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DOE OSTI2021

Material Control & Accountancy for Molten Salt Reactors (FY2021 Report)

There is significant domestic and international interest, investment, and research and development momentum to pursue advanced nuclear reactor technologies. Molten salt reactor (MSR) concepts display the largest variability in fuel type and design features among the current advanced concepts. MSRs have been proposed with various core designs, sizes (power), and fuel cycles. Salt-fueled molten salt systems represent the only advanced reactor type with fuel that is not in a solid form during operation. These “liquid-fueled” MSRs are unique from perspectives of fuel fabrication, spent irradiated fuel and waste components, licensing, and material control and accountability (MC&A) including the potential of fissile material holdup. The liquid fuel salt is the defining distinction in comparison to other advanced reactors that propose TRI-structural ISOtropic particle fuel pebbles, various coolant options (e.g., molten salts or metals, high temperature gas), or small modular alternatives using solid fuel variants including both light water reactors and non-light water reactors. MSRs are appealing to the nuclear energy industry because of the diverse reactor characteristics they can support including various neutron energy spectra, fueling requirements, fuel cycles, and/or fuel utilization. However, because of the significant deviation and diversity of a salt-fueled system compared to traditional solid fuel light water-cooled reactors (LWRs), the history, regulatory licensing framework, modeling capabilities, and supporting engineering technology are either lacking or, in some cases, nonexistent. Therefore, the research community is actively supporting advanced MSR development on many of these fronts in particular to assist MSR vendors with licensing requirements. ORNL is leading the research and development of respective MC&A approaches for salt-fueled MSRs. This report summarizes the research performed at Oak Ridge National Laboratory (ORNL) under the US Department of Energy, Office of Nuclear Energy, Advanced Reactor Safeguards (ARS) program to investigate safeguards and security by design concepts, licensing and regulatory considerations, and dynamic system-level modeling to understand radioisotope concentrations for salt-fueled MSRs. The report builds upon the previous research and literature, identifies the MC&A challenges inherent to a salt-fueled MSR, reviews current regulatory frameworks for LWRs and their applicability towards salt-fueled MSRs, summarizes the status and progress of an MSR dynamic modeling tool, and discusses a prospective MC&A approach based on the Molten Salt Demonstration Reactor (MSDR) model.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2020

Tracking Radioactive Isotopes in HVAC and Application for Hot Cell Analyses - 20155

In recent years, the surge in the number of isotope production facilities under design has increased the need to analyze isotope migration in facility Heating, Ventilation, and Air Conditioning (HVAC) during normal operations and accident scenarios. These facilities are used to produce isotopes for medical, security, and industrial applications and as such are subject to license and regulatory requirements 10CFR20, 10CFR30, 10CFR50, and 10CFR70. GOTHIC, a general-purpose thermal-hydraulics software package, includes the ability to model isotopic tracers, radioactive decay and isotope migration as well as HEPA and charcoal filters for isotope retention. A GOTHIC model was developed by Zachry Nuclear Engineering (ZNE) to examine the effect of negative room pressure, HEPA filtration, and HVAC fluctuations on radiation areas, hot cells and gloveboxes. Radioactive tracers were used to simulate the concentration of spills within contaminated areas, track the migration of isotopes of interest, and determine the isotopic retention and buildup on facility HEPA filters. A variety of isotopes with concern to dose (e.g., Kr-85, Sr-90, I-131, etc.), including their decay and progeny, are included in the analysis. Negative pressures are maintained in the regions of interest by a representative central HVAC system equipped with a volumetric fan that exhausts to the environment after a series of isolation valves and HEPA filters. GOTHIC is an industry trusted tool for providing engineering solutions for a variety of applications, including fission product tracking, aerosol and particulate transport and ventilation assessments. The software provides an integrated analysis environment that includes a graphical user interface (GUI) for constructing analysis models, a numerical solver that includes parallel processing capabilities and a post-processor for evaluating simulation results. It solves the conservation equations for mass, momentum and energy for multicomponent, multi-phase flow in lumped parameter and multi-dimensional geometries (1, 2, or full 3D), including the effects of turbulence, diffusion and buoyancy. It has been developed and maintained under a Quality Assurance program in compliance with the requirements of 10CFR50 Appendix B and applicable portions of ASME NQA-1 since 1995. GOTHIC has been used for assessing both forced and natural convection conditions for a wide range of applications, including: - Tracking concentration of hazardous gases and chemicals for habitability and safety assessments - Determining ventilation and filtration requirements and optimizing location and arrangement of these systems - Room heat-up, including diverse and Flexible coping strategies for Extended Loss of AC Power (FLEX/ELAP) - Equipment Qualification (EQ) A distinctive feature of GOTHIC is the ability to track many different fields/substances in a simulation, including user defined tracer elements, in the liquid, vapor and droplet fields as well as surfaces and filters. This capability allows GOTHIC to model fission product transport and release or the removal of particulates or harmful toxins from exhaust gases using a spray scrubber or other types of filtration systems. GOTHIC also includes models for engineered equipment, such as fans, filters, charcoal filters, dryers/demisters, dampers, etc. The aerosols and other filtered material are removed or accumulated in these components. The range of aerosol and radiological applications that GOTHIC has been used for includes: - Source Term: Primary Coolant (Equilibrium) Activity; Non-Water Coolant Source/Leakage. - Conditions for Iodine Re-evolution: Sump/Suppression Pool Conditions and pH; - RWST Conditions and pH. - Isotope Removal Mechanisms: Containment Sprayed and Unsprayed Region Mixing; Charcoal Filter Heating due to Iodine decay. - Radionuclide Transport and Decay: Post-LOCA Release in containment; Transport between connected Compartments and vent systems; Groundwater transport of radionuclides. - Non-Newtonian Fluid modeling for sludge, waste tanks, etc. ADAMS ML071581053 (titled 'Best Practice Guidelines for the use of CFD in Nuclear Reactor Safety Applications') poses guidelines for applying single phase CFD codes in nuclear reactor safety problems and GOTHIC is listed as a 'tool for 3D flows' and 'dispersal and deposition of radionuclides.' The Nuclear Quality Assurance (NQA) pedigree of GOTHIC is an important aspect for applications in the nuclear industry. The fundamental tracer models (convective transport, molecular and turbulent diffusion, removal mechanisms, etc.) have been verified using analytical solutions and validated against applicable separate effects tests. Also, GOTHIC has been benchmarked to many integrated effects tests, including Phebus FP (Fission Product). GOTHIC gives good agreement for the buildup and decay of fission products in Phebus Test 3. The model developed by ZNE demonstrates GOTHIC's applicability and acceptability for use in analyzing the migration and retention of radioactive isotopes and their progeny in normal operation and accident scenario analyses for isotope production facilities, hot cells, and gloveboxes. The tracer activities calculated by GOTHIC can then be used in downstream radiation transport and shielding codes like RADTRAD-NAI{sup C}, MCNP{sup R}, and MicroShield{sup R} to determine on-site and of-site doses. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Installation of Lysimeters Near Engineered Trench 3

Three new lysimeter stations were installed on the north rim of Engineered Trench 3 (Figure ES-1)at the E-Area Low Level Waste Facility (ELLWF). These stations were designated as ET3-VL-3, ET3-VL-4, and ET3-VL-5. The stations were installed in a line with the two existing stations (ET3-VL-1 and ET3-VL-2) and spaced approximately 100 ft apart. Two lysimeters were installed at each station at the depths shown in Table ES-1. Lysimeter placement was based on borehole lithology and was comparable to the existing lysimeter stations. The deepest lysimeter at each of the three new lysimeter stations was designated as the action-level lysimeter.Following installation, the lysimeters were purged and placed under vacuum for sampling. Sampling occurred in December 2020 with each lysimeter producing 1000 ml of water for tritium analysis. All lysimeters were below the administrative limit for ET3 (43.7 pCi/ml) with all but ET3-VL-5 (222) at background levels. ET3-VL-5 (222) had a tritium concentration of 27.5 pCi/ml.With the addition of the new lysimeters at ET3, the vadose zone monitoring system is now comprised of 309 active lysimeters at 102 lysimeter stations. There are 93 action-level lysimeters at 102 stations

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

On the dissolution of a borosilicate glass with the use of isotopic tracing – Insights into the mechanism for the long-term dissolution rate

An understanding of the mechanisms responsible for controlling the long-term corrosion rate of nuclear waste glass is paramount if reliable glass dissolution models are to be used to calculate the controlled release of radionuclides from nuclear waste glass under geologic disposal conditions. Additionally, understanding silicate glass dissolution is also important for natural glasses to understand the role from the dissolution of these glasses has on the composition of natural aquatic systems. Two general mechanisms appear to be responsible for the elemental release from glass to the surrounding biosphere - ion exchange (release principally of alkalis) and matrix dissolution (release of the structural components of the glass). Key unknowns related to these mechanisms are the impact of surface layers on the altered glass and how these layers participate in corrosion. To better understand the impact of these layers on glass corrosion, we made two glasses of the same elemental composition, but with selected elements enriched in specific isotopes, e.g. more 10 B than 11 B. We reacted these glasses for 1 y then the solutions from each were exchanged and the chemistry of the solutions and the solids were followed for another 2 y and in some cases 3 y. This allowed us to follow changes in the glasses with respect to these elements and how these elements were transported through the alteration layers with time and, for at least one element, into the glass. Results from these experiments demonstrate that the release behavior of different elements is strongly dependent on their structural role in the glass (e.g. network formers and modifiers), but, more importantly, the role of water transport and subsequent ion exchange has in the long-term dissolution of the glass studied here. In this article, we highlight the behavior of four elements: lithium, sodium, silicon, and boron. Lithium and sodium, network modifying elements, have similar chemistries. The behavior of Li could be tracked in more detail by following both 6 Li and 7 Li; Li penetrates through the gel layer in both directions without hinderance and into and released from the glass deeper than sodium. Silicon, a network forming element, reacts with the silica-rich alteration layer. Boron, a network forming element, does not accumulate in the gel or the pristine glass and has a very sharp elemental profile between the pristine glass and alteration layer. Boron, lithium, and sodium elemental profiles suggest that there is little if any transport control within the alteration layer. The correlation between the Li and Na profiles and that of a water species suggest that the limiting release is a steady state between the diffusion of a water species and matrix dissolution that results in a low release rate for alkali and this provides a steady driving force for the long-term dissolution of glass.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

The apparent reversal of the Law of Mass Action in concentrated multicomponent aqueous solutions

Although it is well known that aqueous electrolyte solutions behave non-ideally, few are so non-ideal that adding an electrolyte to a saturated solution with a common ion enhances rather than depresses solubility. Nonetheless, this apparent reversal of the Law of Mass Action (LMA) has been observed in simple nitrate solutions at high concentrations. A leading hypothesis is that ion clusters are formed and stabilized by ions having different charge densities. We report the present study examines this concept, in part by reviewing relevant data from multicomponent aqueous solutions containing sodium nitrate (NaNO 3 ), sodium nitrite (NaNO 2 ), sodium hydroxide (NaOH), and sodium aluminate (NaAl(OH) 4 ) - the major constituents in alkaline nuclear waste. Here, NaOH and NaAl(OH) 4 did not enhance the solubility of NaNO 3 or NaNO 2 , whereas NaNO 2 and NaNO 3 enhanced rather than depressed the solubility of each other despite each having the sodium cation (Na + ) in common. Solutions evaluated in this study have more than 20 molal total Na + concentration, and most have less than one mole of water per mole of ion. Thus, this reversal of the LMA occurs in solutions where there is not enough water to fully hydrate the ions, pointing to the importance of ion cluster formation. Within the composition range of the solutions analyzed here, this reversal of the LMA occurs regardless of NaAl(OH) 4 and NaOH concentrations. Elevated temperatures also result in the reversal of the LMA in the subsystems NaNO 2 -NaNO 3 -H 2 O and NaOH-NaNO 3 -H 2 O, consistent with spectroscopic and computational studies showing enhanced interactions at higher temperatures. Although speciation in these highly concentrated electrolyte solutions is not well understood, the stabilization of ion clusters by: (i) optimizing charge density around the ions through different combinations of mixed cations and anions in solution; and (ii) high temperatures where ions experience prolonged contact, offers important clues for future research into how these species control solubility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

An integrated process for butanol production from cellulosic biomass and CO 2 using engineered clostridia in a linear immobilized bioreactor

Engineered platforms using mixed microbial consortia to consolidate multiple reaction steps and perform disparate conversions simultaneously can substantially enhance the carbon efficiency of biomass conversion processes and lower the biofuel cost to an economically competitive level. In this project, an integrated process will be developed to produce n-butanol from cellulosic biomass and waste gas streams using two engineered clostridial strains, one butanol-tolerant solventogenic strain and one carboxydotrophic acetogen, co-immobilized in a “Linear Immobilized Bioreactor” (LIBR). The CO 2 and H 2 produced by the solventogenic strain will be used by the carboxydotrophic strain to produce acetate (and butyrate) that in turns can be used by the solventogenic strain to produce more butanol. Such a co-cultured fermentation has the potential to increase butanol production from biomass hydrolysate sugars by up to 50% with 100% reduction in CO 2 emission. Butanol produced in the fermentation will be stripped by the rising bubbles of fermentation produced gases (CO 2 and H 2 ) in the LIBR and separated via a condenser, alleviating butanol inhibition while achieving continuous butanol production at a high productivity and product titer, which can reduce both water and energy consumptions by over 50% compared to conventional ethanol and ABE fermentation processes. Phase I study proved the new bioprocess concept and verified our hypothesis that the proposed LIBR and co-cultured fermentation can enhance the conversion of lignocellulosic sugars to butanol with higher butanol yield, productivity and titer, leading to reduced biobutanol cost to compete more favorably with bioethanol and fossil fuels. A prototype lab-scale LIBR for multiphase fermentation was constructed to investigate and demonstrate the technical feasibility and advantages of the LIBR for multiphase fermentation involving sugars and gaseous substrates. The LIBR will be optimized and evaluated for its economic feasibility for biobutanol production from lignocellulosic biomass and industrial waste gases in Phase II.

09 BIOMASS FUELS↗
DOE OSTI2020

Performance of Closed Loop Venturi Aspirated Aeration System: Experimental Study and Numerical Analysis with Discrete Bubble Model

In wastewater treatment plants, aeration plays a significant role as it encourages aerobic respiration of microbes, which are necessary to break down carbonaceous matter in the waste stream. This process can account for the majority of energy use in wastewater treatment plants. The aeration process is also necessary in odor control in lagoons and in the aquaculture industry. Generally, the aeration process is accomplished with compressors or blowers which can be of low efficiency due to ideal gas laws. This study introduces the idea of increasing aeration efficiency by looping water from a reservoir through a piping network which includes a venturi aspirator at its inlet. For this purpose, an experimental study has been conducted in a laboratory setup with a pump which pulls water from a tank, passes it through a Venturi aspirator and a helical piping network intended to increase bubble residence time, before depositing it back into the bulk fluid tank. This same process is modeled computationally, using a discrete bubble method (DBM), with good agreement with experiments. The overall purpose here is to determine the optimal configurations for standard aeration efficiency (SAE) and the standard oxygen transfer rate (SOTR). A parametric study has been implemented using the DBM based on different hydraulic and flow parameters. The model is also used to predict the SAE of a hypothetical aeration system. Results indicate that it is possible to achieve SAE values in the range of surface aerators or submersed jet aerators using the proposed aeration system with less complex components, thereby decreasing overall costs.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2025

Biogeochemical controls on iron speciation and cycling across upland to shoreline gradients in freshwater and estuarine coastal soils (Lake Erie and Chesapeake Bay, United States)

Coastal environments are dynamic interfaces that mediate carbon and nutrient exchanges between terrestrial landscapes and open waters, and understanding the biogeochemical factors controlling these exchanges, particularly iron (Fe) redox transformations, is crucial for predicting coastal ecosystem functions. Here, we investigated the mechanisms controlling Fe speciation changes across upland-to-shoreline gradients in freshwater and estuarine soils using Fe K-edge X-ray absorption spectroscopy, solid and porewater composition analysis, and 16S rRNA sequencing analysis. We show that Fe transformations depend primarily on inundation patterns. In unsaturated uplands, Fe occurs as Fe(III) oxyhydroxides, mainly goethite (9–35 %), Fe(II,III)-phyllosilicates (39–89 %), and Fe(III)-organic species (0–61 %). Soils influenced by estuarine waters exhibit porewater sulfide concentrations reaching up to 221 μM, Fe- and S-cycling bacteria, and up to 81 % pyrite (FeS 2 ), indicating that sulfur-driven redox dynamics control Fe transformations. In lacustrine wetlands, Fe(III) reduction is indicated by porewater Fe(II) concentrations increasing to 1.0–2.1 mM, and ~10–15 % of Fe as Fe(II,III)-(hydr)oxides (green rust), vivianite (Fe 3 (PO 4 ) 2 ·8H 2 O), and/or adsorbed Fe(II) species. EXAFS data also indicate reduction of structural Fe(III) to Fe(II) in phyllosilicates. The presence of Fe- and S-cycling bacteria, as well as sulfide (0–10 μM), suggests that Fe-cycling is microbially driven and potentially coupled with cryptic S-cycling. Fe(II) oxidation was indicated above/near the water table by the presence of Fe(III) oxyhydroxides (ferrihydrite, lepidocrocite). Furthermore, negligible Fe(III) or sulfate reduction was observed at some water-saturated sites located at the upland-wetland transition, likely due to oxic (sub-)surface water inputs. Overall, our results highlight the importance of considering both Fe-speciation and hydro-biogeochemical dynamics when predicting Fe-cycling at coastal interfaces.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Considerations for Defining G-Values for Aluminum-Clad Spent Nuclear Fuel

Sealed-canister dry storage of aluminum-clad spent nuclear fuel (ASNF) generated by research reactors is an alternative to current storage and disposition pathways as directed by the U.S. Department of Energy. The major challenge faced for this storage approach is radiolytic H 2 generation, including from the aluminum (oxy)hydroxide layers on the surface of ASNF. Experimental and modeling activities have been carried out to characterize the radiolytic yield as part of a DOE-sponsored research program to develop the technical basis for ASNF dry storage. The G-value is a commonly way to report results of radiolysis testing and is defined as the radiolytic yield of a species (e.g. molecular hydrogen) per unit radiation energy deposited into the material system. An independent technical review of the ASNF dry storage technical basis performed by Pacific Northwest National Laboratory raised questions about differences in G-value definitions used for experiments on ASNF surrogates consisting of aluminum samples with adherent (oxy)hydroxides compared to G-values reported in prior literature and how the magnitudes compared between different studies. Material systems resembling ASNF pose complications for measuring/defining G-values to predict the evolution of H 2 in a sealed canister, including i) accounting for radiolytic yields potentially arising from multiple sources, i.e., residual free (vapor), physisorbed, and chemisorbed/chemically bound waters; ii) deciding what portions of the multi-material system to include in the absorbed energy (radiation dose) calculation, considering possible energy exchange between materials as well as measurement limitations, and iii) capturing variations in G-value associated with non-linear yield vs. dose curves and/or dependence on the cover gas. This report summarizes previous literature information on radiolytic H 2 generation and associated G-values from mixed-material systems (generally oxides in contact with water or organic compounds) and from (oxy)hydroxides/hydrates to compare with the definitions and values for ASNF surrogate samples containing adherent aluminum (oxy)hydroxides.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Reinventing CEMENT: Carbonation-Enabled Mineralization to Engender Novel Technology

Cement is the most important building material used in civil infrastructure but it is extremely energy intensive to produce. We developed novel ways to make cements at low temperatures by mimicking the chemistry of the calcium silicate mineral pseudowollastonite. Pseudowollastonite is interesting because when it is exposed to hot (90-150oC), alkaline conditions with CO2 and water it reacts to form mineral phases that are much stronger than commercial cements. The resulting phases are also much more resistant to acid attack and have lower permeability, which will make them last longer. Many of the mineral phases in our cements are similar to those that exist in ancient Roman cements that have lasted thousands of years. Our objective was to understand how waste materials from industrial processes (such as power production, municipal solid waste treatment, or power plants) can be used to replicate the conditions that give pseudowollastonite cement its remarkable properties. We worked to optimize our formulations and incorporate the cements into concrete blends that the industry can test and consider using in different applications. Our cements could be used in pre-cast cement structural elements, which makes up nearly 20% of the total cement market and is growing rapidly. This work supports ARPA-E program objectives to significantly improve the industrial efficiency of materials production.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Opportunities for Treatment and Reuse of Agricultural Drainage in the United States

Irrigation accounts for 42% of the total freshwater withdrawals in the United States. Climate change, the pressure of a growing population, degrading water quality, and increased competition from other sectors could constrain continuous supply to meet future agricultural water demand. This study presents an evaluation framework to assess the potential reuse of agricultural drainage water for crop irrigation. Using a regional approach, we review the current state of agricultural drainage treatment and reuse and the institutional, economic, and other barriers that can influence the reuse decision. In the 31 eastern states, agricultural drainage contains valuable nutrients that can be reused for irrigation with minimal treatment, while the 17 western states struggle with large volumes of saline drainage that can contain constituents of concern (e.g., selenium), preventing reuse without treatment. Using a new decision-support tool called WaterTAP3, a potential treatment train for saline agricultural drainage was analyzed to identify treatment challenges, research needs, and the potential implementation at a larger scale. As demonstrated by our case study, desalination of agricultural drainage is costly and energy intensive and will require sizable investments to fully develop and optimize technologies as well as manage the generated waste and brine.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2021

A novel approach to mitigating the potential release of radioisotopes under fire conditions - enhancing fire resiliency of radiological contamination fixatives during deactivation & decommissioning activities

Savannah River National Laboratory (SRNL), in close collaboration with the Florida International University Applied Research Center (FIU ARC), successfully executed a technology development activity on behalf of the Department of Energy, Office of Environmental Management (DOE EM). The purpose of the activity was to improve the capability of fixative technologies in immobilizing residual contamination when exposed to thermal stressors as postulated in accident scenarios in Basis for Interim Operations (BIO) documents across the DOE EM complex. The effort resulted in the test and evaluation of a down-selected, commercial-off-the-shelf (COTS) intumescent technology in a radioactive environment at the Savannah River Site (SRS) Building 235-F Plutonium Fuel Form (PuFF) Facility and highlighted the potential use of this technology as a stand-alone, fire retardant fixative. Furthermore, this activity highlighted significant shortfalls in common fixatives currently used to support decommissioning activities and brought to the forefront the need for a methodical, uniformed approach to certifying fixative technologies for operational use in Deactivation and Decommissioning (D&D) activities. An essential component of this research was to evaluate the state of industry fixatives currently in use and set the foundation for comparison to alternative technological solutions. A baseline of five (5) commonly used fixatives and decontamination gels (hereafter collectively referred to as fixatives) was conducted, and notable shortfalls and deficiencies were revealed, particularly when exposed to thermal, water, and other environmental stressors. At temperatures as low as 300 °F - 400 °F (148.89 °C – 204.44 °C), all commonly used fixatives melted from the substrates within 3-5 minutes of exposure, resulting in contaminant transport. Significant degradation in terms of mass loss, desiccation, and off-gassing occurred, and the chemical breakdown of the polymer was so complete researchers assessed there would likely have been a release of residual contamination. Additional vulnerabilities became evident when exposed to water immersion and high humidity; existing fixatives took up water, swelling and frequently delaminating from the substrate, once again increasing the likelihood of a contaminant release.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

L-Basin Microbial Monitoring Program - Evaluation of 20 Years of Monitoring

The SRNL L-Basin corrosion surveillance and microbial monitoring programs provide early detection and characterization of corrosion attack to the fuel and storage system materials resulting from prolonged exposure to the L-Basin water environment and of changes to and impact of the diverse microbial population, respectively. The early detection of corrosion allows for adjustment of the water quality, engineering management, and fuel storage configurations to mitigate excessive corrosion attack. While microbial influenced corrosion in L-Basin has not been detected, tracking and understanding the effect of microbial populations on the stored fuel and basin water will aid in identifying remedial measures to mitigate any detrimental impact. This report reviews the microbial monitoring activities since initial characterizations in the mid-1990s.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Laboratory Evaluation to Increase Effectiveness of Field-Scale Soil Flushing in the Hanford 100 Areas

This laboratory study was initiated to develop an improved technical understanding of the key controlling geochemical and physical processes of mobilizing residual Cr(VI) in Hanford sediments to provide increased effectiveness in soil flushing activities planned for Hanford 100 Areas. This was accomplished by (1) quantifying Cr mass, release rate, and surface phase changes as Cr is leached from different Hanford sediments; (2) maximizing Cr leaching during soil flushing by evaluating different leach solutions and leach strategies; and (3) minimizing leaching of remaining residual Cr after soil flushing ends. To quantify geochemical controls on Cr leaching from sediments, sequential liquid extractions were used to identify aqueous, adsorbed, and solid Cr surface phases (precipitates or Cr incorporated into other phases) before and after water-saturated and unsaturated leach experiments with pH 8 artificial groundwater and with other amendment solutions. Changes in the Cr release rate from sediments were also correlated to changes in Cr surface phases. During unsaturated infiltration, water advection occurs primarily through larger pores, with less movement through smaller grain layers leading to a slower release of Cr trapped in smaller pores next to smaller grains. To quantify these physical controls on Cr leaching from sediments, 10 ft high 1-D infiltration experiments were conducted at differing leach solution application rates, and Cr leaching during application and subsequent residual water flow was quantified. Qualitative 2-D experiments were also conducted to evaluate surfactant addition to increase flow in low-permeability zones. Cr-contaminated Hanford sediments from the 100-H, 100-K, 100-D, and 200 East Areas exhibited a wide variety of leach behavior from rapid release of a small amount of Cr to fast (i.e., minutes) and slow (i.e., hours or more) release of high Cr. Sediments with low labile Cr (< 0.2 µg/g) exhibited fast Cr release but less overall release, and most (>95%) leached from the sediments within a few pore volumes in water-saturated columns. With nearly no sorption of chromate, aqueous and sorbed Cr (as chromate) were released quickly from sediment within the first few pore volumes, resulting in high leach concentrations, fast initial Cr release rates, and changes in pre- and post-leach extractions. In contrast, sediments with high labile Cr (0.2 to 20 µg/g) exhibited a combination of fast and slow Cr release due to multiple Cr surface phases contributing to Cr release from the sediment at different rates with greater overall release. This resulted in elevated Cr effluent concentrations even after dozens of pore volumes were leached. In addition, the Cr release rate decreased with increasing time during leaching. A decrease in labile Cr (aqueous Cr, adsorbed Cr, pH 5 acetate dissolved precipitates) in post-leach extractions compared to pre-leach extractions showed initial aqueous and adsorbed Cr release, followed by dissolution of high-solubility precipitates such as CaCrO 4 (if present), then slow dissolution of calcite that may contain some chromate and possibly BaCrO 4 . The labile Cr in all sediments correlated well with the Cr release rate (r 2 = 0.81). Labile Cr also correlated well with the leached mass in water-saturated columns (r 2 = 0.98), and therefore can be used for prediction of potential removal with flushing applications.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

CFA-17-12798: Nanostructured Ceramic Membranes for Enhanced Tritium Management

This project focuses on the novel use of interfacial hydrated layers in ionic conducting ceramic materials for tritiated water (HTO) adsorption and recovery. Low-temperature water adsorption properties of nanoscale structured ceramics combined with hydrogen isotope exchange in their hydrated layers could provide a low-cost and transformative avenue to address tritium management challenges.

08 HYDROGEN↗
DOE OSTI2020

Hanford Double Shell Waste Tank Corrosion Studies (Final Report FY2019)

During fiscal year (FY) 2019, the Savannah River National Laboratory (SRNL) focused on four primary tasks for Hanford Double Shell Tanks (DSTs) corrosion studies. The first task, New Limits, was a continuation from the electrochemical work started in FY16, to expand electrochemical testing to elevated temperatures and elevated hydroxide concentrations and evaluate how these factors will influence pitting corrosion. Using the pitting factor (PF) equation, these new conditions were validated to provide a conservative estimate for the susceptibility of pitting corrosion on legacy carbon steel. The second task, Secondary Liner Corrosion, focused on Vapor Space Corrosion (VSC) and immersion testing studies using two commercially available vapor corrosion inhibitors (VCIs). For this FY, the VCI strategy was applied mid-experiment to determine performance on weathered coupons. The third task, Long-Term Open Circuit Potential (OCP) Drift, was performed using simplified simulated chemistries to evaluate change in pitting corrosion risk due to evolution of corrosion potential for mill-scale and freshly polished 600-grit surfaces. Finally, the fourth task, Microbiologically-Influenced Corrosion (MIC) studies, was focused on the study of leak detection pit (LDP) water sent from the Hanford tank farm for determination of bacteria that can be conducive to corrosion using commercially available kits: BART TM and MICkit® 5. In addition, this FY, a secondary task was added which was a continuation of the study of the Quartz-enhanced Photoacoustic Spectroscopy (QEPAS) system. Work was started but was ultimately not pursued. A summary of each task performed is presented below.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Basket Modification Concepts for Disposal Reactivity Control of Dual Purpose Canisters

This report documents work performed supporting the US Department of Energy (DOE) Office of Nuclear Energy (NE) Spent Fuel and Waste Disposition (SFWD), Spent Fuel and Waste Science and Technology, under work breakdown structure element 1.08.01.03.05, “Direct Disposal of Dual Purpose Canisters.” In particular, this report fulfills milestone M3SF-21OR010305125, “DPC criticality analysis with fuel/basket modification,” within work package SF-21OR01030512, “DPC Reactivity and Criticality Modeling—ORNL.” This report uses three of the most reactive canisters that have been analyzed to-date using UNFST&DARDS to examine the performance of three potential reactivity suppression technologies under disposal conditions. Three already loaded canisters were analyzed using as-loaded contents including TSC-37 and MPC-32 pressurized water reactor (PWR) dual-purpose canisters (DPCs) and the MPC-89 DPCs. The reactivity suppression technologies considered were the B4C-filled disposal control rod assembly (DCRA) and the advanced neutron absorber (ANA)–based chevron insert for the PWR canisters and the ANA-based fuel channel replacement absorber for the MPC-89. For each combination of absorber concept and DPC, various insert patterns and absorber material concentrations were considered. The results of the analysis show that the DCRA concept has promise for providing reactivity hold-down for PWR DPCs, and the ANA fuel channel replacement absorber has promise for providing reactivity holddown in BWR DPCs. The ANA chevron basket insert showed mixed results, providing sufficient reactivity hold-down in the lower reactivity canister, but failing to do so in the higher reactivity canister considered herein.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Coupling Interfacial Redox‐Reactions with In Situ Proton Generation for the Photoelectrochemical Separation of Rare‐Earth Elements

Abstract A dual‐function photoelectrochemical (PEC) separation system is demonstrated for rare‐earth element (REE) recovery. The sustainable release of the captured REEs is promoted through the synergistic integration of a redox‐reaction for electrostatic repulsion, and in situ proton generation for ion‐exchange, all driven by photoelectrochemistry. The platform consists of a redox‐copolymer, poly(ferrocenylpropyl methacrylamide‐ co ‐methacrylic acid) (P(FPMAm‐ co ‐MAA)) (PFM), conjugated with carbon nanotubes (CNTs) and coated onto titanium dioxide nanorods (TNRs). The (PFM‐CNT)/TNR spontaneously adsorbs up to 214.2 mg of Yttrium/g PFM by ion‐exchange, and demonstrates broad applicability for other REEs. The adsorbed REEs are released through the PEC oxidation of ferrocene (Fc) to ferrocenium (Fc + ), and the simultaneous PEC water splitting reactions at the TNRs that protonate the carboxylate binding groups. This dual photoelectrochemically‐driven mechanism for REE release is investigated by in situ pH measurements, as well as vibrational and X‐ray photoelectron spectroscopy. Through PEC approaches, a 68.8% reduction in energy consumption during REE recovery has been achieved compared to purely electrochemical systems, with a regeneration efficiency close to 100%. For NdFeB magnets from waste hard disk drives, Nd and Dy recovery efficiencies of 59.2 and 61.1% are achieved. The dual‐functionality of these copolymer PEC systems offers a sustainable platform for modulating critical element recovery.

Cho, Ki‐Hyun [Department of Chemical and Biomolecu↗