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DOE OSTI2020

MH-1A Sturgis Decommissioning and Dismantlement - 20281

The U.S. Army Corps of Engineers (USACE) with its prime contractor, Aptim Federal Services, LLC (APTIM), recycled 5,260 metric tons (11.6 million pounds) of material from Sturgis Barge (Sturgis) during the Decommissioning and Dismantlement of the MH-1A nuclear power reactor. The overall objective of the project was to reduce residual radioactivity associated with MH-1A to levels that permitted release of Sturgis for dismantlement and termination of the Army Reactor Office permit. By effectively applying waste hierarchy's three Rs - reduce, reuse and recycle - the Sturgis project not only minimized the amount of waste that required disposal at landfills, but also reduced the potential for long-term environmental liability emanating from these landfills. The project team completed the physical decommissioning efforts in June 2018 in Galveston, TX. In September 2018, radiological surveys were completed to demonstrate the vessel could be released for shipbreaking. Sturgis was towed from Galveston, TX to Brownsville, TX in late September 2018. Shipbreaking, dismantlement and recycling efforts began in early October 2018 and were completed on 15 March 2019. As part of the decommissioning effort in Galveston, the team shipped 69 shipments (860 metric tons) of low-level radioactive waste and radioactive components to the Waste Control Specialist (WCS) facility in Andrews TX for disposal. Certain radioactive components had to be transferred to the Department of Energy prior to placing the materials into the Federal Waste Facility located within WCS. However, most of the radioactive waste was characterized, profiled, approved and managed under the WCS permitted radioactive waste exemption process authorized and implemented by the Texas Commission on Environmental Quality (TCEQ) and the Radioactive Materials Division. This allows LLRW and LLMW to be shipped as regulated waste and then upon receipt at WCS through satisfying the relevant waste acceptance criteria the waste is exempted and placed into the WCS RCRA permitted cell. An additional 35 shipments (544 metric ton) of contaminated hazardous waste water were transported to U.S. Ecology in Robstown, TX for treatment/disposal. An additional 36 shipments (500 metric tons) of non-hazardous wastewater was sent to Republic Waste Services' facility in Fresno, TX. The disposal of these materials required close coordination with State of Texas regulators. During decommissioning, the project team recycled approximately 270 metric tons (600,000 pounds) of lead and steel. As part of the dismantlement in Brownsville, TX the team recycled approximately 5,000 metric tons (11 million pounds) of ferrous and non-ferrous material, limiting our disposal requirements to about 180 metric tons (400,000 pounds) of material (<4% from entire shipbreaking activity). Although the primary hazard being mitigated by this project was radiological, recycling was always a priority for the project. The team strived to achieve sustainability goals as we implemented this one of a kind project. Scrap metal recycling has a large positive impact on the environment and can also favorably impact project disposal costs. Steel is among the most recycled material in the world. Nearly 40% of the world's steel production is made from scrap. Recycling steel also requires 75% less energy than producing it from raw materials. By using recycled steel rather than virgin materials, 2.33 kg of carbon emissions are eliminated per kg of steel [1]. The project recycled more than 4,500 metric tons (10 million pounds) of steel, which eliminated about 10,400 metric tons (23 million pounds) of CO{sub 2}. By implementing a recycling initiative for the Sturgis project, the team was able to realize cost avoidance for disposal of scrap, cost savings from the metals recycled, plus the project provided benefits to the environment through our recycling efforts. Once the dismantlement was complete, the team prepared a detailed decommissioning closure report, which allowed for the termination of the Army Reactor Decommissioning Permit. While it not only reduced any potential long-term environmental liability, this project to decommission and dismantle a floating nuclear power plant is truly unprecedented - it is a prime example of the USACE mission which is: 'Engineering solutions for the Nation's toughest challenges'. This unique, one of a kind, historical power plant was never designed to be taken apart, and the available information about its construction was lacking in many details. The hazards that required mitigation dictated a painstaking and deliberate process in order to avoid any release to the environment and the community, and to protect the health and safety of the workers involved while keeping the waste hierarchy's three R's - reduce, reuse and recycle at the forefront. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

AN ACID BAKING APPROACH TO ENHANCE RARE EARTH ELEMENT RECOVERY FROM BITUMINOUS COAL SOURCES

Rare earth elements (REE) are a group of 17 elements typically classified as light and heavy rare earth elements, which play a crucial role in developing the latest technologies for energy, defense, and medical sectors. Even though REEs have been found in more than 200 minerals, only bastnaesite, monazite and xenotime are commercially exploited for REE extraction. However, the recent exponential increase in REE demand has spurred countries such as the United States into research for the extraction of REEs from secondary sources such as coal, acid mine drainage, and coal ash. Several coal sources (e.g., Fire Clay seam coal) across the United States have been identified to contain elevated concentrations of rare earth elements (>600 ppm), and various researchers have investigated the feasibility of both physical and hydrometallurgical extraction techniques for rare earth concentration and subsequent extraction. However, both physical and direct leaching were concluded to be inefficient for RE beneficiation and extraction due to low recoveries. Alternatively, thermal treatment provides promising means for RE recovery from bituminous coal sources. The positive impact of thermal treatment/calcination was established to be due to the decarbonization and dehydroxylation of the clays, which released entrapped rare earth elements within the dominant minerals and converted them into an acid-soluble form. Nonetheless, the improvement in recovery was limited to the light REEs (LREEs) with an insignificant increase in the heavy REEs (HREE). It was demonstrated that the light and heavy REEs in the material were associated with difficult-to-leach minerals such as monazite, xenotime, and zircon, which were not decomposed by simple calcination due to their high thermal stability. Hence, roasting in the presence of chemicals was necessary to ensure the decomposition of those REE-containing minerals. As such, this study was focused on the acid baking treatment of bituminous coals with an aim to enhance REE recovery, especially HREEs. Based on the presence of REE minerals like monazite and xenotime, three pre-leach treatment methods, i.e., 1) roasting, 2) direct acid baking, and 3) acid baking after roasting were investigated. Roasting tests at 600 ⁰C revealed that the recovery of light REEs (LREEs) was enhanced while the recovery of HREEs remained relatively unaffected. LREE and HREE recovery values of 38.3% and 21.3%, respectively, were achieved using a 50 g/L sulfuric acid solution at 5% solid concentration and a solution temperature of 75 ⁰C for 2 hours. Comparatively, direct acid baking at 250 °C provided substantial increased LREE and HREE recovery values to approximately 49.4% and 53.0%, respectively, using an equivalent acid dosage. Recoveries were maximized to 77.0% and 79.6% for LREE and HREE, respectively, by roasting followed by acid baking. Similar results were obtained from the treatment of a second bituminous coal source. Due to strong correlations between REE and Al recovery values, tests were performed on kaolinite and illite, which were prominent clay minerals within the source coals. These experiments revealed that the REE recovery improvements were likely a result of dehydroxylation of clays and subsequent release and decomposition of REE-bearing minerals such as monazite, xenotime and zircon. Subsequently, a parametric study was conducted to identify the impact of acid baking parameters on rare earth element recovery. The factors investigated using a three-level statistical experimental program were acid baking time, acid solution concentration, baking temperature, and acid solution-to-solids ratio which were found to significantly impact REE and contaminant element (Al, Fe, and Ca) recovery. An increase in baking temperature up to around 250 ⁰C improved the light and heavy REE recovery values by more than 50 absolute percentage points relative to performances achieved when direct leaching. As aforementioned, acid baking was needed to both decompose the clay minerals and liberate the REE minerals, which allowed access for the acid to solubilize the REEs. Acid concentration of the solution used for acid baking was studied as a means of minimizing the amount of acid needed to achieve a target REE recovery. However, thermo-gravimetric and differential scanning calorimetry analysis (TGA-DSC) of sulfuric acid under oxidizing atmosphere revealed that the addition of water decreased the evaporation temperature, which explains the lower REE recovery values obtained when using acid concentrations less than 100%. Using pure sulfuric acid at an acid-to-solid ratio of 0.8:1 resulted in recovery values of around 70% for both LREEs and HREEs. The decomposition reaction time was relatively quick with 65% of the TREEs recovered within the first 10 minutes. Following the identification of optimum operating conditions through the parametric study, a systematic leaching study was carried out to examine the impact of leaching parameters, such as solid-to-liquid (S/L) ratio, temperature, and time, on REE recovery using acid baking conditions of 1:1 acid to solids ratio at 250 °C for 30 minutes. The solid-to-liquid ratio was varied from 1-20% by weight at 25 °C, 50 °C, and 75 °C solution temperatures. The results indicated that reaction time and solution temperature considerably impacted the recovery of heavy and light REEs. Interestingly, LREE recovery reduced from 68% at 5% S/L to 58% at 20%S/L, whereas HREE recovery of 78% remained unaffected. The decrease in the LREE recovery was determined to be due to La and Ce precipitation, likely through isomorphic substitution with calcium in gypsum. The kinetic data indicated that 67% LREE and 77% HREE recovery could be obtained within the first 15 minutes of the reaction, suggesting fast reaction kinetics. Furthermore, raising the solution temperature from 25 °C to 75 °C increased the LREE and HREE recovery from 60% and 32% to 67% and 79%, respectively. The kinetic modeling results demonstrated that the rate-limiting step in the LREE dissolution was diffusion and chemical reaction, whereas the HREE extraction was controlled by only chemical reaction. The leaching study concluded that using 20% S/L at 75 °C for 15 minutes maximized LREE and HREE recovery. The lab-scale precipitation study showed that Fe and Al in solution could be removed at pH 4.5 followed by REE precipitation at pH 6.0 using 6 mol/L NaOH. Finally, the bench-scale data was used to develop a process flowsheet for REE recovery from low-grade bituminous coal sources using acid baking. Finally, based on the proposed flowsheet, a concentrated RE-cake obtained through selective precipitation at pH 6.5 was re-leached using HCl at pH 1.5. The resultant leachate was used to identify the impact of various operating parameters on REE recovery and purity with an aim to maximize REE precipitation efficiency while minimizing the oxalic acid dosage. The operating parameters for this investigation were oxalic acid dosage, iron (III) contamination, solution pH and temperature. The resultant model suggested that oxalic acid dosage and reaction pH are the most significant factors for the REE precipitation efficiency, followed by the interaction of oxalic dosage and Fe concentration. Test results indicated that increasing the oxalic acid concentration from 0g/L to 80g/L improved the REE precipitation efficiency from approximately 4.2% to 95.0%. Furthermore, raising the solution pH from 0.5 to 2.5 considerably enhanced the precipitation efficiency from 0.0% to 98.9%. A solution temperature elevation decreased REE recovery, which indicated an exothermic reaction between REEs and oxalate anions. Finally, a high level of Fe contamination adversely impacted REE precipitation efficiency. The speciation analysis revealed that the dominant iron species in the solution system were Fe-(C₂O₄)₃³⁻, Fe-(C₂O₄)²⁻, and Fe-(C₂O₄)⁺, which consumed the majority of the oxalate anions

rare earth elements, acid baking, high-temperature↗

DOE OSTI2020

Contaminant Migration Modeling to Support the In Situ Decommissioning of Hardened Nuclear Facilities - 20215

The decommissioning of hardened nuclear facilities provides a unique challenge in balancing current worker dose with exposure to future receptors and media. In situ decommissioning (ISD) is a cost-effective and safe option for the closure of such facilities but requires a detailed understanding of the threat that radioactive and hazardous constituents remaining in the facilities pose to groundwater and surrounding surface water. The Savannah River Site (SRS) extensively employs contaminant migration models within the decommissioning process to develop site-specific removal, grouting, and monitoring strategies in support of safe and effective final end states of nuclear facilities. This work discusses the use of contaminant migration modeling in the ISD process at SRS, including specific examples from the closure of P-Reactor and R-Reactor, Building 235-F, F-Canyon and F/H Laboratory Complex. Migration models developed during the closure of P-Reactor and R-Reactor were divided into four source areas: the reactor vessel, the process area, the disassembly basin, and the purification wing. Each source area was assigned a specific inventory and migration pathway and was then subject to varying hypothetical removal, capping, and grouting schemes. Modeling indicated that groundwater Maximum Concentration Limits (MCLs) might be exceeded if no action was taken for eleven and ten constituents of concern (COCs) at P-Reactor and R-Reactor, respectively. These exceedances could occur in as few as 200 to 500 years. Alternatively, the migration modeling demonstrated that the selected ISD actions reduced contaminant mobility which allowed for significant radioactive decay and resulted in fewer predicted exceedances of groundwater MCLs (five COCs for P-Reactor; eight COCs for R-Reactor). In response to the modeling results for P-Reactor and R-Reactor, effectiveness monitoring programs were developed to target contaminants, specific to each reactor, that may migrate to groundwater. Contaminant migration modeling also revealed that roof collapse was a large factor in the release of COCs to the environment, giving rise to roof improvements, and an inspection and vegetation control program to ensure roof stability over time. Contaminant migration modeling is also aiding in the closure planning for hardened facilities in F Area. Building 235-F housed the Actinide Billet Line, which produced Np-237 billets for irradiation in SRS reactors, and the Plutonium Fuel Form (PuFF) facility that produced Pu-238 heat sources for the space program. As a result of these missions, areas within Building 235-F contain considerable residual amounts of both Pu-238 and Np-237. Contaminant migration modeling of Building 235-F was originally performed in 2012 to identify the feasibility of ISD and the amount of radioactive material removal required to prevent the exceedance of groundwater MCLs. The original model indicated that a 60% reduction in the PuFF facility Pu-238 inventory could keep groundwater concentrations below standards, while Np-237 did not pose a threat to groundwater. However, updates to the model with an emphasis on source impact pathways revealed that, due to the orientation of the source areas relative to groundwater flow, no amount of reasonable removal of Pu-238 would keep groundwater concentrations below MCLs and that Np-237 could be a large contributor to localized MCL exceedances. With this insight, the refined 2019 model is being used to assist in the development of grouting plans specific to each facility source area, where bentonite may be utilized to slow the migration of Pu-238 and its daughter products from the PuFF facility and a reducing grout may decrease Np-237 transport by ensuring the nuclide remains in the less mobile +IV oxidation state. The beginning phases of contaminant migration modeling are underway for F-Canyon and associated facilities using lessons learned from the Reactors and Building 235-F. A contaminant migration pathway, similar to the pathway used for the reactor vessels, is being developed for the hot and warm canyons. The F-Canyon inventories are being spatially refined to identify specific and localized source zones, comparable to Building 235-F, that may impact groundwater. Contaminant migration modeling provides vital input within the ISD process, from facility investigation to post closure effectiveness monitoring, making it a valuable tool in the development of safe and effective end states for hardened nuclear facilities at SRS. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Exploratory Synthesis for Reactive f-Element Separations without Solvent

Solvent extraction is commonly used to separate different f-metals found in spent nuclear fuel, but this process results in large volumes of highly contaminated liquid waste that must be remediated or stored at significant expense. The project funded under this award was aimed at addressing solvent-related issues encountered in conventional f-metal separations. Our strategy focused on using solvent-free mechanochemical reactions to prepare lanthanide and actinide borohydride complexes so that they could be separated based on differences in their volatility. Key deliverables described in this report include proof-of-principle results demonstrating that borohydrides called aminodiboranates can be used for volatile lanthanide/lanthanide and lanthanide/uranium separations, as we proposed. Moreover, exploration of a closely related class of borohydrides called phosphinodiboranates allowed us to identify underlying chemical factors that control the volatility of trivalent lanthanide and uranium borohydride complexes with identical structures. Details of published and pending research products are provided, and these include comprehensive synthesis and characterization efforts required to support fundamental studies related to the proposed separations. These technical efforts supported the training of nine graduate students and three undergraduate researchers, and they established air-sensitive transuranic capabilities at the University of Iowa to enhance radiochemical workforce development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Exploratory Synthesis for Reactive f-Element Separations without Solvent

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Sustaining On-going Risk Communication at the Riverton, Wyoming, Processing Site - 20310

An environmental risk assessment report has been completed to provide an updated assessment regarding current site conditions for the Riverton, Wyoming, Processing site. Argonne National Laboratory conducted the assessment in collaboration with the U.S Department of Energy (DOE) Office of Legacy Management (LM) and the Northern Arapaho Natural Resources Office (NANRO). The data quality objectives process conducted confirmed that data from plants growing on the Riverton site would be useful and would address an outstanding concern. Data available from site soil, groundwater, and surface water were also used in the assessment in conjunction with the new plant data. A plant survey was then conducted in 2018 to identify the plants at the Riverton site with known traditional Native American cultural uses for sampling and analysis. Laboratory analysis was conducted on the plant samples for the contaminants of concern. Samples were collected from plants growing on the groundwater plume area of the site, and the same was done for eight other areas not affected by the groundwater plume but still within the institutional control boundary. These eight areas served as reference areas for this study. This human health and ecological assessment update provide the quantitative risk information that was qualitatively addressed in a 1995 Risk Assessment Report on plants, livestock, and surface water exposures at the Riverton site [1]. The conditions at the Riverton site are protective of human health and the environment given the results of the update, in combination with past completed remedial action and ongoing monitoring activities and IC implementation. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Study of an Unrefined Humate Solution as a Possible Attenuation-based Remedy for Uranium Contamination in Acidic Groundwater - 20351

The Savannah River Site (SRS), joined the environmental cleanup program in 1981 after the Cold War, and was designated as a hazardous waste management facility. About 1.8 billion gallons of acid wastes were disposed into the F/H Area Seepage Basin that included many radionuclides and dissolved metals, resulting in highly contaminated groundwater plumes with pH of 3 - 5.5. The acidity of the plumes contributes to the mobility of several constituents of concern (COC) such as H-3, U-238, I-129, and Sr-90 for the F-Area plume and H-3, Sr-90 and mercury for the H-Area plume. An active treatment (pump-and-treat and re-injection) system was constructed and put in place in 1997 to address the removal of metals and radionuclides from the contaminated groundwater. As remediation projects advanced, active treatments were transitioned to more passive or enhanced-passive approaches such as the subsurface barrier with base injection system, which has been controlling the mobility of contaminants. However, new and more efficient attenuation-based remedies are always sought. Several studies have proposed that humic substances can be used to remediate sites contaminated with heavy metals by creating a permeable reactive barrier. Humic substances (HS) are major components of soil organic matter. HS are polyfunctional organic macromolecules formed by the chemo-microbiological decomposition of biomass or dead organic matter. These substances are usually divided into three main fractions: humin (insoluble at all pH values), humic acid (soluble at pH greater than 3.5), and fulvic acid (soluble at all pH values). Humic substances are major components of the soil at SRS and, in addition, are also helpful in the removal process of uranium. This research focuses on uranium (VI), which is a key contaminant of concern in the F-Area groundwater plume. The interaction of uranium with sediment in the presence or absence of humic substances involves complex mechanisms that are not yet well understood. The interaction of U(VI) with humic substances can affect the adsorption of U on sediment, altering its mobility in the subsurface. The objective of this study is to study the mobility of uranium in the presence of humic acid and to determine if sediments amended by humic acid can enhance the sorption of heavy metals onto sediments. In this research, experiments were conducted using background (clean) F-Area aquifer sediments to understand and predict uranium mobility. A blended material, humate, containing both humic and fulvic acids and a chemically modified humate (KW15 modified humic or mod-HA) was studied as a possible amendment for uranium remediation in SRS groundwater. Batch experiments were conducted in triplicates using 20 ml of aqueous suspension in DI water containing SRS sediment and mod-HA and studied the effect of pH, kinetics of humate sorption onto SRS sediment and also studied the sorption of uranium onto mod-HA amended SRS sediment. Results indicate that mod-HA amended sediment increases uranium removal significantly. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

National Ignition Facility. Facility and Infrastructure Systems Maintenance Plan

Ensuring the reliability of the NIF, including its support systems, laser systems, target diagnostic systems, and utilities, is essential to the availability of the NIF in its support of NNSA missions. NIF is a key capability in the DOE Stockpile Stewardship Program and supports high energy physics experiments for nuclear weapons, energy, and astrophysics applications. High system reliability provides opportunities for shots and scientific discoveries with opportunities to enhance and upgrade capabilities. This Maintenance Plan (MP) identifies the policies and procedures used to perform and support asset management of the NIF Facility and Infrastructure Systems (FInS), NIF Lasers & Alignment (LASE), NIF Target Experimental Operations (TOPS), NIF Target Area Science and Engineering (TASE), and NIF&PS Control Systems (NCS). The FInS systems include the facility, HVAC, contamination control, beampath, and Line Replaceable Units (LRUs) as well as utilities which create the beampath environments, such as vacuum, argon, or clean dry air. The LASE systems are Programmatic systems which include laser diagnostics, alignment, power conditioning, pulsed power, and input laser systems. The TOPS and TASE systems are also Programmatic systems which include target and diagnostic delivery systems and positioners, many different insertable and fixed target diagnostics, and cryogenic and target gas fill systems. Finally, the NCS systems include both software and hardware for industrial and shot operation control systems. Policies governing administrative and operational practices related to maintenance of FInS, LASE, TOPS, TASE, and NCS systems are described in this plan. In addition, the plan provides processes and procedures for managing, tracking, and documenting the work. This document, the NIF Operations Management Plan, NIF-5020544 (Ref. 1), and NIF Shot Operations Plan, NIF-5018506 (Ref. 2), together satisfy the requirements of the Conduct of Operations. Duties, responsibilities, and reporting requirements of the various positions associated with FInS, LASE, and TOPS maintenance are detailed in this plan. The FInS systems include both Real Property systems with asset management requirements specified in DOE Order 430.1C (Ref. 3) and Programmatic systems. In addition, for FInS, there is a list of the System Level Maintenance Plans (SLMPs) in NIF-1007419198 (Ref. 4) which provide the system descriptions and maintenance plan and schedule. In addition, the list includes the Reliability Centered Maintenance (RCM) and Experience Centered Maintenance (ECM) evaluations that have been performed for applicable FInS systems as well as reliability criticality per Section 3.5. The -AM version of the NIF Maintenance Plan focuses on the reliability program for FInS, LASE, TOPS, TASE, and NCS within the context of the overall NIF Reliability, Availability, and Maintainability (RAM) program and incorporates changes since the -AL version from August 2011 and has been updated to be fully consistent with the updates to Ref. 1. It also includes asset management considerations, updates to the Work Order (WO) process within the NIF Computerized Maintenance Management System (CMMS) which is EAM infor® System Maintenance and Reliability Tracking (SMaRT) (Ref. 5), and updates to metrics and key performance indicators (KPIs).

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2019

Phosphate amendments for chemical immobilization of uranium in contaminated soil

Uranium (U) contamination is a major environmental problem associated with the mining and processing of nuclear materials for both weapons and power production. When possible, in situ soil remediation techniques are preferable for reducing the risk associated with diffuse low-level U contamination. Uranium is known to form sparingly soluble phosphate compounds that persist in the environment. Therefore, batch experiments were performed to evaluate the efficacy of three phosphate amendments, hydroxyapatite (HA), sodium phytate (IP6) and sodium tripolyphosphate (TPP), to immobilize U in contaminated sediments. The amendments were added at equivalent phosphorus (P) concentrations and then equilibrated under a range of test conditions, with changes in soluble U and Ptotal monitored at pre-set time intervals. Only HA was effective at reducing the soluble U soil fraction when compared to the control, with IP6 and TPP increasing the soluble U soil fraction. After equilibration, changes in contaminant partitioning in the amended sediments were evaluated using operational extraction methods. Sequential extraction results for HA generally indicated a transfer of U from labile to more recalcitrant phases, while the results for IP6 and TPP were more ambiguous.

Uranyl↗

DOE OSTI2019

H-Canyon Tunnel Inspection System

Cable Analysis: The crawlers is controlled remotely via a long coax cable. In order to make sure we do not damage the cable which could cut our contact (data/power/control), we had to determine the bend radius of it at certain locations. This was done with dimensional analysis in Creo and inputting the information into a MATLAB program. Engineering Drawings: Since many of the crawlers parts, such as the main body, needed to be machined, part drawings were needed to communicate the details necessary for manufacture. Project Overview: The H-Canyon Ventilation Exhaust Tunnel due both to its long service history and exposure to aggressive process offgas chemistry has experienced degradation. In order to allow visual inspection of the condition of the radioactively-contaminated tunnel, a remote crawler was designed to deliver cameras as needed to return high definition video. My involvement included Vendor Searches, Cable Analysis, Thermal Analysis, and Engineering Drawings. Thermal Analysis: In order to see if internal active cooling is needed for the crawler, simplified thermal models were designed to approximate the internal temperatures: Conduction (assumes all heat sources are thermally-coupled to the crawler body); Convection (assumes no heat sources are thermally-bonded to crawler). Going Forward: Continue refining the cable analysis as the crawler model is updated and refined. Use my knowledge gained here to further my skills in engineering.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Assessment the leaching characteristics and long-term leaching behavior of some radionuclides from synthesized zeolite cement matrix

Highlights: • Synthesis and characterization of zeolite cement synthesized from fly ash • Leaching tests were used to assess the release rate of {sup 85}Sr and {sup 60}Co radionuclides. • Simple mathematical models were used to detect leaching mechanisms. • Long-term leaching behavior of {sup 85}Sr and {sup 60}Co from cementitious matrix was assessed. The development of cementitious materials remains a vital goal to produce valuable products with good mechanical, physical and chemical properties suitable for the safe disposal of concentrated radionuclides resulted from the treatment of contaminated solutions. In this paper, zeolite cement with good properties was laboratory synthesized from industrial by-products fly ash and characterized using various characterization techniques. The leaching characteristics of strontium and cobalt radionuclides from the synthesized zeolite cement were scrutinized conforming with the standard leaching methodology of International Atomic Energy Authority (IAEA). A mechanical strength assessment was executed to characterize the extent of immobilization process of the solidified matrices. The cumulative leaching fraction (φ) of the two studied radionuclides was found to be less than 5% in all examined conditions, which implies the applicability of the IAEA-recommended methodology for estimating the diffusion coefficient. The experimental leaching data were regressed nonlinearly to various mathematical kinetic models to assess the controlling leaching mechanism and to determine the leaching parameters. The regression results indicated that strontium ({sup 85}Sr) and cobalt ({sup 60}Co) leaching resulted from two succeeding mechanisms: as first order kinetic reaction, and then diffusion. The calculated values of leachability indices signify that the performance of each of the studied matrices is within an acceptable range. A simplified mathematical model, rooted in the first order reaction and diffusion mechanisms, was simulated to predict the radionuclides leaching rates from zeolite cement matrices. By comparing the synthesized zeolite cement with other cementitious materials, it can be concluded that the synthesized material can be classified as an efficient material suitable to immobilize {sup 85}Sr and {sup 60}Co from radioactive wastes. The acquired findings demonstrated that the studied immobilized waste matrices have acceptable mechanical effectiveness.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Characterizing the Influence of Organic Polymers on the Specific Reactivity of Particulate Remedial Amendments

Commercially available particulate amendments demonstrate high reactivity for effective treatment of water soluble organic and inorganic contaminants in laboratory studies; however, transport of these particles is constrained in the subsurface. In many field applications, particulate amendments are mixed with organic polymers to enhance mobility for direct push applications or stabilize suspensions for high mass loadings. As such, the interactions between particulate amendments, organic polymers and contaminant species need to be systematically investigated to properly understand mechanistic processes that facilitate predictive performance metrics for specific applications in situ . In this study, batch experiments were conducted to quantify the effects of organic polymers (xanthan gum, guar gum, and sodium alginate), polymer concentration (800 and 4,000 mg/L), and aging (up to 28 days) on chromate treatment rate and capacity by two classes of amendments: reductants [granular zero-valent iron (gZVI), micron-ZVI (mZVI), sulfur modified iron (SMI)], and an adsorbent (bismuth sub-nitrate). When particulate amendments were suspended in polymer solutions, reductants retained between 84–100% of the amendment treatment capacity. Conversely, the adsorbent maintained 63–97% relative treatment capacity of the no-polymer control. Polymer solutions had a more pronounced impact on the rate of chromate removal; first order rates of chemical reduction decreased by as much as 70% and adsorption by up to 81% relative to the no-polymer controls. Polymer–amendment aging experiments also showed decreased Cr(VI) treatment capacity; reductants decreased by as much as 24% and adsorption decreased by as much as 44% after 28 days of incubation. While polymer suspensions are needed to aid the injection of particulate amendments into the subsurface, the results from this study indicate potential losses of treatment capacity and a decrease in the rate of remedial performance due to the physical and chemical interactions between polymer suspensions and reactive particulate amendments. Simple batch systems provide baseline characterization of tripartite interactions for the removal of Cr(VI). Additional work is needed to quantify the full impact of polymers on remedial outcomes under site relevant conditions at field scale.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Designing a Site Closure Strategy for Uranium in Groundwater and Surface Water - 19534

A site closure strategy was designed and mapped for residual uranium present in groundwater and surface water at the US DOE Office of Legacy Management (LM) Monticello Mill Tailings Site (MMTS) Operable Unit (OU) III, which is regulated under CERCLA. The MMTS is a former mill site that was used to process uranium and vanadium ore in southeastern Utah until 1960. OU III includes surface water in Montezuma Creek and groundwater present in a shallow alluvial aquifer along the creek valley for several kilometers downgradient of the former mill site. The current remedy consists of an operating pump-and-treat system, monitored natural attenuation (MNA), and institutional controls (ICs). Performance evaluations indicate that a prolonged restoration period is likely, as well as an asymptotic trend in uranium concentrations that still exceed the remediation goal. Multiple strategies and scenarios were evaluated before selecting a preferred site closure strategy. Recommendations were developed to support advancing the site towards closure over the next few years and guide the process of regulatory interactions and decision making at the MMTS OU III. Site closure is an important milestone that reflects successful remedial progress at LM sites. Post-closure site management would be maintained to ensure conditions are protective of human health and the environment. The site closure strategy was considered in the context of site remedial progress. The primary sources of groundwater contamination have been removed, including mill tailings and contaminated soils, sediment, and debris. Five-year reviews have regularly concluded that the remedy is protective of human health and environment and that ICs are effective in preventing exposure to contaminated groundwater. The affected aquifer is low-yielding and has no history of domestic use. In 2004, the final remedy selected in the Record of Decision (ROD) was MNA with ICs. However, a pump-and-treat system was installed and continues to operate as a contingency remedy in the area with the highest residual uranium concentrations. The need for a contingency pump-and-treat system was triggered by a departure of the long-term monitoring data from model projections that were used as the basis for remedy performance metrics specified in the ROD. In 2015, the pump-and-treat system was expanded. Average uranium concentrations have declined locally over time. However, monitoring data and column studies indicate that the system effectiveness will eventually become ineffective in reducing uranium concentrations, likely due to the reequilibration of uranium present in the solid matrix in various states (i.e., sorbed, precipitated). Currently, there are no agreed-upon metrics for discontinuing the contingency pump-and-treat system. Three closure strategies effectively applied at other CERCLA sites were considered at MMTS OU III: (1) restoring natural attenuation conditions and conducting MNA; (2) applying alternate concentration limits (ACLs); and (3) waiving a remedial goal based on technical impracticability (TI). Each closure strategy was evaluated in the following manner: (1) identifying the criteria and requirements associated with current regulations, policy, and guidance, (2) assessing the ability to meet those criteria based on the current site knowledge and the conceptual site model, and (3) identifying data gaps that need to be filled to further assess the closure strategy. Following this evaluation, a preferred closure strategy was selected: to transition to a remedy based on MNA and maintenance of ICs, without active remediation. Several scenarios for transitioning to the preferred closure strategy were identified. Each scenario consisted of 'if/then logic' associated with a larger decision diagram. The decision diagram considered the current conceptual site model (CSM) and potential outcomes of studies that will be conducted to fill data gaps, as well as the performance of the existing treatment system and long-term monitoring data. Two scenarios for transitioning to the preferred closure strategy were highlighted for future planning and were described in detail. For both scenarios, the preferred closure strategy includes demonstrating criteria for MNA acceptance, pump-and-treat termination, long-term monitoring, and eventual site delisting. Recommended actions over the next few years were also developed, including updating the CSM, conducting numerical modeling to predict remedial performance and time frames, conducting geochemical analyses to assess uranium fate and transport, and summarizing the lines of evidence and basis for MNA. This detailed example of the development of a site-specific closure strategy provides the thought process and decision logic used to assess uncertainty using an if/then framework; identify common elements and recommended actions to advance the site towards closure; and navigate the inherent uncertainty in the timing of future events, outcome of regulatory discussions, and remedial progress over time that is common to many complex US DOE facilities. In addition, the national regulations, policy, guidance, and state of practice regarding commonly used site closure strategies was summarized for consideration, including MNA, ACLs, and TI. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2018

IAEA Initiatives that Integrate Stakeholders, Models and Decision Making - 18646

The International Atomic Energy Agency (IAEA) has initiated an effort to provide stakeholder support services as part of Phase II of the Constraints to Implementing Decommissioning and Environmental Remediation (CIDER II) programs. The intent of this sub-group of CIDER II is to provide members states support in areas of stakeholder communication, engagement and participation, with the goal of building trust in decommissioning and environmental remediation (D and ER) decisions for radioactive contamination and facilities. IAEA has also initiated a follow-on effort to address Modeling and Data for Radiological Impact Assessments (MODARIA II), which is aimed at enhancing the capabilities of Member States to simulate radionuclide transfer in the environment, and to ensure appropriate levels of protection from ionizing radiation. Working Group 1 of MODARIA II is focused on the integration of modeling and decision analysis. These two groups have complementary and supporting objectives, which provides an opportunity for collaboration and mutual benefit. The technical integrator is the approach of structured decision making, which follows a five-step process that combines stakeholder values with models through a technically defensible decision analysis. Briefly, the steps are: 1. Provide the context and decision context for the problem; 2. Obtain costs, values and concerns from stakeholders, to develop objectives that need to be achieved (e.g., improve human health, minimize costs, increase jobs); 3. Identify options that might achieve the objectives (e.g., cleanup, institutional controls, education); 4. Develop probabilistic models that connect options to objectives so that the objectives can be evaluated collectively (e.g., a fate and transport and risk model to address the objective of reducing human health risk, a cost model to address costs of taking action); and, 5. Model evaluation, including sensitivity analysis, to determine if an action can be taken with sufficient certainty, or if collection of more data is needed to decrease uncertainty before a decision is made. This approach also supports adaptive management as new data are collected. This approach clarifies the roles of stakeholders and subject matter experts in the decision-making process, where stakeholders specify values, and subject matter experts focus on the models that are needed to evaluate the options. It also provides a technically defensible, reproducible, transparent and traceable approach to all of the components necessary to properly solve the types of complex decision problems that plague radioactive waste management, decommissioning and environmental remediation. This paper introduces the major challenges to implementing such a broad scale of decision analysis, and approaches to overcoming those challenges, which include not only the technical challenges, but also the need to develop capacity in a range of skills not usually accommodated in environmental modeling and includes the need for the IAEA to address decision making in different countries, and with different cultures, religions, political affiliations, and languages. This paper explores the potential for IAEA to benefit from both the CIDER II and MODARIA II programs, and hence to develop a fully integrated approach to effective decision making for radioactive waste management and environmental remediation. Note that there are many people involved in these efforts at the IAEA, and credit belongs to those people for the progress that has been made to date. Our intent here is simply to introduce these IAEA programs at the WM2018 Symposium to provide our perspective and some awareness of some of the directions in which IAEA appears to be headed regarding stakeholder engagement, environmental and risk modeling, data science, and decision analysis. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Development of ultra-pure gadolinium sulfate for the Super-Kamiokande gadolinium project

This paper reports the development and detailed properties of about 13 metric tons of gadolinium sulfate octahydrate, Gd 2 (SO 4 ) 3 • 8H 2 O⁠, which has been dissolved into Super-Kamiokande (SK) in the summer of 2020. We evaluate the impact of radioactive impurities in Gd 2 (SO 4 ) 3 • 8H 2 O on diffuse supernova neutrino background searches and solar neutrino observation and confirm the need to reduce radioactive and fluorescent impurities by about three orders of magnitude from commercially available high-purity Gd 2 (SO 4 ) 3 • 8H 2 O⁠. In order to produce ultra-high-purity Gd 2 (SO 4 ) 3 • 8H 2 O, we have developed a method to remove impurities from gadolinium oxide, Gd 2 O 3 , consisting of acid dissolution, solvent extraction, and pH control processes, followed by a high-purity sulfation process. All of the produced ultra-high-purity Gd 2 (SO 4 ) 3 • 8H 2 O is assayed by inductively coupled plasma mass spectrometry and high-purity germanium detectors to evaluate its quality. Because of the long measurement time of high-purity germanium detectors, we have employed several underground laboratories for making parallel measurements including the Laboratorio Subterráneo de Canfranc in Spain, Boulby in the UK, and Kamioka in Japan. In the first half of production, the measured batch purities were found to be consistent with the specifications. However, in the latter half, the Gd 2 (SO 4 ) 3 • 8H 2 O contained one order of magnitude more 228Ra than the budgeted mean contamination. This was correlated with the corresponding characteristics of the raw material Gd 2 O 3 , in which an intrinsically large contamination was present. Based on their modest impact on SK physics, they were nevertheless introduced into the detector. To reduce 228 Ra for the next stage of gadolinium loading to SK, a new process has been successfully established.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Assessing the Ability of Developmentally Precocious Estrogen Signaling to Recapitulate Ovarian Transcriptomes and Follicle Dynamics in Alligators from a Contaminated Lake

Concern has grown in recent decades over anthropogenic contaminants that interfere with the functioning of endocrine hormones. However, mechanisms connecting developmental processes to pathologies associated with endocrine-disrupting chemical (EDC) exposure are poorly understood in naturally exposed populations. We sought to a) characterize divergence in ovarian transcriptomic and follicular profiles between alligators originating from a historically EDC-contaminated site, Lake Apopka, and a reference site; b) test the ability of developmentally precocious estrogen exposure to recapitulate site-associated patterns of divergence; and c) test whether treatment with exogenous follicle-stimulating hormone (FSH) is capable of rescuing phenotypes associated with contaminant exposure and/or embryonic estrogen treatment. Alligators eggs were collected from a contaminated site and a reference site, and a subset of eggs from the reference site were treated with estradiol (E2) during embryonic development prior to gonadal differentiation. After hatching, alligators were raised under controlled laboratory settings for 5 months. Juveniles from both sites were divided and treated with exogenous FSH. Histological analyses and RNA-sequencing were conducted to characterize divergence in ovarian follicle dynamics and transcriptomes between sites, between reference and E2-treated animals, and between FSH-treated and nontreated animals. We observed broad site-of-origin divergence in ovarian transcriptomes and reductions in ovarian follicle density between juvenile alligators from Lake Apopka and the reference site. Treating embryos from the reference site with E2 overwhelmingly recapitulated transcriptional and histological alterations observed in Lake Apopka juveniles. Ovarian phenotypes observed in Lake Apopka alligators or resulting from estrogen treatment were only partially rescued by treatment with exogenous FSH. Recapitulation of ovarian abnormalities by precocious E2 revealed a relatively simple mechanism underlying contaminant-induced pathologies in a historical example of environmental endocrine disruption. Findings reported here support a model where the developmental timing of estrogen signaling has the potential to permanently alter ovarian organization and function.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2019

From Grain to Floodplain: Evaluating heterogeneity of floodplain hydrostatigraphy using sedimentology, geophysics, and remote sensing

Stratigraphy is a fundamental component of floodplain heterogeneity and hydraulic conductivity and connectivity of alluvial aquifers, which affect hydrologic processes such as groundwater flow and hyporheic exchange. Watershed–scale hydrological models commonly simplify the sedimentology and stratigraphy of floodplains, neglecting natural floodplain heterogeneity and anisotropy. This study, conducted in the upper reach of the East River in the East River Basin, Colorado, USA, combines point–, meander–, and floodplain–scale data to determine key features of alluvial aquifers important for estimating hydrologic processes. We compare stratigraphy of two meanders with disparate geometries to explore floodplain heterogeneity and connectivity controls on flow and transport. Meander shape, orientation, and internal stratigraphy affected residence time estimates of laterally exchanged hyporheic water. Although the two meanders share a sediment source, vegetation, and climate, their divergent river migration histories resulted in contrasting meander hydrofacies. In turn, the extent and orientation of these elements controlled the effective hydraulic conductivity and, ultimately, estimates of groundwater transport and hyporheic residence times. Additionally, the meanders’ orientation relative to the valley gradient impacted the hydraulic gradient across the meanders—a key control of groundwater velocity. In conclusion, we combine our field data with remotely sensed data and introduce a potential approach to estimate key hydrostratigraphic packages across floodplains. Prospective applications include contaminant transport studies, hyporheic models, and watershed models.

58 GEOSCIENCES↗

DOE OSTI2021

Organic contamination detection for isotopic analysis of water by laser spectroscopy

Hydrogen and oxygen stable isotope ratios (δ 2 H, δ 17 O, and δ 18 O values) are commonly used tracers of water. These ratios can be measured by isotope ratio infrared spectroscopy (IRIS). However, IRIS approaches are prone to errors induced by organic compounds present in plant, soil, and natural water samples. A novel approach using 17 O-excess values has shown promise for flagging spectrally contaminated plant samples during IRIS analysis. A systematic assessment of this flagging system is needed to prove it useful. Errors induced by methanol and ethanol water mixtures on measured IRIS and isotope ratio mass spectrometry (IRMS) results were evaluated. For IRIS analyses both liquid- and vapour-mode (via direct vapour equilibration) methods are used. The δ 2 H, δ 17 O, and δ 18 O values were measured and compared with known reference values to determine the errors induced by methanol and ethanol contamination. In addition, the 17 O-excess contamination detection approach was tested. This is a post-processing detection tool for both liquid and vapour IRIS triple-isotope analyses, utilizing calculated 17 O-excess values to flag contaminated samples. Organic contamination induced significant errors in IRIS results, not seen in IRMS results. Methanol caused larger errors than ethanol. Results from vapour-IRIS analyses had larger errors than those from liquid-IRIS analyses. The 17 O-excess approach identified methanol driven error in liquid- and vapour-mode IRIS samples at levels where isotope results became unacceptably erroneous. For ethanol contaminated samples, a mix of erroneous and correct flagging occurred with the 17 O-excess method. Here our results indicate that methanol is the more problematic contaminant for data corruption. The 17 O-excess method was therefore useful for data quality control. Organic contamination caused significant errors in IRIS stable isotope results. These errors were larger during vapour analyses than during liquid IRIS analyses, and larger for methanol than ethanol contamination. The 17 O-excess method is highly sensitive for detecting narrowband (methanol) contamination error in vapour and liquid analysis modes in IRIS.

60 APPLIED LIFE SCIENCES↗