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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 325 records · Page 18

Metal-Organic Framework Glasses as Rad Contaminant Sequesters and Nuclear Waste Forms

Remediation of Tc remains an unresolved problem at SRS and other DOE sites. The objective of this project was to develop novel metal organic framework (MOF) glasses for radioactive contaminant sequestration and stabilization from aqueous media. During FY20, we synthesized, characterized and evaluated additional cetyltrimethylcimmonium bromide (CTAB)-functionalized and F - , Cl - , I - , CF 3 SO 3 - exchanged MIL-101-Cr samples. MIL-10l-Cr-NO 3 -CTAB was demonstrated to have high ReO 4 - removed capacity (139 mg/g sorbent) from artificial groundwater (AGW). Re chemical specicition and binding mechanism on MIL-101-CTAB were also studied by synchrotron X-ray absorption spectroscopy. ReO 4 - was demonstrated as being in the pore structure with slightly larger Re-O bond distances than those in NciReO 4 and binding with the positively charged sites of CTAB. In addition, a new Ni-TIPA MOF was demonstrated to be very stable, selective and effective for TcO 4 - removed from the SRS tank waste stream (~90% removed). The Ni-TIPA MOF sample containing ReO 4 - was prepared and shipped/planned for vitrification studies by a high-pressure technique. This research may provide a highly applicable platform for solving critical DOE and industrial problems related to nuclear environmental stewardship and nuclear power production.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Generation and Characteristics of Plutonium and Americium Contaminated Soils Underlying Waste Sites at Hanford

In 2012, a Hanford site-wide review on plutonium and americium geochemistry (Cantrell and Felmy 2012) identified remaining research challenges associated with defining scientifically defensible end-states and supporting remediation decisions. Three research challenges were identified in this review: 1. Determine the transformations of Hanford Site sediments in response to changes in waste/groundwater composition. Significant mineralogical transformations can take place when wastes contact Hanford sediments. These transformations can significantly impact the solubility and acidic adsorption of plutonium and americium and possibly result in the generation of pseudo colloids that could facilitate plutonium/americium migration. 2. Assess the impact of changes in waste/groundwater chemistry on the potential for plutonium/americium solubilization or colloid formation. Changes in waste or groundwater chemistry can greatly impact the chemical form or speciation of plutonium and americium. Knowledge of plutonium and americium speciation will be crucial in terms of evaluating the potential for solubilization, adsorption or remobilization of adsorbed complexes, colloid formation, and colloid interactions with sedimentary minerals. 3. Establish the role of organic complexants and/or non-aqueous solvents in the transport of plutonium/americium in the deep subsurface. Plutonium has been found to be associated with TBP and the presence of non-aqueous solvents, at least in certain Z-9 sediments. It will be important to establish the role of non-aqueous solvent in past movement of plutonium and its potential role in future mobility. This report provides the technical basis for interpreting data obtained from field samples and will allow waste chemistry impacts on plutonium/americium re-mobilization mechanisms to be assessed. This report helps address the three previously identified research challenges – sediment transformations, solution chemistry impacts, and the role of organic complexants and solvents – in plutonium and americium contaminated Hanford sediments. Ultimately, these and potential future studies will lead to a defensible description of plutonium and americium mobility in relation to waste site conditions that can be interpreted to balance the risks posed by their migration and envisioned remediation activities.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NTS-SS-SNL-NMSITE-2017-0004,"Contamination Monitor Left in Service After Inadequate Calibration" Causes Not Fully Addressed (ES&H Causal Analysis Report)

Sandia National Laboratories Radiation Protection department did not successfully address the causes leading to the issue NTS-SS-SNL-NMSITE-2017-0004, “Contamination Monitor Left in Service After Inadequate Calibration”, nor identify through the verification and validation process that corrective actions were not fully implemented and effective at addressing the issue(s). This report is the third causal in four years associated with the iPCM12 instrument and the Radiation Protection Instrumentation (RPI) organization within Radiation Protection (00628).

61 RADIATION PROTECTION AND DOSIMETRY↗

NTS-SS-SNL-NMSITE-2017-0004 "Contamination Monitor Left in Service After Inadequate Calibration" Causes Not Fully Addressed (Causal Analysis Report)

On June 5th, 2020 Sandia National Laboratories signed and recommended for closure the evidence package for the Noncompliance Tracking System NTS—SS-SNL-NMSITE-2017-0004, Contamination Monitor Left in Service After Inadequate Calibration. On July 16th, 2020 the Sandia Field Office sent a follow-up question list to the Radiation Protection Instrumentation Program Lead to clarify some points while reviewing the evidence package. The follow-up questions readily identified deficiencies with all three calibrations of the iPCM12 systems. On July 30th, 2020 Radiation Protection hosted a meeting to better understand the exact nature of the concerns, determine if the iPCM12 machines were out of calibration and therefore would have to be taken out of service. One result of this meeting was to determine if SNL could withdraw the evidence package. SNL transmitted a letter on August 26th, 2020 recalling the evidence package and committed to performing a thorough causal analysis and invoke the required issues management processes to ensure that corrective actions are sustained.

54 ENVIRONMENTAL SCIENCES↗

Preliminary Deposition Modeling: For Determining the Deposition of Corrosive Contaminants on SNF Canisters

This report fulfills the M3 milestone M3SF-20PN010207045. During fiscal year (FY) 2019, Pacific Northwest National Laboratory (PNNL) worked to develop initial deposition and particle tracking models which could be used to better understand how corrosive contaminants deposit on the surfaces of spent nuclear fuel (SNF) canisters during dry storage. These models may be useful in understanding the likelihood of chloride induced stress corrosion cracking (CISCC) on SNF canisters

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Gaussian process regression for radiological contamination mapping- Applied to optimal motion planning for mobile sensor platforms [Slides]

Want to achieve best representative characterization of the entire area efficiently and accurately-Unmanned aerial/ground vehicles (UAV/UGVs) for contamination mapping. Some major challenges include: Limited battery life (move smart), Human operated (fully autonomous controls) and Many measurements (predictive mapping capabilities). The objective: Develop fully autonomous controls for mobile sensor platforms to improve efficiency and maintain performance.

61 RADIATION PROTECTION AND DOSIMETRY↗

Marshall Islands Dose Assessment and Radioecology Program: Report on the (i) 2018 Visual Study of Exterior Concrete of the Cactus Crater Containment Structure (ii) Periodic Monitoring of Groundwater on Runit Island and (iii) Initial Health Risk Assessment from Contaminants in the Cactus Crater Containment Structure

In 2012, Congress passed P.L. 112-149, Insular Areas Act of 2011, which amended the Compact of Free Association Amendments Act of 2003 by assigning Cactus Crater containment monitoring and reporting requirements to the Secretary of Energy (Secretary). Effective January 1, 2012, the Secretary was required to “periodically (but not less frequently than every 4 years) conduct -- (I) a visual study of the concrete exterior of the Cactus Crater Containment Structure on Runit Island; and (II) a radiochemical analysis of the groundwater surrounding and in the Cactus Crater Containment Structure on Runit Island.” 48 U.S.C. 1921b(f)(1)(B)(i). The Secretary was also directed to submit to Congress a report describing the results of each visual survey and the radiochemical analysis and “a determination on whether the surveys and analyses indicate any significant change in the health risks to the people of Enewetak from the contaminants within the Cactus Crater Containment Structure.” 48 U.S.C. 1921b(f)(1)(B)(ii)(II).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Hanford Site Composite Analysis Special Analysis: P2R Model Predictive Contaminant Transport Simulations - Sensitivity Case

This environmental calculation file (ECF) documents the methodologies, assumptions, and results of predictive fate and transport simulations using the Plateau-to-River (P2R) model. This ECF supports the reevaluation of the representativeness of solid-waste radionuclide inventory and release rate from three solid waste sites included in the recently completed Hanford Site Composite Analysis (CA) (DOE-RL-2019-52, Composite Analysis for Low-Level Waste Disposal in the Hanford Site Central Plateau (FY 2020)). Specifically, this ECF supports the reevaluation of the representativeness of the base case inventory and radionuclide waste release rates from three solid waste sites (i.e., 218-E-12B, 218-W-3A and 218-W-3AE) and two radionuclides (carbon-14 [C-14] and technetium [Tc-99]). These three waste sites and two radionuclides were identified as being the most significant contributors to groundwater contamination and dose in the CA at time periods after the compliance period. The release rates and footprints of the releases from the vadose zone are implemented in the fate and transport modeling utilizing the HSS package.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Behavior of contaminants and simulant fission products in the advanced chlorination process

The University of Tennessee, Knoxville and Oak Ridge National Laboratory have completed proof-of principle testing on an advanced sulfur-based zirconium and aluminum chlorination process for the recovery of Zr or Al from spent fuel claddings and purification of the products. This process could be used to recover hafnium-free nuclear-grade zirconium for reuse or disposal as low-level waste. Testing showed that even non-optimized reaction protocols could produce zirconium product streams from simulated irradiated fuel with purities >90%. The chlorination process was tested on representative fission product species that would be found in Advanced Test Reactor fuel (ATR). First, fission product generation was determined through modeling and simulation of the ATR. The generation of fission products was used to selected contaminants and potentially volatile fission product simulants for laboratory testing. The goal is to identify which species may react with the sulfur-chlorine reagents and be transported into the advanced chlorination off-gas.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Understanding Surface Contamination Effects in Mid-T Baked Cavities

Medium-temperature baking is applied to niobium SRF cavities to enhance their quality factor. However, mid-T baking performed in the 300-350 °C range may lead to the formation of surface carbides, which can prevent the cavities from exhibiting the full benefit of mid-T baking. To investigate the effect of potential surface contaminants, the top RF layer of mid-T-baked cavities was removed using an ultralight electropolishing process. The performance of the mid-T baked cavities was significantly improved after applying this ultralight EP. This presentation summarizes the latest results on this study.

Chouhan, Vijay [Fermilab]↗

Identifying the speciation of salt-based actinides in the presence of contaminants [Slides]

Molten salt reactors (MSR) present advantages over light water reactors, such as higher safety and energy efficiency, convenient waste processing, and the ability to use more abundant thorium instead of uranium as the fuel source. However, due to the high temperatures associated with these reactors the reactor container corrosion product can have a high influence on the molten salt system, and they are considered as a part of the fuel salt system. It is essential to have a comprehensive understanding of the chemical reactions that are occurring in the molten salt in the presence of contaminants such as nickel, manganese, chromium chlorides and oxides. Because they can change the local structure of these salts and the local structures of these salts govern the thermophysical properties of the molten salts, which would determine the safety and operational parameters of the reactor. This study is focused on identifying f-element materials speciation resulting from reaction with corrosion/degradation products in a molten salt environment to understand the flow of MSR. In this work, f-element chlorides are mixed with alkali and alkali earth metals and corrosion products such as transition metal chlorides are introduced systematically, inside a glovebox. Then these are heated to around 700 ? and slowly cooled to room temperature. Afterwards, these are analyzed using different characterization techniques such as powder X-ray diffraction, UV-vis and Raman spectroscopy and solid-state NMR. The initial work was conducted with lanthanide chlorides as a surrogate for actinides and the acquired data strongly indicates that in the presence of corrosion products new phase formation/ change in coordination environments occurs. This work has been presented at multiple conference presentations. The proposed work would allow to extend this work to actinides (depleted uranium and thorium) and this would assist to identify the speciation of actinide chloride in the presence of corrosion products. Also, this work would open an opportunity to compare the coordination behavior of lanthanides with the actinides.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

Nutrient Exposure Alters Microbial Composition, Structure, and Mercury Methylating Activity in Periphyton in a Contaminated Watershed

The conversion of mercury (Hg) to monomethylmercury (MMHg) is a critical area of concern in global Hg cycling. Periphyton biofilms may harbor significant amounts of MMHg but little is known about the Hg-methylating potential of the periphyton microbiome. Therefore, we used high-throughput amplicon sequencing of the 16S rRNA gene, ITS2 region, and Hg methylation gene pair (hgcAB) to characterize the archaea/bacteria, fungi, and Hg-methylating microorganisms in periphyton communities grown in a contaminated watershed in East Tennes(see United States). Furthermore, we examined how nutrient amendments (nitrate and/or phosphate) altered periphyton community structure and function. We found that bacterial/archaeal richness in experimental conditions decreased in summer and increased in autumn relative to control treatments, while fungal diversity generally increased in summer and decreased in autumn relative to control treatments. Interestingly, the Hg-methylating communities were dominated by Proteobacteria followed by Candidatus Atribacteria across both seasons. Surprisingly, Hg methylation potential correlated with numerous bacterial families that do not contain hgcAB, suggesting that the overall microbiome structure of periphyton communities influences rates of Hg transformation within these microbial mats. To further explore these complex community interactions, we performed a microbial network analysis and found that the nitrate-amended treatment resulted in the highest number of hub taxa that also corresponded with enhanced Hg methylation potential. This work provides insight into community interactions within the periphyton microbiome that may contribute to Hg cycling and will inform future research that will focus on establishing mixed microbial consortia to uncover mechanisms driving shifts in Hg cycling within periphyton habitats.

59 BASIC BIOLOGICAL SCIENCES↗

Understanding Contaminant Migration within a Dynamic River Corridor through Field Experiments and Reactive Transport Modeling

The behavior of a persistent uranium plume within an extended river corridor at the DOE Hanford site is dominantly controlled by river stage fluctuations in the adjacent Columbia River. The plume behavior is further complicated by substantial heterogeneity in physical and geochemical properties of the host aquifer sediments. Multi-scale field and laboratory experiments and reactive transport modeling were integrated to understand the complex plume behavior influenced by highly variable hydrologic and geochemical conditions in time and space. In this paper, we (1) describe multiple data sets from field-scale uranium adsorption and desorption experiments performed at our experimental well-field, (2) develop a reactive transport model that incorporates hydrologic and geochemical heterogeneities characterized from multi-scale and multi-type datasets and a surface complexation reaction network based on laboratory studies, and (3) compare the modeling and observation results to provide insights on how to refine the conceptual model and reduce prediction uncertainties. The experimental results revealed significant spatial variability in uranium adsorption/desorption behavior, while modeling demonstrated that ambient hydrologic and geochemical conditions and heterogeneities in sediment physical and chemical properties both contributed to complex plume behavior and its persistence. This research underscores the great challenges in adequately characterizing this type of site to model the reactive transport processes over scales of 10 m or more. Our analysis provides important insights into the characterization, understanding, modeling, and remediation of groundwater contaminant plumes influenced by dynamic surface water and groundwater interactions.

Chen, Xingyuan↗

A Graphics Processing Unit (GPU) Approach to Large Eddy Simulation (LES) for Transport and Contaminant Dispersion

Recent advances in the development of large eddy simulation (LES) atmospheric models with corresponding atmospheric transport and dispersion (AT&D) modeling capabilities have made it possible to simulate short, time-averaged, single realizations of pollutant dispersion at the spatial and temporal resolution necessary for common atmospheric dispersion needs, such as designing air sampling networks, assessing pollutant sensor system performance, and characterizing the impact of airborne materials on human health. The high computational burden required to form an ensemble of single-realization dispersion solutions using an LES and coupled AT&D model has, until recently, limited its use to a few proof-of-concept studies. An example of an LES model that can meet the temporal and spatial resolution and computational requirements of these applications is the joint outdoor-indoor urban large eddy simulation (JOULES). A key enabling element within JOULES is the computationally efficient graphics processing unit (GPU)-based LES, which is on the order of 150 times faster than if the LES contaminant dispersion simulations were executed on a central processing unit (CPU) computing platform. JOULES is capable of resolving the turbulence components at a suitable scale for both open terrain and urban landscapes, e.g., owing to varying environmental conditions and a diverse building topology. In this paper, we describe the JOULES modeling system, prior efforts to validate the accuracy of its meteorological simulations, and current results from an evaluation that uses ensembles of dispersion solutions for unstable, neutral, and stable static stability conditions in an open terrain environment.

54 ENVIRONMENTAL SCIENCES↗

Biogeochemical Controls on the Potential for Long-Term Contaminant Leaching from Soils Developing on Historic Coal Mine Spoil

Coal mine spoil is widespread in US coal mining regions, and the potential long-term leaching of toxic metal(loid)s is a significant and underappreciated issue. This study aimed to determine the flux of contaminants from historic mine coal spoil at a field site located in Appalachian Ohio (USA) and link pore water composition and solid-phase composition to the weathering reaction stages within the soils. The overall mineralogical and microbial community composition indicates that despite very different soil formation pathways, soils developing on historic coal mine spoil and an undisturbed soil are currently dominated by similar mineral weathering reactions. Both soils contained pyrite coated with clays and secondary oxide minerals. However, mine spoil soil contained abundant residual coal, with abundant Fe- and Mn- (oxy)hydroxides. These secondary phases likely control and mitigate trace metal (Cu, Ni, and Zn) transport from the soils. While Mn was highly mobile in Mn-enriched soils, Fe and Al mobility may be more controlled by dissolved organic carbon dynamics than mineral abundance. There is also likely an underappreciated risk of Mn transport from coal mine spoil, and that mine spoil soils could become a major source of metals if local biogeochemical conditions change.

58 GEOSCIENCES↗