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At least 865 records · Page 48

Separation and Purification of Berkelium-249 and Einsteinium-254

Berkelium-249 ( 249 Bk) and einsteinium-254 ( 254 Es) are isotopes of great importance for the investigation of berkelium and einsteinium chemical properties and super heavy element research. Therefore, it is necessary to be able to isolate acceptable, pure quantities of both isotopes to further research capabilities. These isotopes, along with californium-252 ( 252 Cf), are synthesized through the irradiation of mixed-curium targets in the High Flux Isotope Reactor (HFIR), which has the highest continuous thermal neutron flux in the world. Once irradiated, the targets are transferred to the Radiochemical Engineering Development Center for further chemical processing and final purification to separate 249 Bk and 254 Es from the remainder of isotopes present. Several methods of separation, such as the Berkex batch solvent extraction along with cation-exchange and alpha-hydroxy-isobutyrate (AHIB) columns, are employed to achieve a clean separation of the isotopes. Production Campaigns 74–77 are discussed in depth for 252 Cf, 249 Bk, and 254 Es production and isolation of 249 Bk and 254 Es. An attempt to isolate 257 Fm in Campaign 77 is discussed as well. Table 1 summarizes the total amount of material isolated in each campaign.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Conversion, Stability, and Selectivity Improvements Through Catalyst Development for the Reductive Etherification Reaction

Economical pathways from lignocellulosic non-food biomass feedstocks to biofuels with appropriate fuel properties are necessary for displacing fossil-fuel derived diesel use in medium-/heavy duty vehicles. Oxygenated compounds have recently shown promise due to low sooting tendencies and autoignition properties and molecules with sufficiently high carbon numbers can meet the requisite standards for water solubility and flash point. Coupling waste biomass derived small molecules into bioblendstock targets through the reductive etherification reaction shows potential for increasing molecular weight without losing the advantages of oxygenates. However, the transition to industrial viability for this process is limited by strong catalyst deactivation in typical flow reactor systems. Strong acid resins such as Amberlyst-15 (A-15) show excellent activity in batch reactions but are limited to low temperatures and are poisoned by the side-product, water. In this talk, I will describe our recent work in catalyst synthesis and testing to select superior options with improved aqueous and thermal stability in reductive etherification flow reactions. Water-tolerant solid acid catalysts have potential to improve the conversion and selectivity to the ether target at temperatures above the degradation point of A-15. Analysis techniques such as physisorption, chemisorption, x-ray diffraction and transmission electron microscopy are being used to characterize the active sites. These techniques are also being used to evaluate degradation of the catalyst after extensive flow reactions in addition to comparative efficiency testing with standardized cyclohexene hydrogenation reactions. Finally, I will discuss a demonstration of the full pathway from bio-derived butyric acid to the performance-advantaged ether product and the additional obstacles from side-products and purification limitations in the preliminary upgrading reactions.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Use of Novel Diglycolamide Extractants in Liquid-liquid Separations of Light Rare Earths

Creation of a novel extractant that can improve rare earth separations both economically and environmentally will be pivotal for industry progression. Diglycolamide (DGA) extractants provide chemistries that support this goal by serving as an extractant with high affinity for lanthanides and improved separation factors for light rare earths as compared to current extractants like PC88A. Initial organic phase loading capacity and phase dispersion tests performed with various modified DGAs generated results that were unfavorable for industrial processing, but further modification of the DGA alkyl chain substituents have resulted in new structures with promising results. Dispersion time measurements taken in small scale batch contacts of the extractant with a simulated leach liquor containing La, Ce, Nd, and Pr support implementation in both mixer-settlers and centrifugal contactors for larger scale separations. Furthermore, this confirmation allowed for preliminary flowsheet design using extraction equilibria at various organic to aqueous flow ratios (O/A) for extraction, scrubbing, and stripping stages. These values along with expected product/effluent compositions for each section aid in the testing for specific distribution ratios and final flowsheet design. Implementation of the DGA extractant into solvent extraction equipment will provide essential information for the next steps of this project and how this extractant may be optimized for future applications.

42 ENGINEERING↗

Quantification of Cation Sorption to Engineered Barrier Materials Under Extreme Conditions

The objective of this research is to examine mechanisms and thermodynamics of actinide sorption to engineered barrier materials (iron (oxyhydr)oxides and bentonite clay) for nuclear waste repositories under high temperature and high ionic strength conditions using a suite of macroscopic and microscopic techniques which will be coupled with interfacial reaction models. Gaining a mechanistic understanding of interfacial processes governing the sorption/sequestration of actinides at mineral-water interfaces is fundamental for the accurate prediction of actinide behavior in waste repositories. Although macroscale sorption data and various spectroscopic techniques have provided valuable information regarding speciation of actinides at solid-water interfaces, significant knowledge gaps still exist with respect to sorption mechanisms and the ability to quantify sorption, particularly at high temperatures and ionic strengths. This objective is addressed through three major tasks: (1) influence of oxidation state on actinide sorption to iron oxides and clay minerals at elevated temperatures and ionic strengths; (2) calorimetric titrations of actinide-mineral suspensions; (3) evaluation of bentonite performance under repository conditions. The results of the work will include a qualitative conceptual model and a quantitative thermodynamic speciation model describing actinide partitioning to minerals and sediments, which is based upon a mechanistic understanding of specific sorption processes as determined from both micro-scale and macroscale experimental techniques. The speciation model will be a thermodynamic aqueous and surface complexation model of actinide interactions with mineral surfaces that is self-consistent with macroscopic batch sorption data, calorimetric and potentiometric titrations, X-ray absorption Spectroscopy (XAS, mainly Extended X-ray Absorption Fine Structure (EXAFS)), and electron microscopy analyses. The novelty of the proposed work lies largely in the unique system conditions which will be examined (i.e. elevated temperature and ionic strength) and the manner in which the surface complexation model will be developed in terms of specific surface species identified using XAS. These experiments will thus provide a fundamental understanding of the chemical and physical processes occurring at the solid-solution interface under expected repository conditions. Additionally, the focus on thermodynamic treatment of actinide ion interactions with minerals as proposed will provide information on the driving forces involved and contribute to the overall understanding of the high affinity many actinide ions have for oxide surfaces. The utility of this model will be demonstrated in this work through a series of advective and diffusive flow experiments.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Bench Scale Process for Low Cost CO 2 Capture Using a Phase-Changing Absorbent: Final Scientific/Technical Report

The objective of this project is to design and build a bench-scale process for a novel phase-changing aminosilicone-based CO 2 -capture solvent. The project will establish scalability and technical and economic feasibility of using a phase-changing CO 2 -capture absorbent for post-combustion capture of CO 2 from coal-fired power plants. The U.S. Department of Energy’s goal for Transformational Carbon Capture Technologies is the development of technologies available for demonstration by 2025 that can capture 90% of emitted CO 2 with at least 95% CO 2 purity for less than $40/tonne of CO 2 captured. In the first budget period of the project, the bench-scale phase-changing CO2 capture process was designed using data and operating experience generated under a previous project (ARPA-e project DE-AR0000084). Sizing and specification of all major unit operations was completed, including detailed process and instrumentation diagrams. The system was designed to operate over a wide range of operating conditions to allow for exploration of the effect of process variables on CO 2 capture performance. In the second budget period of the project, individual bench-scale unit operations were tested to determine the performance of each of each unit. Solids production was demonstrated in dry simulated flue gas across a wide range of absorber operating conditions, with single stage CO 2 conversion rates up to 75mol%. Desorber operation was demonstrated in batch mode, resulting in desorption performance consistent with the equilibrium isotherms for GAP-0/CO 2 reaction. Important risks associated with gas humidity impact on solids consistency and desorber temperature impact on thermal degradation were explored, and adjustments to the bench-scale process were made to address those effects. Corrosion experiments were conducted to support selection of suitable materials of construction for the major unit operations in the process. The bench scale unit operations were assembled into a continuous system to support steady state system testing. In the third budget period of the project, continuous system testing was conducted, including closed-loop operation of the absorber and desober systems. Slurries of GAP-0/GAP-0 carbamate/water mixtures produced in the absorber were pumped successfully to the desorber unit, and regenerated solvent was returned to the absorber. A techno-economic analysis, EH&S risk assessment, and solvent manufacturability study were completed.

20 FOSSIL-FUELED POWER PLANTS↗

Centrifugal Contactor Operations for UREX Process Flowsheet

The UREX process separates uranium, technetium, and a fraction of the iodine from the other components of the irradiated fuel in nitric acid solution. The time and equipment requirements were evaluated for treatment of 260-L batches of a solution containing 130 g-U/L using commercial annular centrifugal contactors from CINC Industries. An earlier evaluation was done assuming 150 L of feed solution per batch. Two different contactor versions from CINC were evaluated, the V-2 and V-5 units. The V-2 has a 2-in. (5-cm) rotor with a reported maximum total organic-plus-aqueous throughput of 1.9 L/min. We evaluated this version for a throughput of 1 L/min. The V-5 has a 5-in. (~12.5-cm) rotor with a reported maximum throughput of 19 L/min. We evaluated this unit for throughputs of 10 and 15 L/min. The lower-than-maximum throughputs selected for this evaluation are based on the Argonne National Laboratory (Argonne) ROTOR model, which calculates the operational envelope for a given process O:A (organic-flow-rate/aqueous-flow rate) ratio based on contactor parameters (weir dimensions, rotor diameter, etc.), the physical properties of the two immiscible fluids, and the allowable other-phase-carryover. Because the UREX process designed for this application has O:A ratios ranging from 0.8 to 5.6, adjustments to the weirs in different sections of the contactor bank can broaden the operational envelope for satisfactory separations, but throughput will remain short of the equipment maximum due to the physical characteristics of the two phases.

Pereira, Candido↗

Pyrolysis of waste tyres: A review

Graphical abstract: - Highlights: • Pyrolysis of waste tyres produces oil, gas and char, and recovered steel. • Batch, screw kiln, rotary kiln, vacuum and fluidised-bed are main reactor types. • Product yields are influenced by reactor type, temperature and heating rate. • Pyrolysis oils are complex and can be used as chemical feedstock or fuel. • Research into higher value products from the tyre pyrolysis process is reviewed. - Abstract: Approximately 1.5 billion tyres are produced each year which will eventually enter the waste stream representing a major potential waste and environmental problem. However, there is growing interest in pyrolysis as a technology to treat tyres to produce valuable oil, char and gas products. The most common reactors used are fixed-bed (batch), screw kiln, rotary kiln, vacuum and fluidised-bed. The key influence on the product yield, and gas and oil composition, is the type of reactor used which in turn determines the temperature and heating rate. Tyre pyrolysis oil is chemically very complex containing aliphatic, aromatic, hetero-atom and polar fractions. The fuel characteristics of the tyre oil shows that it is similar to a gas oil or light fuel oil and has been successfully combusted in test furnaces and engines. The main gases produced from the pyrolysis of waste tyres are H{sub 2}, C{sub 1}–C{sub 4} hydrocarbons, CO{sub 2}, CO and H{sub 2}S. Upgrading tyre pyrolysis products to high value products has concentrated on char upgrading to higher quality carbon black and to activated carbon. The use of catalysts to upgrade the oil to a aromatic-rich chemical feedstock or the production of hydrogen from waste tyres has also been reported. Examples of commercial and semi-commercial scale tyre pyrolysis systems show that small scale batch reactors and continuous rotary kiln reactors have been developed to commercial scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Simulated moving bed-inspired method for continuous adsorptive denitrogenation of model fuel

Efficient, continuous routes for removing nitrogen-containing compounds from hydrothermal liquefaction-derived synthetic aviation fuel are needed to enable direct blending with conventional jet fuels. Here, we report a simulated moving bed-inspired process for adsorptive denitrogenation of a model fuel. Unlike conventional simulated moving bed systems, which are designed for sharp separations between similar solutes, this approach was run deliberately outside the classical separation region so that both pyridine and indole were removed together from the hydrocarbon stream. Alcohol solvents were used to regenerate the silica adsorbent, maintaining performance over extended operation and avoiding the downtime and energy demand associated with calcination. Under these conditions, the system demonstrates removal of more than 98% of nitrogen while cutting solvent use by 28% compared to batch operation. Classical modeling tools predicted column concentration profiles even in this nontraditional regime, suggesting a straightforward path to scaling. Together, these results motivate solvent-efficient, continuous denitrogenation strategies that could be integrated with biorefinery processes.

Adsorption↗

Developing a Scalable System for Biorecovery of Critical Materials from Industrial Waste with Gluconobacter Oxydans

Organic acid production by Gluconobacter oxydans has been proposed as part of a potential economical and environmentally friendly heterotrophic bioleaching process for recovery of rare earth elements from industrial waste. To provide organic acids in a quantity and at a rate useful for commercial bioleaching, continuous culture of the acid-producing organism will be necessary. The objective of this research project was to determine optimal conditions for continuous cultivation of G. oxydans for production of organic acids. Cultures were subjected to dilution rates ranging from .05 hr -1 to .38 hr -1 to determine the optimum conditions for production of lixiviant agents. Previous studies have identified methods for maximizing production of gluconic acid and 2,5-diketogluconic acid from G. oxydans , yet the utilization of these and other unidentified G. oxydans metabolites for leaching of rare earth metals is largely unexplored. Continuous cultures exhibited sustained organic acid production for at least 110 hours, while batch fermentations showed slowed growth rates after 16 hours. Several parameters, namely optical density, dissolved oxygen, organic acid concentration and pH, were monitored to characterize the steady state conditions of the fermentation process. The observed trend was increasing acidity with decreasing dilution rates, as the lowest dilution rate of 0.05 hr -1 yielded the highest gluconic acid concentration of 176 mM and lowest pH of 2.20. Trace amounts of 2,5-diketogluconic acid were detected only at the 0.05 hr-1 dilution rate, likely because the pH of the bioreactors was not maintained within the window for gluconate dehydrogenase activity [Silberbach, M., et al., Appl Microbiol Biotechnol, 2003. 62(1): p. 92-8].

60 APPLIED LIFE SCIENCES↗

Direct Feed Low Activity Waste Test Platform - Pretreatment Unit Operations - 18613

The Low-Activity Waste Pretreatment System (LAWPS) facility is planned to pretreat Hanford tank waste supernate by filtering solids and processing through ion exchange columns to remove cesium. Note that cesium ion exchange is not discussed in this paper. The filtration process is achieved through cross flow filtration using a stainless steel Mott filter with a 0.1-micron grade. The goal of this effort was to assess whether a batch, or dead end, filtration (DEF) device replicating the LAWPS cross flow filter could be employed to qualify each feed campaign prior to delivery to LAWPS. The objective for filtration feed qualification is to determine whether the cross flow filters deployed in LAWPS will remove solids while maintaining a de minimis flow rate of permeate. To that end, the DEF was tested with simulants and the results compared with those obtained from cross flow filtration tests. In addition, actual waste samples were retrieved from Hanford Site Tank AP-105 and were composited for testing. These composited samples were first tested with cross flow filtration to determine the filter flux under typical LAWPS conditions. The same material was subsequently tested with DEF to determine a filter flux. While the DEF correctly predicted the cross flow filter's ability to filter solids from the feed, there was limited correlation between DEF and cross flow filtration flux results. This lack of correlation suggests a fundamental difference between cross flow filtration and DEF as used in these tests. Taken in total, these results indicate that DEF is not a good candidate to provide qualification of feed for LAWPS cross flow filtration. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Scalable Synthesis of Ti 3 C 2 T x MXene

Scaling the production of synthetic 2D materials to industrial quantities has faced significant challenges due to synthesis bottlenecks whereby few have been produced in large volumes. These challenges typically stem from bottom‐up approaches limiting the production to the substrate size or precursor availability for chemical synthesis and/or exfoliation. In contrast, MXenes, a large class of 2D transition metal carbides and/or nitrides, are produced via a top‐down synthesis approach. The selective wet etching process does not have similar synthesis constraints as some other 2D materials. The reaction occurs in the whole volume; therefore, the process can be readily scaled with reactor volume. Herein, the synthesis of 2D titanium carbide MXene (Ti 3 C 2 T x ) is studied in two batch sizes, 1 and 50 g, to determine if large‐volume synthesis affects the resultant structure or composition of MXene flakes. Characterization of the morphology and properties of the produced MXene using scanning electron microscopy, X‐ray diffraction, dynamic light scattering, Raman spectroscopy, X‐ray photoelectron spectroscopy, UV–visible spectroscopy, and conductivity measurements show that the materials produced in both batch sizes are essentially identical. This illustrates that MXenes experience no change in structure or properties when scaling synthesis, making them viable for further scale‐up and commercialization.

Shuck, Christopher E.↗

Ru-Sn/AC for the Aqueous-Phase Reduction of Succinic Acid to 1,4-Butanediol under Continuous Process Conditions

Succinic acid is a biomass-derived platform chemical that can be catalytically converted in the aqueous phase to 1,4-butanediol (BDO), a prevalent building block used in the polymer and chemical industries. Despite significant interest, limited work has been reported regarding sustained catalyst performance and stability under continuous aqueous-phase process conditions. As such, this work examines Ru-Sn on activated carbon (AC) for the aqueous-phase conversion of succinic acid to BDO under batch and flow reactor conditions. Initially, powder Ru-Sn catalysts were screened to determine the most effective bimetallic ratio and provide a comparison to other monometallic (Pd, Pt, Ru) and bimetallic (Pt-Sn, Pd-Re) catalysts. Batch reactor tests determined that a ~1:1 metal weight ratio of Ru to Sn was effective for producing BDO in high yields, with complete conversion resulting in 82% molar yield. Characterization of the fresh Ru-Sn catalyst suggests that the sequential loading method results in Ru sites that are colocated and surface-enriched with Sn. Postbatch reaction characterization confirmed stable Ru-Sn material properties; however, upon a transition to continuous conditions, significant Ru-Sn/AC deactivation occurred due to stainless steel leaching of Ni that resulted in Ru-Sn metal crystallite restructuring to form discrete Ni-Sn sites. Computational modeling confirmed favorable energetics for Ru-Sn segregation and Ni-Sn formation at submonolayer Sn incorporation. To address stainless steel leaching, reactor walls were treated with an inert silica coating by chemical vapor deposition. With leaching reduced, stable Ru-Sn/AC performance was observed that resulted in a molar yield of 71% BDO and 15% tetrahydrofuran for 96 h of time on stream. Postreaction catalyst characterization confirmed low levels of Ni and Cr deposition, although early-stage islanding of Ni-Sn will likely be problematic for industrially relevant time scales (i.e., thousands of hours). Overall, these results (i) demonstrate the performance of Ru-Sn/AC for aqueous phase succinic acid reduction, (ii) provide insight into the Ru-Sn bimetallic structure and deactivation in the presence of leached Ni, and (iii) underscore the importance of compatible reactor metallurgy and durable catalysts.

09 BIOMASS FUELS↗

Optical follow-up of gravitational wave triggers with DECam

Gravitational wave (GW) events have several possible progenitors, including black hole mergers, cosmic string cusps, supernovae, neutron star mergers, and black hole{neutron star mergers. A subset of GW events are expected to produce electromagnetic (EM) emission that, once detected, will provide complementary information about their astrophysical context. To that end, the LIGO-Virgo Collaboration has partnered with other teams to send GW candidate alerts so that searches for their EM counterparts can be pursued. One such partner is the Dark Energy Survey (DES) and Dark Energy Camera (DECam) Gravitational Waves Program (DES- GW). Situated on the 4m Blanco Telescope at the Cerro Tololo Inter-American Observatory in Chile, DECam is an ideal instrument for optical followup observations of GW triggers in the southern sky. The DES-GW program performs subtraction of new search images with respect to preexisting overlapping images to select candidate sources. Due to the short decay timescale of the expected EM counterparts and the need to quickly eliminate survey areas with no counterpart candidates, it is critical to complete the initial analysis of each night's images within 24 hours. The computational challenges in achieving this goal include maintaining robust I/O pipelines during the processing, being able to quickly acquire template images of new sky regions outside of the typical DES observing regions, and being able to rapidly provision additional batch computing resources with little advance notice. We will discuss the search area determination, imaging pipeline, general data transfer strategy, and methods to quickly increase the available amount of batch computing. We will present results from the rst season of observations from September 2015 to January 2016 and conclude by presenting improvements planned for the second observing season.

79 ASTRONOMY AND ASTROPHYSICS↗

Testing and characterization of engineered forms of monosodium titanate (MST)

Engineered forms of MST and mMST were prepared at ORNL using an internal gelation process. Samples of these two materials were characterized at SRNL to examine particle size and morphology, peroxide content, tapped densities, and Na, Ti, and C content. Batch contact tests were also performed to examine the performance of the materials. The E mMST material was found to contain less than 10% of the peroxide found in a freshly prepared batch of mMST. This was also evidenced in batch contact testing with both simulated and actual waste, where little difference in performance was seen between the two engineered materials, E MST and E mMST.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Evolution of HEP Processing Frameworks

HEP data-processing software must support the disparate physics needs of many experiments. For both collider and neutrino environments, HEP experiments typically use data-processing frameworks to manage the computational complexities of their large-scale data processing needs. Data-processing frameworks are being faced with new challenges this decade. The computing landscape has changed from the past three decades of homogeneous single-core x86 batch jobs running on grid sites. Frameworks must now work on a heterogeneous mixture of different platforms: multi-core machines, different CPU architectures, and computational accelerators; and different computing sites: grid, cloud, and high-performance computing. We describe these challenges in more detail and how frameworks may confront them. Given their historic success, frameworks will continue to be critical software systems that enable HEP experiments to meet their computing needs. Frameworks have weathered computing revolutions in the past; they will do so again with support from the HEP community

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Centrifugal contactor operations for UREX process flowsheet. An update

The uranium extraction (UREX) process separates uranium, technetium, and a fraction of the iodine from the other components of the irradiated fuel in nitric acid solution. In May 2012, the time, material, and footprint requirements for treatment of 260 L batches of a solution containing 130 g-U/L were evaluated for two commercial annular centrifugal contactors from CINC Industries. These calculated values were based on the expected volume and concentration of fuel arising from treatment of a single target solution vessel (TSV). The general conclusions of that report were that a CINC V-2 contactor would occupy a footprint of 3.2 m 2 (0.25 m x 15 m) if each stage required twice the nominal footprint of an individual stage, and approximately 1,131 minutes or nearly 19 hours is required to process all of the feed solution. A CINC V-5 would require approximately 9.9 m 2 (0.4 m x 25 m) of floor space but would require only 182 minutes or ~ 3 hours to process the spent target solution. Subsequent comparison with the Modular Caustic Side Solvent Extraction Unit (MCU) at Savannah River Site (SRS) in October 2013 suggested that a more compact arrangement is feasible, and the linear dimension for the CINC V-5 may be reduced to about 8 m; a comparable reduction for the CINC V-2 yields a length of 5 m. That report also described an intermediate-scale (10 cm) contactor design developed by Argonne in the early 1980s that would better align with the SHINE operations as they stood in May 2012. In this report, we revisit the previous evaluation of contactor operations after discussions with CINC Industries and analysis of the SHINE process flow diagrams for the cleanup of the TSV, which were not available at the time of the first assessment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High solids loading biorefinery for the production of cellulosic sugars from bioenergy sorghum

A novel process applying high solids loading in chemical-free pretreatment and enzymatic hydrolysis was developed to produce sugars from bioenergy sorghum. Hydrothermal pretreatment with 50% solids loading was performed in a pilot scale continuous reactor followed by disc refining. Sugars were extracted from the enzymatic hydrolysis at 10% to 50% solids content using fed-batch operations. Here, three surfactants (Tween 80, PEG 4000, and PEG 6000) were evaluated to increase sugar yields. Hydrolysis using 2% PEG 4000 had the highest sugar yields. Glucose concentrations of 105, 130, and 147 g/L were obtained from the reaction at 30%, 40%, and 50% solids content, respectively. The maximum sugar concentration of the hydrolysate, including glucose and xylose, obtained was 232 g/L. Additionally, the glucose recovery (73.14%) was increased compared to that of the batch reaction (52.74%) by using two- stage enzymatic hydrolysis combined with fed-batch operation at 50% w/v solids content.

09 BIOMASS FUELS↗

K-Basins Sludge Treatment and Packaging at the Hanford Site - 13585

Highly radioactive sludge resulting from the storage of degraded spent nuclear fuel has been consolidated in Engineered Containers (ECs) in the 105-K West Storage Basin located on the Hanford site near the Columbia River in Washington State. CH2M Hill Plateau Remediation Company (CHPRC) is proceeding with a project to retrieve the sludge, place it in Sludge Transport and Storage Containers (STSCs) and store those filled containers within the T Plant Canyon facility on the Hanford Site Central Plateau (Phase 1). Retrieval and transfer of the sludge material will enable removal of the 105-K West Basin and allow remediation of the subsurface contamination plumes under the basin. The U.S. Department of Energy (DOE) plans to treat and dispose of this K Basins sludge (Phase 2) as Remote Handled Transuranic Waste (RH TRU) at the Waste Isolation Pilot Plant (WIPP) located in New Mexico. The K Basin sludge currently contains uranium metal which reacts with water present in the stored slurry, generating hydrogen and other byproducts. The established transportation and disposal requirements require the transformation of the K Basins sludge to a chemically stable, liquid-free, packaged waste form. The Treatment and Packaging Project includes removal of the containerised sludge from T Plant, the treatment of the sludge as required, and packaging of all the sludge into a form that is certifiable for transportation to and disposal at WIPP. Completion of this scope will require construction and operation of a Sludge Treatment and Packaging Facility (STPF), which could be either a completely new facility or a modification of an existing Hanford Site facility. A Technology Evaluation and Alternatives Analysis (TEAA) for the STP Phase 2 was completed in 2011. A Request for Technology Information (RFI) had been issued in October 2009 to solicit candidate technologies for use in Phase 2. The RFI also included a preliminary definition of Phase 2 functions and requirements. Potentially applicable technologies were identified through a commercial procurement process, technical workshops, and review of the numerous previous sludge treatment technology studies. The identified technology approaches were screened using the criteria established in the Decision Plan, and focused bench top feasibility testing was conducted. Engineering evaluations of the costs, schedules, and technical maturity were developed and evaluated. Recommendations were developed based on technical evaluations. The criteria used in the evaluation process were as follows: (1) Safety, (2) Regulatory/stakeholder acceptance, (3) Technical maturity, (4) Operability and maintainability, (5) Life cycle cost and schedule, (6) Potential for beneficial integration with ongoing STP-Phase 1 activities, and (7) Integration with Site-wide RH-TRU processing/packaging, planning, schedule, and approach. The TEAA recommended Warm Water Oxidation (WWO) as the baseline treatment technology and two risk reduction enhancement options for further consideration during development of the process - size reduction and chemical oxidation (Fenton's reagent). The enhancement options would potentially allow a useful reduction in the total operating time required to process the K Basins sludge. The U.S. Department of Energy's Richland Field Office (DOE-RL) has approved this recommended technical approach. The baseline process can be broken down into the following main process steps: (1) STSC transfer from T Plant to the Sludge Treatment and Packaging Facility (STPF). (2) Retrieval of sludge from the STSCs and transfer to the Receipt and Reaction Tank (RRT). (3) Preparation for immobilization by oxidation using heated water (i.e., WWO) for those batches that require it and concentration by evaporating water at about atmospheric pressure in the RRT. (4) Immobilization by using additives to eliminate free liquids and packaging of the treated sludge into drums. (5) Inspection and handling of the filled drums prior to transfer to a separate storage and shipping facility. (6) Handling of vapor, condensate, and other waste streams generated by the process. Each of these steps is discussed in the paper, together with the current state of progress in developing the technology and requirements for continued development. A schematic of the recommended baseline WWO treatment process is given below. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗