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DOE OSTI2020

Lessons Learned from Hanford's Purex Tunnel 2 Structural Stabilization Project - 20509

In 2019, U.S. Department of Energy (DOE) contractor CH2M Hill Plateau Remediation Company (CHPRC) completed structurally stabilizing the Plutonium Uranium Extraction Plant (Purex) waste storage Tunnel 2 with engineered grout. This action significantly reduced risk to Hanford workers, the surrounding community and environment by preventing future collapse of the tunnel and possible release of radioactive materials. Decades of plutonium production at the Purex facility required construction of two large underground tunnels for storage of highly contaminated plutonium processing equipment that had failed during the operation of Purex and other facilities across the Hanford Site. Following the partial collapse of Purex Tunnel 1 on May 9, 2017, DOE and CHPRC took immediate action to safely stabilize the collapsed section of the tunnel. The hole in the tunnel was filled the next day as a temporary stabilization measure, and no contamination was detected as a result of the partial collapse of the tunnel. Workers then stabilized Tunnel 1 in its entirety by filling with engineered grout, which also encapsulated the radioactive equipment and railcars within the tunnel. Grouting eliminated the risk of further collapse and stabilized the tunnel contents, all while not precluding future remedial actions or final closure decisions. While conducting an integrity analysis of Tunnel 1 by using construction drawings, photos and other historical documents, project teams also analyzed the much larger Purex Tunnel 2. The analysis found Tunnel 2 did not meet current codes for structural integrity, and it may not be able to bear the weight of the soil above the tunnel. Therefore, it was determined that Tunnel 2 was also at risk of collapse. DoE's independent panel of experts determined grouting to be the best choice for stabilizing Tunnel 2 because it provides the highest level of stability and protection, and does not preclude future remedial actions. DOE authorized CHPRC to commence work and the Purex Tunnel 2 Structural Stabilization Project was launched in December of 2017. The paper will discuss the process of recognizing the following critical aspects and risks associated with stabilizing Tunnel 2, and the actions taken by the project team to mitigate these risks, including: - Tunnel investigation and data collection to assist with future remediation; - On-site batching and mock-ups to provide the large quantity of grout required for stabilizing the tunnel; - Workforce involvement and innovative actions that mitigated the project's most significant potential hazards, including traffic control; - Project team high level of execution translated into successful project execution. Sharing lessons learned from this critical risk-reduction effort can enhance the safety and efficiency of other complex and hazardous projects across the DOE complex. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

THE DISTRIBUTION OF MASS SURFACE DENSITIES IN A HIGH-MASS PROTOCLUSTER

We study the probability distribution function (PDF) of mass surface densities, Σ, of infrared dark cloud (IRDC) G028.37+00.07 and its surrounding giant molecular cloud. This PDF constrains the physical processes, such as turbulence, magnetic fields, and self-gravity, that are expected to be controlling cloud structure and star formation activity. The chosen IRDC is of particular interest since it has almost 100,000 solar masses within a radius of 8 pc, making it one of the most massive, dense molecular structures known and is thus a potential site for the formation of a “super star cluster.” We study Σ in two ways. First, we use a combination of NIR and MIR extinction maps that are able to probe the bulk of the cloud structure up to Σ ∼ 1 g cm{sup −2}( A {sub V}≃ 200 mag). Second, we study the FIR and submillimeter dust continuum emission from the cloud utilizing Herschel -PACS and SPIRE images and paying careful attention to the effects of foreground and background contamination. We find that the PDFs from both methods, applied over a ∼20′(30 pc)-sized region that contains ≃1.5 × 10{sup 5} M {sub ⊙} and enclosing a minimum closed contour with Σ ≃ 0.013 g cm{sup −2} ( A {sub V} ≃ 3 mag), shows a lognormal shape with the peak measured at Σ ≃ 0.021 g cm{sup −2} ( A {sub V}≃ 4.7 mag). There is tentative evidence for the presence of a high-Σ power-law tail that contains from ∼3% to 8% of the mass of the cloud material. We discuss the implications of these results for the physical processes occurring in this cloud.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Oil and Natural Gas Development near and beneath Uranium Tailings Cells and Other Remediated Sites - 20358

DOE LM is responsible for maintaining remedies at more than 50 remediated sites that require active long-term surveillance and maintenance (LTS and M). Institutional controls (ICs) were established to limit human and environmental exposures to residual contamination by controlling land use, restricting access to potential hazards, and making the public aware of potential dangers from the residual contamination. ICs for each site were developed based on current and foreseeable conditions; however, these controls should evolve to mitigate potential human health and other environmental risks from unanticipated changes in activities or site conditions. Activities conducted beyond the DOE long-term care boundaries by non-DOE parties may impact the effectiveness of ICs or even the long-term stability of disposal cells and groundwater remedies. Several sites that LM manages or that will transfer to LM for LTS and M are in active oil and gas production basins. The sites are associated with uranium ore milling or nuclear test sites and have been remediated or are in the process of remediation and have no ongoing DOE mission. Particularly since 2005, hydraulic fracturing ('fracking') combined with directional drilling has dramatically increased oil and natural gas (oil/gas) production in the United States, now making it the number one hydrocarbon-producing country. Fracking has allowed production from shale and other rocks of low natural permeability that were historically not considered viable oil/gas resources. Also, because wellbores can now be drilled as many as 5 kilometers or more horizontally, hydrocarbons can be recovered from zones without having access to the surface above them. Drilling activity near Rulison, Colorado, the location of an underground nuclear detonation managed by LM, has raised public concerns that remnant radioactivity in the detonation zone could migrate to producing wells and enter the natural gas distribution system. At sites like the Falls City, Texas, Disposal site, transitioned to LM with a split estate, increased production in the region has resulted in wellbores beneath the long-term care boundary of the site. While the DOE license for Falls City was approved by the NRC in 1997 without the acquisition of the subsurface rights, NRC has raised concerns on whether this activity impacts the integrity of the cell and/or groundwater remedies. In Wyoming, LM is anticipating receiving the license for the Bear Creek site and manages the Spook site, both locations of uranium mill tailings disposal cells. These Wyoming sites are in an active region of major oil and gas development. This change in surrounding land use will require LM to work collaboratively with NRC to address these concerns. At several DOE sites radioactive waste, and often intermixed nonradioactive constituents, is permanently isolated in engineered disposal cells. At other sites, residual contamination can be present in groundwater, blast cavities, and infinite amounts within soil. Areas targeted for oil and gas development at the Texas and Wyoming sites range from depths of 2440 to 3350 meters (8000-11000 feet) below ground surface. When most site remedies were designed, oil and gas development was not considered to be an issue within the site boundary. With the more recent uses of directional drilling, fracking, and associated wastewater injections, the evaluative criteria for incoming sites and ICs for managing long-term protectiveness and regulatory compliance are changing. Although DOE surface ownership was previously thought to be a robust IC to prevent surface and subsurface development, particularly at disposal sites, that may no longer be the case. Whereas the subsurface development at Texas and Wyoming sites is currently occurring at thousands of meters beneath the surface, shallower and direct onsite development would be more of a concern for LM. The energy introduced when a well is hydraulically fractured causes microseismic events (magnitude -2 to 1.0) as the fractures propagate but does not directly cause seismic events (earthquakes) of sufficient magnitude to damage surface structures. Additionally, the extent of the hydraulic fractures is limited to the targeted depths, which are far below the surface. However, earthquakes of sufficient magnitude to damage surface structures have been attributed to the injection of wastewater into disposal wells. States that have experienced these effects have enacted regulations that limit the rate and pressures that wastewater can be injected into disposal wells. Items LM may consider are the need for monitoring the volume of water injected into nearby disposal wells and possibly installing seismic stations at sites most susceptible to damage. While the need to demonstrate that no impact from oil and gas extraction activities on a site groundwater remedy or disposal cells will vary from site to site, LM is assessing risk criteria for this activity. Though LM has not experienced an issue yet at a uranium tailings disposal site, it cannot assume that there will be none, and must address NRC concerns. LM is building on past experiences at other sites and beginning to form new processes with the hope that these concepts can be applied for other future sites. (authors)

04 OIL SHALES AND TAR SANDS↗
DOE OSTI2026

Innovative laser-based methods for monitoring fuel retention in ITER

This paper addresses the challenge of tritium inventory management in ITER and future fusion reactors, highlighting the importance of accurate tritium measurement and its spatial distribution within the vacuum vessel. Given ITER’s operational constraints, especially the limit on tritium retention, precise measurement is essential for both safety and regulatory compliance. To tackle these questions, the paper presents the T-monitor diagnostic system developed by Forschungszentrum Jülich, which uses Laser-Induced Desorption (LID) in combination with Diagnostic Residual Gas Analysis (DRGA) to measure hydrogen isotope concentrations on the surface of divertor tiles. The system integrates a high-power laser, advanced optical components, and a Fast Scanning Mirror Unit (FSMU) for accurate laser spot positioning with rapid response. Designed to measure in situ tritium retention, the diagnostic provides high-resolution spatial mapping, vital for evaluating detritiation strategies. The laser heating process increases the divertor surface temperature to 1600 K within the laser spot, promoting hydrogen isotope desorption. Accurate measurements require the precise control of laser parameters, including pulse duration and spot size, with a target relative accuracy of 20%. The optical design includes both in-vessel and ex-vessel components, such as durable high-reflectivity mirrors made of gold and copper, selected not only for their infrared performance but also for their transmission of visible wavelengths for observation purposes. To protect optical components from contamination, a pneumatic shutter is used.

Hydrogen isotopes↗
DOE OSTI2026

Advanced Test Reactor Safety Basis Update for Gas-Cooled Experiments

The Advanced Test Reactor (ATR) supports neutron irradiation of several types of experiments. One such experiment type is referred to as a gas leadout. Gas leadout experiments actively flow gas through the experiment which allows for active temperature control. It also allows for in-situ data of the experiment. For example, fission gas migration through a fuel sample can be monitored via activity of the sweep gas. Historically, ex-pile equipment and fission product monitors were housed in shielded ATR cubicles. Due to other facility updates, cubicle space is no longer available for gas leadout experiment equipment. To support continued operation of gas leadout experiments, ATR completed a safety basis update that supports a new housing for leadout equipment that may process potentially contaminated gas. In addition to the structure and associated equipment, technical safety requirements regarding handling and storage of experiments needed to be revised to support fueled gas leadout experiments and associated outage configurations. The safety basis update addressed the full lifecycle of these experiments, including experiment movement and interim storage, and credible abnormal events such as failures or leaks in contaminated gas tubing in occupied areas. This paper discusses the completed analyses performed to support the safety basis update associated with gas leadout experiments, including thermal-hydraulic evaluation, probabilistic analysis, and dose consequence analyses.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Salt Vessel-Sample Generator Interface

The goal of the salt sampling program at Argonne is to develop and deploy automated molten salt sampling approaches for interfacing relevant unit operations with salt analysis to improve the timeliness and accuracy of sampling-based accountancy measurements. One technology under development is a vacuum sampler loop module. In this system, molten salt is drawn from a process vessel through a heated sampling line and into a charge vessel. Next, one or more samples are split from the volume in the charge vessel and the remaining salt is returned to the process. The vacuum sampler loop module is being developed to interface with other sample processing and analysis modules to enable rapid at-line sample characterization. The main purpose of the vacuum sampling loop module is to enable the collection of samples that are more representative of the bulk salt by replacing traditional point samplers (i.e., dip probes) with a sampling approach that captures a larger cross section of salt. Additionally, the vacuum sampling approach eliminates the risk of dross contamination of samples and avoids the use of moving parts in the salt. Two methods of interfacing the vacuum sampling loop with a precision pneumatic sample generator were investigated in FY21. This report covers the testing of fluidic coupling between the two modules. Two iterations of the fluidically coupled modules were tested. The first iteration system coupled the two modules using a freeze valve to seal the vacuum sampler during filling and to control flow into the pneumatic sample generator. While this integrated system functioned as intended, some changes were implemented to make the system more robust and better suited to remote deployment. Specifically, the system was made to be more modular and active control of the vacuum filling operation was replaced with a passive control mechanism. For passive filling, the salt charge vessel was vented to a small gas tank that was at negative pressure, causing salt to be drawn into the vessel until the force of the fluid head was in equilibrium with the gas pressure. The passive control system performed well and will be used in future iterations. Another change in the second system was a newly configured pneumatic sample generator in which sample ejection occurred through a hole in the reservoir’s stainless-steel side wall instead of through a non-wetted sapphire orifice on the bottom. This alternate configuration may be better suited for near-process deployment because it enables on-line orifice maintenance and an orifice bypass drain back to the process. A third change in the second iteration system was the transition to a two-chamber charge vessel which split off a fraction of the sampled salt as a liquid aliquot. The goal was to create a buffer mechanism that would allow reproducible aliquoting of samples, independently of variability in the charge vessel fill height. While the two-chamber design was functional, the sample size reproducibility was below target values. To improve reproducibility and overcome many of the impediments to remote deployment of the vacuum sampling loop module, separate work was conducted to replace the two-chamber liquid aliquoting mechanism with aliquoting into single-use sample tubes. Solid salt transfer in the sample tubes will replace fluidic coupling for integrating the vacuum sampler with downstream modules. Because the proposed operations can all be executed with simple overhead actuation mechanisms or other existing hot-cell technology, there will be no need for large investments in novel hot cell sample handling technologies using this alternate approach. As such, near-term deployment of the vacuum sampling technology will be achievable. This new approach for automated coupling of sample tubes with down-stream modules is covered in a separate FY21 report, and a remotely operated version of the vacuum sampler loop module with the tube aliquoting feature is planned for FY22.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2015

Application of Hotelling’s T{sup 2} charts in monitoring quality parameters in a drinking water supply system

In water supply systems with distribution networkthe most critical aspects of control and Monitoring of water quality, which generates crises system, are the effects of cross-contamination originated by the network typology. The classics of control of quality systems through the application of Shewhart charts are generally difficult to manage in real time due to the high number of charts that must be completed and evaluated. As an alternative to the traditional control systems with Shewhart charts, this study aimed to apply a simplified methodology of a monitoring plan quality parameters in a drinking water distribution, by applying Hotelling’s T{sup 2} charts and supplemented with Shewhart charts with Bonferroni limits system, whenever instabilities with processes were detected.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

The Application of a Genetic Algorithm to the Optimization of a Mesoscale Model for Emergency Response

Besides solving the equations of momentum, heat, and moisture transport on the model grid, mesoscale weather models must account for subgrid-scale processes that affect the resolved model variables. These are simulated with model parameterizations, which often rely on values preset by the user. Such “free” model parameters, along with others set to initialize the model, are often poorly constrained, requiring that a user select each from a range of plausible values. Finding the values to optimize any forecasting tool can be accomplished with a search algorithm, and one such process—the genetic algorithm (GA)—has become especially popular. As applied to modeling, GAs represent a Darwinian process: an ensemble of simulations is run with a different set of parameter values for each member, and the members subsequently judged to be most accurate are selected as “parents” who pass their parameters onto a new generation. At the U.S. Department of Energy’s Savannah River Site in South Carolina, we are applying a GA to the Regional Atmospheric Modeling System (RAMS) mesoscale weather model, which supplies input to a model to simulate the dispersion of an airborne contaminant as part of the site’s emergency response preparations. An ensemble of forecasts is run each day, weather data are used to “score” the individual members of the ensemble, and the parameters from the best members are used for the next day’s forecasts. As meteorological conditions change, the parameters change as well, maintaining a model configuration that is best adapted to atmospheric conditions. Significance Statement We wanted to develop a forecasting system by which a weather model is run over the Savannah River Site each day and repeatedly adjusted according to how well it performed the previous day. To run the model, a series of values (parameters) must be set to control how the model will calculate winds, temperatures, and other desired variables. Each day the model was run several times using different combinations of these parameters and later compared with observed meteorological conditions. Parameters that produced the most accurate forecasts were preferentially reused to create the forecasts for the next day. The process was tested for the summer of 2020 and exhibited lower errors than forecasts produced by the model using default values of the parameters.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Nanomineralogy as a new dimension in understanding elusive geochemical processes in soils: The case of low-solubility-index elements

Nanomineralogical studies of mineral surface coatings in soils reveal insights into biogeochemical processes that heretofore were not known to exist. This is a new dimension in understanding past and present biogeochemical processes in soils, and in this study it is a way to better understand the behavior of low-solubility-index elements such as Al, Ti, and Zr. Soils were sampled from selected sites in Sudbury (Ontario, Canada) that have been affected by acidification and particulate matter emissions from base-metal smelters with subsequent remediation within the past century. These anthropogenic processes have affected an entire landscape, but are now recorded in assemblages of nano-size phases that can be only studied using a combination of focused ion beam technology (for sample preparation) and high-resolution analytical transmission electron microscopy (for phase identification). A first generation of clay minerals (pre-acidification phase), their partial replacement by nano-size hematite and amorphous silica (anthropogenic acidification), and a second generation of clay minerals (post-acidification, including soil remediation) are products of changes in soil biogeochemical processes during these natural and anthropogenic-induced weathering stages. Furthermore, complex assemblages of nanophases formed prior to the second generation of clay minerals depict underlying mechanisms for the mobilization and sequestration of the low-solubility-index elements Zr and Ti under acidic conditions. The occurrence of baddeleyite (ZrO 2 ), anatase (TiO 2 ), and the Magneli phases Ti 4 O 7 and Ti 5 O 9 (all present at the nanoscale) suggest an influx of nanocolloidal Zr and Ti oxides during weathering of smelter-derived particulate matter. Kelyshite {NaZr[Si 2 O 6 (OH)]}, authigenic zircon (ZrSiO 4 ), and kleberite [Fe 3+ Ti 6 O 11 (OH) 5 ] are most likely products of the sequestration of the Zr- and Ti-bearing nanocolloids.

58 GEOSCIENCES↗
DOE OSTI2013

Iso standardization of theoretical activity evaluation method for low and intermediate level activated waste generated at nuclear power plants

Disposal of low-and intermediate-level activated waste generated at nuclear power plants is being planned or carried out in many countries. The radioactivity concentrations and/or total quantities of long-lived, difficult-to-measure nuclides (DTM nuclides), such as C-14, Ni-63, Nb-94, α emitting nuclides etc., are often restricted by the safety case for a final repository as determined by each country's safety regulations, and these concentrations or amounts are required to be known and declared. With respect to waste contaminated by contact with process water, the Scaling Factor method (SF method), which is empirically based on sampling and analysis data, has been applied as an important method for determining concentrations of DTM nuclides. This method was standardized by the International Organization for Standardization (ISO) and published in 2007 as ISO21238 'Scaling factor method to determine the radioactivity of low and intermediate-level radioactive waste packages generated at nuclear power plants' [1]. However, for activated metal waste with comparatively high concentrations of radioactivity, such as may be found in reactor control rods and internal structures, direct sampling and radiochemical analysis methods to evaluate the DTM nuclides are limited by access to the material and potentially high personnel radiation exposure. In this case, theoretical calculation methods in combination with empirical methods based on remote radiation surveys need to be used to best advantage for determining the disposal inventory of DTM nuclides while minimizing exposure to radiation workers. Pursuant to this objective a standard for the theoretical evaluation of the radioactivity concentration of DTM nuclides in activated waste, is in process through ISO TC85/SC5 (ISO Technical Committee 85: Nuclear energy, nuclear technologies, and radiological protection; Subcommittee 5: Nuclear fuel cycle). The project team for this ISO standard was formed in 2011 and is composed of experts from 11 countries. The project team has been conducting technical discussions on theoretical methods for determining concentrations of radioactivity, and has developed the draft International Standard of ISO16966 'Theoretical activation calculation method to evaluate the radioactivity of activated waste generated at nuclear reactors' [2]. This paper describes the international standardization process developed by the ISO project team, and outlines the following two theoretical activity evaluation methods:? Point method? Range method. (authors)

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

Plasma-assisted atomic layer etching of single-crystal diamond

Applications of near-surface nitrogen-vacancy (NV) centers in diamond are often limited by surface defects created during processing. Understanding and controlling plasma-induced surface damage is important for preserving the optical and spin properties of diamond NV centers. We report molecular dynamics simulations of a novel form of plasma-aided atomic layer etching of diamond. In this proposed scheme, the initial surface modification step consists of Ar + ion bombardment. This creates an amorphous layer at the surface, the thickness of which is controlled by the ion energy. Amorphization is known to help smooth the surface, at least locally, and would also serve to sputter clean an initially contaminated surface. A second step impacts the amorphous carbon layer with O + between about 1 and 5 eV. Simulations show that this energy range will remove the amorphous carbon but will not etch the underlying diamond. Though this energy range is not trivial to achieve in a conventional low-temperature plasma, potential methods for creating these low-energy O + ions are discussed. In addition to a-C etching, the O + impacts are predicted to remove any isolated (100) diamond terraces by selectively attacking the edges of the terraces. The proposed atomic layer etching (ALE) approach reverses the conventional ALE sequence in which the surface modification step is usually chemical modification (oxidation in this case), followed by a removal step using Ar + impacts. This plasma ALE procedure is predicted to create a diamond surface that is atomically flat and defect free.

Draney, J. S. [Princeton University, NJ (United St↗
DOE OSTI2012

Design and Testing of a Labview- Controlled Catalytic Packed- Bed Reactor System For Production of Hydrocarbon Fuels

Gasified woody biomass (producer gas) was converted over a Mo/H+ZSM-5 catalyst to produce gasolinerange hydrocarbons. The effect of contaminants in the producer gas showed that key retardants in the system included ammonia and oxygen. The production of gasoline-range hydrocarbons derived from producer gas was studied and compared with gasoline-range hydrocarbon production from two control syngas mixes. Certain mole ratios of syngas mixes were introduced into the system to evaluate whether or not the heat created from the exothermic reaction could be properly controlled. Contaminant-free syngas was used to determine hydrocarbon production with similar mole values of the producer gas from the gasifier. Contaminant-free syngas was also used to test an ideal contaminant-free synthesis gas situation to mimic our particular downdraft gasifier. Producer gas was used in this study to determine the feasibility of using producer gas to create gasoline-range hydrocarbons on an industrial scale using a specific Mo/H+ZSM-5 catalyst. It was determined that after removing the ammonia, other contaminants poisoned the catalyst and retarded the hydrocarbon production process as well.

Gasification, Hydrocarbons, Mo/HZSM-5, Mo/H+ZSM-5,↗
DOE OSTI2016

Evaluation and Application of Phyto-remediation at FUSRAP Projects - 16275

The Niagara Falls Storage Site (NFSS) and associated vicinity properties (VPs) occupy approximately 607 hectares (1,500 acres) of the original 3,035-hectare (7,500-acre) Lake Ontario Ordnance Works (LOOW). The NFSS was used to store radioactive materials, residues and waste from uranium ore processing between 1944 and 1952. A field-study is currently underway to evaluate the potential use of hybridized trees to stabilize radionuclides, mainly uranium, and chlorinated solvents derived from trichloroethylene degradation in groundwater at the NFSS. The purpose of this effort is to support the USACE-Buffalo District in the evaluation and implementation of phyto-remediation approaches to contain groundwater impacts on the site. This demonstration project is considered a site maintenance action and will have relevance to the Formerly Utilized Sites Remedial Action Program (FUSRAP) mission. The demonstration is designed to determine the ability of trees to withstand and uptake Uranium (U), and to a lesser extent Trichloroethylenes (TCEs), and hydraulically control groundwater where historical practices produced a series of disconnect plumes. Although the groundwater at the NFSS is naturally high in total dissolved solids that preclude untreated consumption, the groundwater contaminant levels are very high in some areas and may limit the options for future site re-use. Active groundwater remediation is impractical due to the clayey site soils and low risk of transport. The phyto-remediative approach is a passive action to lessen the groundwater impacts during the project's life cycle and property re-use planning. The target contaminant sources and plumes occur near the property boundaries, along legacy sanitary sewer lines, and near on-site surface-water courses. The demonstration includes soil characteristic determinations, the testing of optimal hybrid tree species, field implementation at target sites, and soil moisture and groundwater monitoring during the long-term evaluation phase. The final disposition of the trees will be included in future site decision and maintenance documents. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Rates and mechanisms of uranyl oxyhydroxide mineral dissolution

Uranyl oxyhydroxide minerals are important weathering products in uranium-contaminated surface and subsurface environments that regulate dissolved uranium concentrations. However, dissolution rates for this class of minerals and associated dissolution mechanisms have not been previously reported for circumneutral pH conditions, particularly for the case of flow through porous media. In this paper, the dissolution rates of K- and Na-compreignacite (K 2 (UO 2 ) 6 O 4 (OH) 6 ·8H 2 O and Na 2 (UO 2 ) 6 O 4 (OH) 6 ·8H 2 O respectively) were measured using flow-through columns reacted with two simulated background porewater (BPW) solutions of low and high dissolved total carbonate content (ca. 0.2 and 2.8 mmol L -1 ). Column materials were characterized before and after reaction with electron microscopy, bulk chemistry, and EXAFS to identify structural and chemical changes during dissolution and to obtain insight into molecular-scale processes. The reactive transport code CrunchFlow was used to calculate overall dissolution rates while accounting for fluid transport and changes in mineral volume and reactive surface area and results were compared to steady-state dissolution rate calculations. In low carbonate BPW systems, interlayer K and Na were initially leached from both minerals, and in Na-compreignacite, K and minor divalent cations from the input solution were incorporated into the mineral structure. Results of characterization analyses suggested that after reaction both K- and Na-compreignacite resembled a disordered K-compreignacite with altered surfaces. A 10-fold increase in dissolved carbonate concentration and corresponding increase in pH (from 6.65 to 8.40) resulted in a net removal of 58-87% of total uranium mass from the columns, compared to <1% net loss in low carbonate BPW systems. Steady-state release of dissolved uranium was not observed with high carbonate solutions and post-reaction characterizations indicated a lack of development of leached or altered surfaces. Dissolution rates (normalized to specific surface area) were about 2.5-3 orders-of-magnitude faster in high versus low carbonate BPW systems, with Na-compreignacite dissolving more rapidly than K-compreignacite under both BPW conditions, possibly due to greater ion exchange (1.57·10 -10 vs. 1.28·10 -13 mol m -2 s -1 [log R = -9.81 and -12.89] and 5.79·10 -10 vs. 3.71·10 -13 mol m -2 s -1 [log R = -9.24 and -12.43] for K- and Na-compreignacite respectively). Experimental and spectroscopic results suggest that the dissolution rate is controlled by bond breaking of a uranyl group and detachment from polyhedral layers of the mineral structure. With higher dissolved carbonate concentrations, this rate-determining step is accelerated by the formation of Ca-uranyl carbonate complexes (dominant species under these conditions), which resulted in an increase of the dissolution rates. Optimization of both dissolution rate and mineral volume fraction in the reactive transport model to account for uranium mass removal during dissolution more accurately reproduced effluent data in high carbonate systems, and resulted in faster overall rates compared with a steady-state dissolution assumption. Finally, this study highlights the importance of coupling reaction and transport processes during the quantification of mineral dissolution rates to accurately predict the fate of contaminants such as uranium in porous geomedia.

58 GEOSCIENCES↗
DOE OSTI2019

Climate change impact on residual contaminants under sustainable remediation

This study investigates the potential impact of climate change on residual contaminants in vadose zones and groundwater. We assume that the effect of climate changes can be represented by perturbations in the natural recharge through the aquifer system. We perform numerical modeling of unsaturated/saturated flow and transport and consider different performance metrics: contaminant concentrations at observation wells and contaminant export at the site's boundary. We evaluate the effect of increasing and decreasing recharge as well as the impact of potential failure of surface capping structures employed to immobilize vadose zone contaminants. Our approach is demonstrated in a real case study by simulating transport of non-reactive radioactive tritium at the U.S. Department of Energy's Savannah River Site. Results show that recharge changes significantly affect well concentrations: after an initial slight dilution we identify a significant concentration increase at different observation wells some years after the recharge increase and/or the cap failure, as a consequence of contaminants' mobilization. This effect is generally emphasized and occurs earlier as the recharge increases. Under decreased aquifers' recharge the concentration could slightly increase for some years, due to a decrease of dilution, depending on the magnitude of the negative recharge shift. We identify trigger levels of recharge above which the concentration/export breakthrough curves and the time of exceedance of the Maximum Contaminant Level for tritium are remarkably affected. Moreover, we observe that the contaminant export at the control plane, identified as the risk pathway to the downgradient population, may only be minimally affected by shifts in the natural recharge regime, except for some extreme cases. We conclude that more frequent sampling and in-situ monitoring near the source zone should be adopted to better explain concentrations' anomalies under changing climatic conditions. Moreover, the maintenance of the cap is critical not only to sequester residual contaminants in the vadose zone, but also to reduce the uncertainty associated with future precipitation changes. Finally, realistic flow and transport simulations achieved through proper calibration processes, rather than conservative modeling, should be adopted to identify non-trivial trade-offs which enable better allocation of resources towards reducing uncertainty in decision making.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Issue Resolution During the Development of the Performance Assessment for the Savannah River Site Saltstone Disposal Facility - 20125

In 2019, Savannah River Remediation developed a revision to the performance assessment (PA) on behalf of the U.S. Department of Energy (DOE) Savannah River Operations Office (SR) for the near-surface disposal of low-level waste at the Savannah River Site (SRS) Saltstone Disposal Facility (SDF). Soluble waste from SRS Tank Farms undergoes salt processing to remove cesium and other high-activity constituents. The low-activity decontaminated salt solution (DSS) is then immobilized by mixing it into a cementitious waste form known as saltstone. After mixing, the saltstone is poured into leak-tight concrete vaults, known as saltstone disposal units (SDUs), where the waste form cures. By the time of facility closure, the SDF is expected to consist of 15 SDUs with a combined capacity of 1.06 E+09 L (280 Mgal) of cured saltstone. The facility operates under a Disposal Authorization Statement from DOE and a permit from the South Carolina Department of Health and Environmental Control (SCDHEC). Since the start of operations in 1990, the SDF has received almost 6.7 E+07 L (18 Mgal) of DSS, resulting in the safe disposal of 2.7 E+16 Bq (7.3 E+05 Ci) of activity. Due to the radioactive decay of short-lived contaminants, the total remaining activity in the disposed waste is estimated to be approximately 1.4 E+16 Bq (3.9 E+05 Ci), as of September 2018. The Disposal Authorization Statement requires a demonstration that the system of engineered and natural features of the disposal facility will limit releases from the facility and be protective of human health and the environment for at least the next 1,000 years. The long-term performance of the facility was evaluated under the requirements of the DoE's Radioactive Waste Management Manual (US DOE Manual 435.1-1). Simulations were performed to demonstrate that the disposal facility would meet performance objectives specified in the manual. The evaluation was based on numerical models that simulate the releases of contaminants from the saltstone waste form. Contaminants were transported through groundwater and air pathways to points of assessment to evaluate compliance (i.e., 100 m from the SDUs). In addition, the potential consequences of an inadvertent human intrusion (IHI) were also evaluated. A number of issues were overcome during the development of these simulations. These issues were identified as part of internal technical reviews. Simulations are developed by people and people make mistakes, so the internal technical review process is a vital step in PA development. Specific examples of resolved issues include a unit-conversion error, an inappropriate definition for a model boundary condition, a model time-stepping issue, and an error in the calculation for the buildup of contaminants in soil. Actions taken to address these issues resulted in an improved product with a better supported technical basis and more defensible results. The identification and correction of these issues are discussed. By understanding these issues, model developers and technical reviewers working on PAs in the future may avoid repeating these types of mistakes. Transparency with respect to these mistakes builds trust between waste management sites, regulators, and stakeholders. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Pilot-Scale Silicone Process for Low-Cost Carbon Dioxide Capture

GE Global Research is developing technology to remove carbon dioxide (CO 2) from the flue gas of coal-fired powerplants. A mixture of 3-aminopropyl end-capped polydimethylsiloxane (GAP-1m) and triethylene glycol (TEG) is the preferred CO2-capture solvent. GE Global Research was contracted by the Department of Energy to test a pilot-scale continuous CO2 absorption/desorption system using a GAP-1m/TEG mixture as the solvent. As part of that effort, an Environmental, Health, and Safety (EH&S) assessment for a CO2-capture system for a 550 MW coal-fired powerplant was conducted. Five components of the solvent, CAS#2469-55-8 (GAP-0), CAS#106214-84-0 (GAP-1-4), TEG, and methanol and xylene (minor contaminants from the aminosilicone) are included in this assessment. One by-product, GAP- 1m/SOX salt, and dodecylbenzenesulfonicacid (DDBSA) were also identified foranalysis. An EH&S assessment was also completed for the manufacturing process for the GAP-1m solvent. The chemicals associated with the manufacturing process include methanol, xylene, allyl chloride, potassium cyanate, sodium hydroxide (NaOH), tetramethyldisiloxane (TMDSO), tetramethyl ammonium hydroxide, Karstedt catalyst, octamethylcyclotetrasiloxane (D4), Aliquat 336, methyl carbamate, potassium chloride, trimethylamine, and (3-aminopropyl) dimethyl silanol. The toxicological effects of each component of both the CO2 capture system and the manufacturing process were defined, and control mechanisms necessary to comply with U.S. EH&S regulations are summarized. Engineering and control systems, including environmental abatement, are described for minimizing exposure and release of the chemical components. Proper handling and storage recommendations are made for each chemical to minimize risk to workers and the surrounding community.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2019

Lithographically defined synthesis of transition metal dichalcogenides

Abstract Transition metal dichalcogenides (TMDs) promise to revolutionize optoelectronic applications. While monolayer exfoliation and vapor phase growth produce extremely high quality 2D materials, direct fabrication at wafer scale remains a significant challenge. Here, we present a method that we call ‘lateral conversion’, which enables the synthesis of patterned TMD structures, with control over the thickness down to a few layers, at lithographically predefined locations. In this method, chemical conversion of a metal-oxide film to TMD layers proceeds by diffusion of precursor propagating laterally between silica layers, resulting in structures where delicate chalcogenide films are protected from contamination or oxidation. Lithographically patterned WS 2 structures were synthesized by lateral conversion and analyzed in detail by hyperspectral Raman imaging, scanning electron microscopy and transmission electron microscopy. The rate of conversion was investigated as a function of time, temperature, and thickness of the converted film. In addition, the process was extended to grow patterned MoS 2 , WSe 2 , MoSe 2 structures, and to demonstrate unique WS 2 /SiO 2 multilayer structures. We believe this method will be applicable to a variety of additional chalcogenide materials, and enable their incorporation into novel architectures and devices.

Kemelbay, Aidar (ORCID:0000000233211483)↗