonstration portion of the waste feed qualification process. This unit operation generally consists of combining each of the waste feed streams (high-level waste (HLW) and low-activity waste (LAW)) with Glass Forming Chemicals (GFCs), fabricating glass coupons, performing chemical composition analysis before and after glass fabrication, measuring hydrogen generation rate either before or after glass former addition, measuring rheological properties before and after glass former addition, and visual observation of the resulting glass coupons. Critical aspects of this unit operation are mixing and sampling of the waste and melter feeds to ensure representative samples are obtained as well as ensuring the fabrication process for the glass coupon is adequate. Testing was performed using a range of simulants (LAW and HLW simulants), and these simulants were mixed with high and low bounding amounts of GFCs to evaluate the mixing, sampling, and glass preparation steps in shielded cells using laboratory techniques. The tests were performed with off-the-shelf equipment at the Savannah River National Laboratory (SRNL) that is similar to equipment used in the SRNL work during qualification of waste feed for the Defense Waste Processing Facility (DWPF) and other waste treatment facilities at the Savannah River Site. It is not expected that the exact equipment used during this testing will be used during the waste feed qualification testing for WTP, but functionally similar equipment will be used such that the techniques demonstrated would be applicable. For example, the mixing apparatus could use any suitable mixer capable of being remoted and achieving similar mixing speeds to those tested.

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DOE OSTI2016

Technology Development in Support of Accelerating the Waste Treatment Mission - 16409

The feed for vitrification to produce a nuclear waste glass is a mixture of waste with glass-forming and modifying additives that is charged onto the cold cap that covers 90-95% of the melt surface. The cold cap consists of a layer of reacting molten glass floating on the surface of the melt in an all-electric, continuous glass melter. As the feed moves through the cold cap, it undergoes chemical reactions and phase transitions through which it is converted to molten glass that moves from the cold cap into the melt pool. Multiple overlapping reactions occur within the cold cap. The process involves a series of reactions that generate multiple gases and subsequent mass loss and foaming significantly influence the mass and heat transfers. The rate of glass melting, is greatly influenced by mass and heat transfers, affects the vitrification process and the efficiency of the immobilization of nuclear waste. Therefore, understanding the cold-cap reactions over the temperature range of the conversion process is critical. It also helps to formulate melter feeds for higher production rate, initiation of crystal forming reactions, and chemical reactions that determine the ultimate fate of technetium in the glass melt. Though the flowsheets at each of the two sites is vastly different development and insertion of mature technological chemical processes and mechanical components can have a significant impact on the duration of the treatment mission and hence the total costs. (authors)

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NASA NTRS1975

Energy recovery from solid waste. Volume 2: Technical report

A systems analysis of energy recovery from solid waste demonstrates the feasibility of several current processes for converting solid waste to an energy form. The social, legal, environmental, and political factors are considered in depth with recommendations made in regard to new legislation and policy. Biodegradation and thermal decomposition are the two areas of disposal that are considered with emphasis on thermal decomposition. A technical and economic evaluation of a number of available and developing energy-recovery processes is given. Based on present technical capabilities, use of prepared solid waste as a fuel supplemental to coal seems to be the most economic process by which to recover energy from solid waste. Markets are considered in detail with suggestions given for improving market conditions and for developing market stability. A decision procedure is given to aid a community in deciding on its options in dealing with solid waste, and a new pyrolysis process is suggested. An application of the methods of this study are applied to Houston, Texas.

Huang, C. J.↗

DOE OSTI2015

Spinel dissolution via addition of glass forming chemicals. Results of preliminary experiments

Increased loading of high level waste in glass can lead to crystallization within the glass. Some crystalline species, such as spinel, have no practical impact on the chemical durability of the glass, and therefore may be acceptable from both a processing and a product performance standpoint. In order to operate a melter with a controlled amount of crystallization, options must be developed for remediating an unacceptable accumulation of crystals. This report describes preliminary experiments designed to evaluate the ability to dissolve spinel crystals in simulated waste glass melts via the addition of glass forming chemicals (GFCs).

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DOE OSTI2024

Biological Upcycling of Plastics Waste

Plastic wastes accumulate in the environment, impacting wildlife and human health and representing a significant pool of inexpensive waste carbon that could form feedstock for the sustainable production of commodity chemicals, monomers, and specialty chemicals. Current mechanical recycling technologies are not economically attractive due to the lower-quality plastics that are produced in each iteration. Thus, the development of a plastics economy requires a solution that can deconstruct plastics and generate value from the deconstruction products. Biological systems can provide such value by allowing for the processing of mixed plastics waste streams via enzymatic specificity and using engineered metabolic pathways to produce upcycling targets. We focus on the use of biological systems for waste plastics deconstruction and upcycling. We highlight documented and predicted mechanisms through which plastics are biologically deconstructed and assimilated and provide examples of upcycled products from biological systems. Additionally, we detail current challenges in the field, including the discovery and development of microorganisms and enzymes for deconstructing non–polyethylene terephthalate plastics, the selection of appropriate target molecules to incentivize development of a plastic bioeconomy, and the selection of microbial chassis for the valorization of deconstruction products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

EBS Task Force: Task 9/FEBEX Modeling Final Report: Thermo-Hydrological Modeling with PFLOTRAN

This report outlines Sandia National Laboratories modeling studies applied to Stage 1 and Stage 2 of the Full-scale Engineered Barriers Experiment in Crystalline Host Rock (FEBEX) in situ test for the SKB EBS Task Force Task 9. The FEBEX test was a full-scale test conducted over ~18 years at the Grimsel, Switzerland Underground Research Laboratory (URL) managed by NAGRA. It involved emplacing simulated waste packages, in the form of welded cylindrical heaters, inside a tunnel in crystalline granitic rock and surrounded by a bentonite barrier and cement plug. Sensors emplaced within the bentonite monitored the wetting-up, heating, and drying out of the bentonite barrier, and the large resulting data set provides an excellent opportunity for validation of multiphysics Thermal-Hydrological (TH), Thermal-Hydrologic-Chemical (THC), and Thermal-Hydrological-Mechanical (THM) modeling approaches for underground nuclear waste storage and the performance of engineered bentonite barriers. The present status of the EBS Task Force is finalizing Task 9, which follows years of modeling studies of the FEBEX test, by many notable modeling teams (Gens et al., 2009; Sanchez et al. 2010; 2012; Samper et al., 2018). These modeling studies generally use two-dimensional axisymmetric meshes, ignoring threedimensional effects, gravity and asymmetric wetting and dry out of the bentonite engineered barrier. This study investigates these effects with use of the PFLOTRAN THC code with massively parallel computational methods in modeling FEBEX Stage 1 and Stage 2 results. The PFLOTRAN numerical code is an open source, state-of-the-art, massively parallel subsurface flow and reactive transport code operating in a high-performance computing environment (Hammond et al., 2014). Section 2 describes the applied partial differential equations describing mass, momentum and energy balance used in this study, considerations derived by assuming phase equilibrium between gas and liquid phases, constitutive equations for granite, cement plug, and bentonite domains, and specific approaches for use inthe PFLOTRAN code. Section 3 describes the geometry, meshing, and model set-up. Section 4 describes modeling results, Section 5 compares modeling results to field testing data, and Section 6 gives conclusions. The Appendix provides detailed information required by the EBSTask Force for final reporting.

42 ENGINEERING↗

DOE OSTI2017

Using polymerization, glass structure, and quasicrystalline theory to produce high level radioactive borosilicate glass remotely: a 20+ year legacy

Vitrification is currently the most widely used technology for the treatment of high level radioactive wastes (HLW) throughout the world. Most of the nations that have generated HLW are immobilizing in borosilicate glass. One of the primary reasons that glass has become the most widely used immobilization media is the relative simplicity of the vitrification process, e.g. melt a highly variable waste with some glass forming additives such as SiO 2 and B 2 O 3 in the form of a premelted frit and pour the molten mixture into a stainless steel canister. Seal the canister before moisture can enter the canister (10’ tall by 2’ in diameter) so the canister does not corrode from the inside out. Glass has also become widely used for HLW is that due to the fact that the short range order (SRO) and medium range order (MRO) found in the structure of glass atomistically bonds the radionuclides and hazardous species in the waste. The SRO and MRO have also been found to govern the melt properties such as viscosity and resistivity of the melt and the crystallization potential and solubility of certain species. Furthermore, the molecular structure of the glass also controls the glass durability, i.e. the contaminant/radionuclide release, by establishing the distribution of ion exchange sites, hydrolysis sites, and the access of water to those sites. The molecular structure is flexible and hence accounts for the flexibility of glass formulations to HLW waste variability. Nuclear waste glasses melt between 1050-1150°C which minimizes the volatility of radioactive components such as 99 Tc, 137 Cs, and 129 I. Nuclear waste glasses have good long term stability including irradiation resistance. Process control models were developed based on the molecular structure of glass, polymerization theory of glass, and quasicrystalline theory of glass crystallization. These models create a glass which is durable, pourable, and processable with 95% accuracy without knowing from batch to batch what the composition of the waste coming out of the storage tanks will be. These models have operated the Savannah River Site Defense Waste Processing Facility (SRS DWPF), which is the world’s largest HLW Joule heated ceramic melter, since 1996. This unique “feed forward” process control, which qualifies the durability, pourability, and processability of the waste plus glass additive mixture before it enters the melter, has enabled ~8000 tons of HLW glass and 4242 canisters to be produced since 1996 with only one melter replacement.

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NASA NTRS1982

Process for the production of ultrahigh purity silane with recycle from separation columns

Tri- and dichlorosilanes formed by hydrogenation in the course of the reaction of metallurgical silicon, hydrogen and recycle silicon tetrachloride are employed as feed into a separation column arrangement of sequential separation columns and redistribution reactors which processes the feed into ultrahigh purity silane and recycle silicon tetrachloride. A slip stream is removed from the bottom of two sequential columns and added to the recycle silicon tetrachloride process stream causing impurities in the slip streams to be subjected to reactions in the hydrogenation step whereby waste materials can be formed and readily separated.

Coleman, Larry M.↗

DOE OSTI2013

A History of the Environmental Management Advisory Board: 20 Years of Service and Partnership - 13219

The Environmental Management Advisory Board (EMAB or Board) was chartered under the Federal Advisory Committee Act (FACA) in 1992 to provide the Assistant Secretary for Environmental Management (EM) with independent and external advice, information, and recommendations on corporate issues relating to accelerated site clean-up and risk reduction throughout the EM complex. Over the course of the past 20 years, the composition and focus of the Board have varied widely to address the changing needs of the program. EMAB began as the Environmental Restoration and Waste Management Advisory Committee, formed to provide advice on an EM Programmatic Environmental Impact Statement. In 1994, the Board was restructured to function more as an executive-level, limited member advisory board whose membership provides insight of leading industry experts and the viewpoints of representatives from critical stakeholder constituencies. Throughout the 20 years of its existence, EMAB has covered a wide variety of topics and produced nearly 200 recommendations. These recommendations have resulted in several policy changes and improvements within EM. Most recently, EMAB has been credited for its contribution to the EM Energy Park Initiative, forerunner of the DOE Asset Revitalization Initiative; creation of the EM Offices of Communications and External Affairs; improvement of acquisition and project management strategies and culture; and several recommendations related to the Waste Treatment Plant and the tank waste programs at Hanford and the Savannah River Site. The wealth of experience and knowledge the Assistant Secretary can leverage through utilization of the Board continues to support fulfillment of EM's mission. In commemoration of EMAB's 20. anniversary, this paper will provide further context for the evolution of the Board, the role FACA plays in its administration, and a look at the members' current objectives and EM's expectations for the future. (authors)

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DOE OSTI2013

Kinetics of Cold-Cap Reactions for Vitrification of Nuclear Waste Glass Based on Simultaneous Differential Scanning Calorimetry - Thermogravimetry (DSC-TGA) and Evolved Gas Analysis (EGA)

For vitrifying nuclear waste glass, the feed, a mixture of waste with glass-forming and modifying additives, is charged onto the cold cap that covers 90-100% of the melt surface. The cold cap consists of a layer of reacting molten glass floating on the surface of the melt in an all-electric, continuous glass melter. As the feed moves through the cold cap, it undergoes chemical reactions and phase transitions through which it is converted to molten glass that moves from the cold cap into the melt pool. The process involves a series of reactions that generate multiple gases and subsequent mass loss and foaming significantly influence the mass and heat transfers. The rate of glass melting, which is greatly influenced by mass and heat transfers, affects the vitrification process and the efficiency of the immobilization of nuclear waste. We studied the cold-cap reactions of a representative waste glass feed using both the simultaneous differential scanning calorimetry thermogravimetry (DSC-TGA) and the thermogravimetry coupled with gas chromatography-mass spectrometer (TGA-GC-MS) as complementary tools to perform evolved gas analysis (EGA). Analyses from DSC-TGA and EGA on the cold-cap reactions provide a key element for the development of an advanced cold-cap model. It also helps to formulate melter feeds for higher production rate.

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DOE OSTI2016

Treatment of LLW Components for Waste Minimization and Recycling - 16258

The Studsvik Melting Facility has been in operation for almost 30 years. Many turbines, heat exchangers and other retired components, pipes, structures have been treated in the facility during those years. The ambition of all projects is to minimize the waste volumes for final disposal and to maximize the amount of material that can be recycled. Another objective, respecting ALARA, is to keep dose exposition to the personnel at very low levels. The overall concept comprises the whole sequence of preparations from road and sea transports, the management of the metallic LLW by segmentation, decontamination and sorting using specially devised tools and shielded treatment cell, to the decision criteria for recycling of the metals, radiological analyses and conditioning of the residual waste into a final form suitable for customer-related disposal. The records show that the amount of material possible for conditional clearance to open market after treatment is between 95 - 97 % on weight for falling metallic scrap. For large components there is a larger span and especially for heat exchangers. This paper describes the Studsvik technical concept and experience related to treatment of metals from the program for modernization and power upgrade of the Swedish nuclear power plants. (authors)

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DOE OSTI2014

Application of evolved gas analysis to cold-cap reactions of melter feeds for nuclear waste vitrification

In the vitrification of nuclear wastes, the melter feed (a mixture of nuclear waste and glass-forming and modifying additives) experiences multiple gas-evolving reactions in an electrical glass-melting furnace. We employed the thermogravimetry-gas chromatography-mass spectrometry (TGA-GC-MS) combination to perform evolved gas analysis (EGA). Apart from identifying the gases evolved, we performed quantitative analysis relating the weighed sum of intensities of individual gases linearly proportional with the differential themogravimetry. The proportionality coefficients were obtained by three methods based on the stoichiometry, least squares, and calibration. The linearity was shown to be a good first-order approximation, in spite of the complicated overlapping reactions.

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DOE OSTI2019

Robotic Solutions for Remote Access and Retrieval of High-Level Radioactive Waste - 19544

This paper describes the ongoing development of robotic solutions for accessing and retrieving high-level radioactive waste from underground storage bins as part of the Calcine Retrieval Project at the INL Site. The waste is in the form of a solid powder, referred to as calcine, stored in a set of stainless steel bins within an underground concrete vault. Due to the radiation field produced by the calcine, all operations must be performed remotely. The Calcine Retrieval Project is currently carrying out proof-of-concept testing of methods for the various stages of calcine retrieval. The bins were designed with no means for access, so retrieval operations will require welding access riser pipes to the bins, followed by cutting through the bin walls from within the risers. These tasks are complicated by the fact that four of the risers must be placed off center on a domed surface, resulting in a weld joint that is curved and tilted relative to the riser axis. The Access Riser Connection robot is being developed to perform these operations using interchangeable welding and plasma cutting attachments. The majority of the calcine will be removed using a vacuum system and pneumatically transferred to storage. This system is not described in this paper. However, the bins contain several internal features that are expected to retain calcine, most notably circumferential stiffening rings on the walls and radial ribs on the floors. One of the solutions being developed for the task of retrieving this residual calcine is a vacuum crawler, a wheeled robot using vacuum to adhere to the interior walls of the bins. The vacuum crawler would use a separate vacuum system to remove residual calcine or would use compressed air to move calcine to a location from which it can be retrieved more easily. While comparable welding and wall-climbing robots have been developed before, this particular application has several constraints that are not satisfied by existing systems. For this reason, both the access riser welder and the vacuum crawler, although still under development, may be of interest to other projects faced with similar constraints. (author)

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DOE OSTI2020

Nonlinear Logistic Regression Mixture Experiment Modeling for Binary Data Using Dimensionally Reduced Components

This article presents and illustrates an approach using nonlinear logistic regression for modeling binary response data from a mixture experiment when the components can be partitioned into groups used to form dimensionally-reduced pseudocomponents (DRPs). A DRP is a linear combination of the components in a group, where the linear combinations over all groups are normalized so that the DRP proportions sum to unity. Nonlinear logistic regression is required because, after normalization of the linear combinations, the model expressed in terms of the DRPs is nonlinear in the parameters that specify the linear combinations. A method for obtaining nonparametric tolerance limits on the probability of a “success” for the binary response variable using a bootstrap approach is also presented. Having three DRPs enables viewing data and modeling results on a ternary plot even though there may be many more than three mixture components. A real database, involving whether or not nepheline crystals form in simulated nuclear waste glass after cooling, is used to illustrate the nonlinear logistic regression modeling and nonparametric tolerance limit approaches when there are three DRPs.

Waste glass, Nepheline, Mixture experiment, Logist↗

DOE OSTI2016

Energy Harvesting from Pipeline Vibration: CRADA Final Report

Investigating the extraction of energy from pipeline vibrations related to operations in the oil and gas industry. The wasted energy in the form of mechanical vibrations can be exploited to generate useful energy for low and medium power electronic devices (e.g., sensors) operating independently in deep sea and surface environments. Existing energy harvesting technologies and literature were surveyed to come up with a feasible design employing piezoelectric material. The project was important to reduce energy wastage and hence to national energy security.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2023

Optimization Efforts at DWPF to Ensure Waste Tank Closure by 2037 – 24404

At the Savannah River Site (SRS) in Aiken, South Carolina, the Defense Waste Processing Facility (DWPF) produces a glass-form product by processing high-level liquid waste (HLW) with borosilicate glass in a high-heated Melter, then putting the vitrified waste into stainless-steel canisters. Since 1996, DWPF has performed this vitrification process for the liquid waste mission at the SRS; the overall objective for this mission is to reduce the volume in the upstream waste tanks, so those tanks can be emptied and operationally closed. This mission seeks to eliminate the single biggest environmental risk in the state of South Carolina, which requires a robust processing strategy within the DWPF, along with optimal interface between the other facilities in the liquid waste organization (LWO). As of the end of July 2023, DWPF has safely remediated 63.7 MCi of HLW, and filled 4,319 canisters (We project that about 4,000 more canisters are needed to be filled to reach the closure goal.)

Armstead, III, Frank L.↗