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DOE OSTI2025

Syntrophic bacterial and host–microbe interactions in bacterial vaginosis

Bacterial vaginosis (BV) is a common, polymicrobial condition of the vaginal microbiota that is associated with symptoms such as malodor and excessive discharge, along with increased risk of various adverse sequelae. Host–bacteria and bacteria–bacteria interactions are thought to contribute to the condition, but many of these functions have yet to be elucidated. Using untargeted metaproteomics, we identified 1068 host and 1418 bacterial proteins in a set of cervicovaginal lavage samples collected from 20 participants with BV and 9 who were negative for the condition. We identified Dialister micraerophilus as a major producer of malodorous polyamines and identified a syntrophic interaction between this organism and Fannyhessea vaginae that leads to increased production of putrescine, a metabolite characteristic of BV. Although formate synthesis has not previously been noted in BV, we discovered diverse bacteria associated with the condition express pyruvate formate-lyase enzymes in vivo and confirm these organisms secrete formic acid in vitro. Sodium hypophosphite efficiently inhibited this function in multiple taxa. We also found that the fastidious organism Coriobacteriales bacterium DNF00809 can metabolize formic acid secreted by Gardnerella vaginalis, representing another syntrophic interaction. We noted an increased abundance of the host epithelial repair protein transglutaminase 3 in the metaproteomic data, which we confirmed by enzyme-linked immunosorbent assay. Other proteins identified in our samples implicate Finegoldia magna and Parvimonas micra in the production of malodorous trimethylamine. Some bacterial proteins identified represent novel targets for future therapeutics to disrupt BV communities and promote vaginal colonization by commensal lactobacilli.

bacterial vaginosis↗

DOE OSTI2022

Identification of a new circulating recombinant form of human immunodeficiency virus type 1, CRF124_cpx involving subtypes A, G, H, and CRF27_cpx in Angola

Angola, located in Central Africa, has around 320,000 (270,000–380,000) people living with human immunodeficiency virus (HIV)/AIDS, equivalent to 1% of the country’s population at the end of 2021. A previous study conducted in 2012, using Angolan samples collected between 2008 and 2010 revealed a high prevalence of HIV-1 recombinants, around 42% of sequences, with 21% showing the same UH profile in partial pol region which were grouped into a monophyletic cluster with high bootstrap support. Thus, the objective of the present work was to obtain complete genomes of those sequences and characterize them, aiming at a description of a new circulating recombinant form (CRF). Whole blood from nine HIV-1 UH pol -infected individuals had their genomic DNA extracted, and nested PCR was used to amplify seven overlapping fragments targeting the full-length HIV-1 genome. The final classification was based on maximum likelihood trees, and recombination analyses were performed using a bootscan from the Simplot program. BLAST and Los Alamos Database inspections were used to search other similar H-like pol sequences. Complete genome amplification was possible for three samples, partial genomes were obtained for the other three, and only pol was available for the remaining three sequences. Bootscan analysis of the two whole-genome and three partial genome sequences retrieved from people living with HIV/AIDS (PLHIVA) without epidemiological linkage showed the same complex recombination profile involving HIV-1 subtypes A/G/H/CRF27_cpx, with a total of six recombinant breakpoints, aiming to classify a new HIV-1 CRF124_cpx. We found no other full-length HIV-1 genomes with the same mosaic profile; however, we identified 33 partial pol sequences, mainly sampled from Angola between 2001 to 2019, with the same H-like profile. Bayesian analysis of H and H-like pol sequences indicates that CRF124_cpx probably originated in Angola at mid-1970s, indicating that this CRF has been circulating in the country for a long time. In summary, our study describes a new CRF circulating principally in Angola and highlights the importance of continuing molecular surveillance studies, especially in countries with high molecular diversity of HIV.

60 APPLIED LIFE SCIENCES↗

NASA NTRS2010

Heart Rate Response During Mission-Critical Tasks After Space Flight

Adaptation to microgravity could impair crewmembers? ability to perform required tasks upon entry into a gravity environment, such as return to Earth, or during extraterrestrial exploration. Historically, data have been collected in a controlled testing environment, but it is unclear whether these physiologic measures result in changes in functional performance. NASA?s Functional Task Test (FTT) aims to investigate whether adaptation to microgravity increases physiologic stress and impairs performance during mission-critical tasks. PURPOSE: To determine whether the well-accepted postflight tachycardia observed during standard laboratory tests also would be observed during simulations of mission-critical tasks during and after recovery from short-duration spaceflight. METHODS: Five astronauts participated in the FTT 30 days before launch, on landing day, and 1, 6, and 30 days after landing. Mean heart rate (HR) was measured during 5 simulations of mission-critical tasks: rising from (1) a chair or (2) recumbent seated position followed by walking through an obstacle course (egress from a space vehicle), (3) translating graduated masses from one location to another (geological sample collection), (4) walking on a treadmill at 6.4 km/h (ambulation on planetary surface), and (5) climbing 40 steps on a passive treadmill ladder (ingress to lander). For tasks 1, 2, 3, and 5, astronauts were encouraged to complete the task as quickly as possible. Time to complete tasks and mean HR during each task were analyzed using repeated measures ANOVA and ANCOVA respectively, in which task duration was a covariate. RESULTS: Landing day HR was higher (P < 0.05) than preflight during the upright seat egress (7%+/-3), treadmill walk (13%+/-3) and ladder climb (10%+/-4), and HR remained elevated during the treadmill walk 1 day after landing. During tasks in which HR was not elevated on landing day, task duration was significantly greater on landing day (recumbent seat egress: 25%+/-14 and mass translation: 26%+/-12; P < 0.05). CONCLUSION: Elevated HR and increased task duration during postflight simulations of mission-critical tasks is suggestive of spaceflight-induced deconditioning. Following short-duration microgravity missions (< 16 d), work performance may be transiently impaired, but recovery is rapid.

Arzeno, Natalia M.↗

NASA NTRS1999

Space Weathering in the Fine Size Fractions of Lunar Soils: Soil Maturity Effects

The effects of space weathering on the optical properties of lunar materials have been well documented. These effects include a reddened continuum slope, lowered albedo, and attenuated absorption features in reflectance spectra of lunar soils as compared to finely comminuted rocks from the same Apollo sites. However, the regolith processes that cause these effects are not well known, nor is the petrographic setting of the products of these processes fully understood. A Lunar Soil Characterization Consortium has been formed with the purpose of systematically integrating chemical and mineralogical data with the optical properties of lunar soils. Understanding space-weathering effects is critical in order to fully integrate the lunar sample collection with remotely-sensed data from recent robotic missions (e.g., Lunar Prospector, Clementine, and Galileo) We have shown that depositional processes (condensation of impact-derived vapors, sputter deposits, accreted impact material, e.g., splash glass, spherules, etc.) are a major factor in the modification of the optical surfaces of lunar regolith materials. In mature soils, it is the size and distribution of the nanophase metal in the soil grains that has the major effect on optical properties. In this report, we compare and contrast the space-weathering effects in an immature and a mature soil with similar elemental compositions. For this study, we analyzed <10 micron sieve fractions of two Apollo 17 soils, 79221 (mature, Is/FeO = 81) and 71061 (immature, Is/FeO = 14). Details of the sieving procedures and allocation scheme are given else where. The results of other detailed chemical, mineralogical, and spectroscopic analyses of these soil samples are reported elsewhere. A representative sample of each soil was embedded in low-viscosity epoxy, and thin sections (about 70nm thick) were obtained through ultra microtomy. The thin sections used for these analyses typically contained cross sections of up to 500 individual grains. The thin sections were studied using a JEOL 2010 transmission electron microscope (TEM) equipped with a thin window energy-dispersive X-ray (EDX) spectrometer. An individual thin section was selected from each soil, and for each grain in the section we determined (1) the elemental composition by EDX; (2) whether the grain was crystalline or glassy using electron diffraction and darkfield imaging; (3) the presence or absence of rims and accreted material; and (4) the distribution of nanophase Fe where present. Most of the categories are self-evident; however, we divide the agglutinate derived material into agglutinitic glass (glass with approximately the same composition as the bulk soil that contains nanophase Fe with or without vesicles) and agglutinate fragments, which are composed of crystalline grains and agglutinitic glass. Lithic fragments are defined as polymineralic grains with no glass. Pyroxene grains have been divided into high- and low-Ca groups. As expected, there are a number of differences in the petrography of the <10-microns fractions of 79221 and 71061 given the great difference in their respective maturities, but we focus here on two major distinctions: agglutinate content and the number of grains with micropatina. Slightly over 50% of the particles in 79221 consist of agglutinitic glass and agglutinate fragments, while the remainder are predominantly crystalline mineral grains. The agglutinic glass particles contain abundant nanophase Fe and vesicles. Angular particles are rare, with most showing smooth, rounded exteriors, Of the mineral grains analyzed thus far, over 90% of the grains have amorphous rims that contain nanophase Fe (these rims are believed to have formed by vapor deposition and irradiation effects). The nanophase Fe in these rims probably accounts for a significant fraction of the increase in Is/FeO measured in these size fractions. In addition to the rims, the majority of particles also show abundant accreted material in the form of glass splashes and spherules that also contain nanophase Fe. In stark contrast, the surfaces of the mineral grains in the 71061 sample are relatively prisitine, as only about 14% of the mineral grains in the sample exhibited amorphous rims. Furthermore, the mineral particles are more angular and show greater surface roughness than in the mature sample. Accreted material on particle surfaces is rare. Agglutinitic material is a major component of the 71061 sample; however, nanophase Fe and vesicles are not as well developed as in the 79221 sample. It is now recognized that nanophase Fe is probably the main agent in modifying the optical properties of lunar soil grains. The most important result of this study is the observation that in the fine size fractions of mature soils, nearly every grain has nanophase Fe within 100 run of the particle surface. (Additional Information contained in original)

Keller, L. P.↗

DOE OSTI2015

Development of a low background liquid scintillation counter for a shallow underground laboratory

Pacific Northwest National Laboratory has recently opened a shallow underground laboratory intended for measurement of lowconcentration levels of radioactive isotopes in samples collected from the environment. The development of a low-background liquid scintillation counter is currently underway to further augment the measurement capabilities within this underground laboratory. Liquid scintillation counting is especially useful for measuring charged particle (e.g., B, a) emitting isotopes with no (orvery weak) gamma-ray yields. The combination of high-efficiency detection of charged particle emission in a liquid scintillation cocktail coupled with the low-background environment of an appropriately-designed shield located in a clean underground laboratory provides the opportunity for increased-sensitivity measurements of a range of isotopes. To take advantage of the 35-meter water-equivalent overburden of the underground laboratory, a series of simulations have evaluated the instrumental shield design requirements to assess the possible background rate achievable. This report presents the design and background evaluation for a shallow underground, low background liquid scintillation counter design for sample measurements.

liquid scintillation counting↗

DOE OSTI2018

Using strontium isotopes to evaluate the spatial variation of groundwater recharge

Recharge of alluvial aquifers is a key component in understanding the interaction between floodplain vadose zone biogeochemistry and groundwater quality. The Rifle Site (a former U-mill tailings site) adjacent to the Colorado River is a well-established field laboratory that has been used for over a decade for the study of biogeochemical processes in the vadose zone and aquifer. This site is considered an exemplar of both a riparian floodplain in a semiarid region and a post-remediation U-tailings site. In this paper we present Sr isotopic data for groundwater and vadose zone porewater samples collected in May and July 2013 to build a mixing model for the fractional contribution of vadose zone porewater (i.e. recharge) to the aquifer and its variation across the site. The vadose zone porewater contribution to the aquifer ranged systematically from 0% to 38% and appears to be controlled largely by the microtopography of the site. The area-weighted average contribution across the site was 8% corresponding to a net recharge of 7.5 cm. Given a groundwater transport time across the site of ~1.5 to 3 years, this translates to a recharge rate between 5 and 2.5 cm/yr, and with the average precipitation to the site implies a loss from the vadose zone due to evapotranspiration of 83% to 92%, both ranges are in good agreement with previously published results by independent methods. A uranium isotopic ( 234 U/ 238 U activity ratios) mixing model for groundwater and surface water samples indicates that a ditch across the site is hydraulically connected to the aquifer and locally significantly affects groundwater. Groundwater samples with high U concentrations attributed to natural bio-reduced zones have 234 U/ 238 U activity ratios near 1, suggesting that the U currently being released to the aquifer originated from the former U-mill tailings.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Modeling geogenic and atmospheric nitrogen through the East River Watershed, Colorado Rocky Mountains

There is a growing understanding of the role that bedrock weathering can play as a source of nitrogen (N) to soils, groundwater and river systems. The significance is particularly apparent in mountainous environments where weathering fluxes can be large. However, our understanding of the relative contributions of rock-derived, or geogenic, N to the total N supply of mountainous watersheds remains poorly understood. In this study, we develop the High-Altitude Nitrogen Suite of Models (HAN-SoMo), a watershed-scale ensemble of process-based models to quantify the relative sources, transformations, and sinks of geogenic and atmospheric N through a mountain watershed. Our study is based in the East River Watershed (ERW) in the Upper Colorado River Basin. The East River is a near-pristine headwater watershed underlain primarily by an N-rich Mancos Shale bedrock, enabling the timing and magnitude of geogenic and atmospheric contributions to watershed scale dissolved N-exports to be quantified. Several calibration scenarios were developed to explore equifinality using >1600 N concentration measurements from streams, groundwater, and vadose zone samples collected over the course of four years across the watershed. When accounting for recycling of N through plant litter turnover, rock weathering accounts for approximately 12% of the annual dissolved N sources to the watershed in the most probable calibration scenario (0–31% in other scenarios), and 21% (0–44% in other scenarios) when considering only “new” N sources (i.e. geogenic and atmospheric). On an annual scale, instream dissolved N elimination, plant turnover (including cattle grazing) and atmospheric deposition are the most important controls on N cycling.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Integrated experimental studies of pore structure and fluid uptake in the Bossier Shale in eastern Texas, USA

Within the Haynesville-Bossier Shale complex, the Bossier Shale has not been extensively studied by either industry and academia, despite it being an unconventional gas reservoir and a potential caprock for carbon storage in the underlaying Haynesville Shale. The lack of knowledge of the complex pore structures and fluid-rock interactions hinders the effective extraction of gas and the characterization of fluid reservoirs and sealing capacity. Integrated experimental studies of pore structure and fluid-rock interactions were conducted in seven Bossier Shale core samples collected in eastern Texas. Petrographic, geochemical, and petrophysical properties such as mineral composition, organic richness, thermal maturity, porosity, pore/pore throat diameter distribution, water-accessible pores, liquid water imbibition, and water vapor adsorption were characterized using complementary approaches of thin-section petrography, scanning electron microscopy, X-ray diffraction, total organic matter, pyrolysis, mercury intrusion porosimetry, nuclear magnetic resonance, (Ultra-) small angle X-rays scattering as well as small angle neutron scattering with deuterated liquids and contrast variation. Further, the results show that the thermally mature Bossier Shales are composed of mixed argillaceous mudstone, mixed mudstone, and mixed carbonate mudstone. The shale contains both organic and inorganic pores, with porosities of 3.24-9.37 %, pore-to-throat ratios of 1.65 to 19.4, and water-accessible pores accounting for 28.7-72.6 % of total pores. Approaches of liquid water imbibition and water vapor adsorption, with and without direct contact of water with shale samples, indicate that liquid water first enters the nano-sized pores under high capillary pressures, and water vapor adsorption is mainly controlled by both clay minerals and pores with diameters less than 10 nm. These findings contribute to a better understanding of pore structures and water-shale interactions and their controlling factors in the Bossier Shale.

58 GEOSCIENCES↗

DOE OSTI2024

Bridging New Observational Capabilities and Process-Level Simulation: Insights into Aerosol Roles in the Earth System

The spatial distribution of ambient aerosol particles significantly impacts aerosol–radiation–cloud interactions, which contribute to the largest uncertainty in global anthropogenic radiative forcing estimations. However, the atmospheric boundary layer and lower free troposphere have not been adequately sampled in terms of spatiotemporal resolution, hindering a comprehensive characterization of various atmospheric processes and impeding our understanding of the Earth system. To address this research data gap, we have leveraged the development of uncrewed aerial systems (UAS) and advanced measurement techniques to obtain mesoscale spatial data on aerosol microphysical and optical properties around the U.S. Southern Great Plains (SGP) atmospheric observatory. Our study also benefits from state-of-the-art laboratory facilities that include three-dimensional molecular imaging techniques enabled by secondary ion mass spectrometry and nanogram-level chemical composition analysis via micronebulization aerosol mass spectrometry. Through our study, we have developed a framework for observation–modeling integration, enabling an examination of how various assumptions about the organic–inorganic components mixing state, inferred from chemical analysis, affect clouds and radiation in observation-constrained model simulations. By integrating observational constraints (derived from offline chemical analysis of the aerosol surface using collected samples) with in situ UAS observations, we have identified a prominent role of organic-enriched nanometer layers located at the surface of aerosol particles in determining profiles of aerosol optical and hygroscopic properties over the SGP observatory. Furthermore, we have improved the agreement between predicted clouds and ground-based cloud lidar measurements. This UAS–model–laboratory integration exemplifies how these new advanced capabilities can significantly enhance our understanding of aerosol–radiation–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water

Organic aerosol formation and transformation occurs within aqueous aerosol and cloud droplets, yet little is known about the composition of high molecular weight organic compounds in cloud water. Cloud water samples collected at Whiteface Mountain, New York, during August-September 2014 were analyzed by ultra-high-resolution mass spectrometry to investigate the molecular composition of dissolved organic carbon, with a focus on sulfur- and nitrogen-containing compounds. Organic molecular composition was evaluated in the context of cloud water inorganic ion concentrations, pH, and total organic carbon concentrations to gain insights into the sources and aqueous-phase processes of the observed high molecular weight organic compounds. Cloud water acidity was positively correlated with the average oxygen : carbon ratio of the organic constituents, suggesting the possibility for aqueous acid-catalyzed (prior to cloud droplet activation or during/after cloud droplet evaporation) and/or radical (within cloud droplets) oxidation processes. Many tracer compounds recently identified in laboratory studies of bulk aqueous-phase reactions were identified in the cloud water. Organosulfate compounds, with both biogenic and anthropogenic volatile organic compound precursors, were detected for cloud water samples influenced by air masses that had traveled over forested and populated areas. Oxidation products of long-chain (C 10-12 ) alkane precursors were detected during urban influence. Influence of Canadian wildfires resulted in increased numbers of identified sulfur-containing compounds and oligomeric species, including those formed through aqueous-phase reactions involving methylglyoxal. Light-absorbing aqueous-phase products of syringol and guaiacol oxidation were observed in the wildfire-influenced samples, and dinitroaromatic compounds were observed in all cloud water samples (wildfire, biogenic, and urban-influenced). Overall, the cloud water molecular composition depended on air mass source influence and reflected aqueous-phase reactions involving biogenic, urban, and biomass burning precursors.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Investigation and Recovery Following the Drum Event at INL's ARP-V Facility - 19517

Contractors working under the Department of Energy's (DoE's) Idaho Field Office have been exhuming and processing buried legacy waste from early weapons development and productions operations since 1984. Since operations began, nearly 400,000 drums have passed through this process. On April 11, 2018, repackaged drums were staged in an airlock (radiological buffer area) awaiting transfer to another facility for characterization. Late in the evening after operations had ended, four of the drums over pressurized causing an energetic displacement of their lids. A significant fraction of drum contents was ejected and dispersed throughout the airlock. The event activated the fire detection system in the facility initiating an emergency response from the site fire department, radiological protection, and operations. Initial intervention by fire department personnel was unsuccessful at quenching the reaction, so the responders egressed to a safe distance and monitored the situation. After determining the event had terminated and it was safe to enter, the facility was assessed revealing significant contamination in the airlock from the ejected waste. The area surrounding the facility was surveyed and it was determined that no contamination was released outside the facility. The Fluor Idaho, LLC (Fluor Idaho) Program Manager commissioned an investigation and recovery effort, which focused on three aspects: (1) technical investigation, (2) event and causal analysis, and (3) facility recovery. A team of highly qualified individuals from around the DOE Complex was assembled to support the technical investigation. The team included representatives from several Fluor Idaho, Fluor Corporate, Battelle Energy Alliance, LLC (INL), LANL, SRNL, South West Research Institute, DOE Carlsbad Field Office, and Defense Nuclear Facility Safety Board, and DOE-Headquarters. This team addressed the reaction mechanism of the event by guiding the sampling activities and coordinating analysis and testing by the analytical laboratories. Independent and experienced investigators were brought in to conduct a rigorous event and cause analysis. The Causal Analysis Team pursued direct, root, and contributing causes. Interviews were conducted, and documents were reviewed to develop an event and causal analysis. The Accelerated Retrieval Project V Operations team mobilized to decontaminate and recover the facility. Significant progress has been made in this effort, area and airborne contamination levels have been significantly reduced allowing limited activities to resume. In addition, this group supported sample collection efforts as directed by the Technical Investigation Team. This paper reviews key findings and milestones from the technical investigation, the event and causal analysis, and facility recovery operations. From these elements of the investigation, lessons learned are identified that would benefit other organizations involved with legacy waste management and disposition. Waste management is common to all sites in the DOE Complex and the events and recovery efforts described in this paper may provide beneficial insights to these operations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Investigation of Thermolytic Hydrogen Generation Rate in Tank 44 Dissolved Saltcake Samples

Saltcake core samples collected from Tank 44 in 2006 were dissolved to provide material for HGR measurements applicable to F-Area dissolved saltcake material. Additionally, characterization was performed on the Tank 44 saltcake material. The following are key results from the Tank 44 saltcake characterization. The Tank 44 Upper Saltcake Composite, corresponding to the 171 to 285 inch tank level, contained by mass approximately 69% sodium nitrate, 11% sodium carbonate, 8% sodium nitrite, smaller amounts of other salts and components, and 9% unquantified (which includes water, water of hydration, oxygen/hydrogen content of oxides and hydroxides, and uncertainty). The Tank 44 Lower Saltcake Composite, corresponding to the 76 to 114 inch tank level, contained by mass approximately 49% sodium carbonate, 18% sodium nitrate, smaller amounts of other salts, at least 8% sludge, and 9% unquantified (see above). The dissolved saltcake contained free hydroxide less than quantifiable (<0.01 M) due to the limited quantity of material that could be removed from the Shielded Cells based on the sample radioactivity. Measurement by pH paper provided an approximate pH of 12. The following are key results from the Tank 44 HGR testing. During boiling at 106.7 °C, HGR for Tank 44 dissolved saltcake without added glycolate was 7.2×10 -8 ft 3 h -1 ga l-1 . During boiling at 106.9 °C, HGR for Tank 44 dissolved saltcake with 1000 mg/L of added glycolate was 8.2×10 -8 ft 3 h -1 gal -1 . ∙ For the test without added glycolate, the first several HGR measurements at 70, 85, and 100 °C gave indication of the release of dissolved hydrogen and should not be used to represent the sustained thermolytic HGR for those temperatures. The measurements at boiling are the best representation of thermolysis in this testing. Carbon dioxide was observed at concentrations up to 6 vol% in the flow-system offgas for the test at boiling. ∙ Methane generation was observed at 100 °C and boiling. Methane concentration in the total gas generated during testing remained well below the lower flammability limit for methane in air. The addition of 1000 mg/L of glycolate did not have a significant impact on the hydrogen generation rates measured during this testing. The low hydroxide concentration in the Tank 44 dissolved saltcake likely influenced the relatively low thermolytic HGR and high carbon dioxide release observations in this testing. Based on the observation that methane was generated or released upon heating SRS radioactive Tank 44 waste samples to 100 °C and above, we recommend gaining a greater understanding of the cause and mechanism of its generation. First, the applicable literature should be reviewed to reveal the thermolytic methane generation mechanisms of possible methane generating species in the SRS CSTF. If warranted, a plan should be developed for simulant tests with methylated siloxanes and other applicable compounds in order to gain a better mechanistic understanding of methane generation in the SRS CSTF.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Y-12 Groundwater Protection Program Groundwater and Surface Water Sampling and Analysis Plan (CY 2021)

This plan provides a description of the groundwater and surface water quality monitoring activities planned for calendar year (CY) 2021 at the U.S. Department of Energy Y-12 National Security Complex (Y-12) that will be managed by the Y-12 Groundwater Protection Program (GWPP). Groundwater and surface water monitoring is performed by the GWPP. Groundwater and surface water monitoring will be performed in three hydrogeologic regimes at Y-12: the Bear Creek Hydrogeologic Regime (Bear Creek Regime), the Upper East Fork Poplar Creek Hydrogeologic Regime (East Fork Regime), and the Chestnut Ridge Hydrogeologic Regime (Chestnut Ridge Regime). The Bear Creek and East Fork regimes are located in Bear Creek Valley and the Chestnut Ridge Regime is located south of Y-12. Additional surface water monitoring will be performed north of Pine Ridge along the boundary of the Oak Ridge Reservation. The following sections of this report provide details regarding the CY 2021 groundwater and surface water monitoring activities. Section 2 describes the monitoring locations in each regime and the processes used to select the sampling locations. A description of the field measurements and laboratory analytes is provided in Section 3. Sample collection methods and procedures are described in Section 4, and Section 5 lists the documents cited for more detailed operational and technical information. The narrative sections of the report reference several appendices. Figures (maps and diagrams) and tables (excluding a data summary table presented in Section 4) are in Appendix A and Appendix B, respectively. Groundwater Monitoring Schedules (when issued throughout CY 2021) will be inserted in Appendix C, and addenda to this plan (if issued) will be inserted in Appendix D. Laboratory requirements (bottle lists, holding times, etc.) are provided in Appendix E, and an approved Waste Management Plan is provided in Appendix F. Modifications to the CY 2021 monitoring program may be necessary during implementation. Changes in programmatic requirements may alter the analytes specified for selected monitoring wells or may add or remove wells from the planned monitoring network. Each modification to the monitoring program will be approved by the Y-12 GWPP manager and documented as an addendum to this sampling and analysis plan.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Investigation of Thermolytic Hydrogen Generation Rate in Tank 44 Dissolved Saltcake Samples

Saltcake core samples collected from Tank 44 in 2006 were dissolved to provide material for HGR measurements applicable to F-Area dissolved saltcake material. Additionally, characterization was performed on the Tank 44 saltcake material. The following are key results from the Tank 44 saltcake characterization. The Tank 44 Upper Saltcake Composite, corresponding to the 171 to 285 inch tank level, contained by mass approximately 69% sodium nitrate, 11% sodium carbonate, 8% sodium nitrite, smaller amounts of other salts and components, and 9% unquantified (which includes water, water of hydration, oxygen/hydrogen content of oxides and hydroxides, and uncertainty). The Tank 44 Lower Saltcake Composite, corresponding to the 76 to 114 inch tank level, contained by mass approximately 49% sodium carbonate, 18% sodium nitrate, smaller amounts of other salts, at least 8% sludge, and 9% unquantified (see above). The dissolved saltcake contained free hydroxide less than quantifiable (<0.01 M) due to the limited quantity of material that could be removed from the Shielded Cells based on the sample radioactivity. Measurement by pH paper provided an approximate pH of 12. The following are key results from the Tank 44 HGR testing. During boiling at 106.7 °C, HGR for Tank 44 dissolved saltcake without added glycolate was 7.2×10 -8 ft 3 h -1 gal -1 . During boiling at 106.9 °C, HGR for Tank 44 dissolved saltcake with 1000 mg/L of added glycolate was 8.2×10 -8 ft 3 h -1 gal -1 . For the test without added glycolate, the first several HGR measurements at 70, 85, and 100 °C gave indication of the release of dissolved hydrogen and should not be used to represent the sustained thermolytic HGR for those temperatures. The measurements at boiling are the best representation of thermolysis in this testing. Carbon dioxide was observed at concentrations up to 6 vol% in the flow-system offgas for the test at boiling. Methane generation was observed at 100 °C and boiling. Methane concentration in the total gas generated during testing remained well below the lower flammability limit for methane in air. The addition of 1000 mg/L of glycolate did not have a significant impact on the hydrogen generation rates measured during this testing. The low hydroxide concentration in the Tank 44 dissolved saltcake likely influenced the relatively low thermolytic HGR and high carbon dioxide release observations in this testing. Based on the observation that methane was generated or released upon heating SRS radioactive Tank 44 waste samples to 100 °C and above, we recommend gaining a greater understanding of the cause and mechanism of its generation. First, the applicable literature should be reviewed to reveal the thermolytic methane generation mechanisms of possible methane generating species in the SRS CSTF. If warranted, a plan should be developed for simulant tests with methylated siloxanes and other applicable compounds in order to gain a better mechanistic understanding of methane generation in the SRS CSTF.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2004

Application of Colorimetric Solid Phase Extraction (C-SPE) to Monitoring Nickel(II) and Lead(II) in Spacecraft Water Supplies

Archived water samples collected on the International Space Station (ISS) and returned to Earth for analysis have, in a few instances, contained trace levels of heavy metals. Building on our previous advances using Colorimetric Solid Phase Extraction (C-SPE) as a biocide monitoring technique, we are devising methods for the low level monitoring of nickel(II), lead(II) and other heavy metals. C-SPE is a sorption-spectrophotometric platform based on the extraction of analytes onto a membrane impregnated with a colorimetric reagent that are then quantified on the surface of the membrane using a diffuse reflectance spectrophotometer. Along these lines, we have determined nickel(II) via complexation with dimethylglyoxime (DMG) and begun to examine the analysis of lead(II) by its reaction with 2,5- dimercapto-1,3,4-thiadiazole (DMTD) and 4-(2- pyridylazo)-resorcinol (PAR). These developments are also extending a new variant of C-SPE in which immobilized reagents are being incorporated into this methodology in order to optimize sample reaction conditions and to introduce the colorimetric reagent. This paper describes the status of our development of these two new methods.

Diaz, Neil C.↗

DOE OSTI2016

The Effect of Bicarbonate on Autunite Dissolution in the Presence of Shewanella oneidensis under Oxygen Restricted Conditions - 16429

Uranium is a key contaminant at many U.S. Department of Energy sites that served a leading role in the nation's defense for over 50 years. Uranium contamination of soil and groundwater is of great environmental concern due to the toxicological properties of the uranyl species. In an effort to decrease the concentration of soluble uranium, tripolyphosphate injections were identified as a feasible remediation strategy for sequestering uranium in situ in contaminated groundwater at the Hanford Site (WA). The introduction of sodium tripolyphosphate into uranium-bearing porous media results in the formation of uranyl phosphate minerals (autunite) of general formula (X{sub 1-2}[(UO{sub 2})(PO{sub 4})]{sub 2-1}.nH{sub 2}O), where X is a monovalent or divalent cation. The stability of the uranyl phosphate minerals in the subsurface is a critical factor since it determines the long-term effectiveness of the sodium tripolyphosphate injection as a remediation strategy. The behavior of uranium and its mobility in the subsurface are affected by various factors such as the chemistry of pore water, groundwater and soil minerals, the presence of complex-forming ligands, and micro-organisms that thrive under these conditions. Bicarbonate presence in the aqueous phase facilitates uranium desorption from soil and sediments and promotes the release of U(VI) into the aqueous phase, thus increasing uranium mobility in natural waters. In neutral or basic pH conditions, uranium can readily complex with a wide variety of ligands such as carbonate and form soluble uranyl-carbonato complexes such as UO{sub 2}(CO{sub 3}){sub 2}{sup 2-} and UO{sub 2}(CO{sub 3}){sub 3}{sup 4-}. Bicarbonate complexes have been identified in contaminated pore water at the Hanford Site. Furthermore, the presence of bacteria can significantly affect uranium mobility since bacteria may bio-enhance the release of U (VI) from uranyl-phosphate minerals, thus liberating uranium in the aqueous phase in an effort to obtain phosphorous, a vital nutrient for their metabolism. The Columbia River at the site exhibits large stage variations, causing fluctuations in the water table. These water table fluctuations and multiple rise-and-fall cycles in the river created an oxic-anoxic interface in this region. Previous assessments of Hanford sediment samples collected from this area noted a decline in cultivable aerobic bacteria and suggested the presence of facultative anaerobic bacteria. Shewanella oneidensis MR1 is a common bacterial group in soils and Shewanella species have been found in the Hanford soil. Shewanella oneidensis is a facultative anaerobic species which also belongs to a group known as dissimilatory metal-reducing bacteria (DMRB), due to their ability to reduce metals as a part of their metabolic pathway. Therefore, understanding the role of Shewanella is a critical factor affecting the outcome of environmental remediation. The objective of this research was to demonstrate the significance of bacteria-uranium interactions and investigate the effect of bicarbonate in the aqueous phase on Ca-autunite dissolution in the oxygen-restricted conditions. Sterile 100-mL glass mixed bioreactors with weighed amounts of ground Ca-autunite particles were used for initial experimentation. These autunite-containing bioreactors were injected with bacterial cells after the autunite equilibrated with the media solution amended with 0 mM, 3 mM 5 mM and 10 mM concentrations of bicarbonate. Additional abiotic samples were prepared without bacterial inoculation to provide a control for the biotic samples. The concentration of U(VI) determined in the aqueous phase was in direct correlation to the concentration of bicarbonate present in the solution. It was noted that an increase in bicarbonate concentration led to higher U(VI) concentration in the aqueous phase. A sharp decrease in U(VI) concentration was observed in the bicarbonate-free samples, probably due to a microbe mediated reduction of U(VI) to U(IV). In the case of samples amended with 3 mM bicarbonate, a slight, yet significant, decrease in U(VI) was also observed compared to the abiotic control. However, compared to the abiotic controls, there was no change in U(VI) levels in the aqueous phase as a result of bacterial inoculation for the samples amended with 5 and 10 mM bicarbonate for a period of time as long as 50 days. These results imply that the uranyl-carbonate complexes (UO{sub 2}(CO{sub 3}){sub 2}{sup 2-} and UO{sub 2}(CO{sub 3}){sub 3}{sup 4-}) that are present in carbonate-rich environments might be interfering with the microbial reduction in the oxygen- restricted conditions; however, this conclusion requires further investigation. Finally, the data indicate that release of U, P and Ca from autunite was non-stoichiometric. In conclusion, the high stability of uranyl-phosphate complexes makes them a strong candidate for the remediation efforts to sequester uranium in the subsurface. Nevertheless, in a bicarbonate-rich environment, Ca-autunite has a high probability of dissolution and the presence of metal-reducing bacteria does not seem to impede this process in the presence of higher bicarbonate concentrations under oxygen restricted conditions. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS2019

BioBot: Innovative Offloading of Astronauts for More Effective Exploration

The BioBot concept consists of a robotic rover which is capable of traversing the same terrain as a spacesuited human. It carries the primary life support system for the astronaut, including consumables, atmosphere revitalization systems (e.g., CO2 scrubbing, humidity and temperature management, ventilation fan), power system (e.g., battery, power management and distribution),and thermal control system (e.g., water sublimator, cooling water pump), along with umbilical lines to connect to the supported astronaut. Although not technically part of life support, it would be logical for the BioBot to also provide long-range communications, video monitoring, tool and sample transport, and other functions to enable and enhance EVA productivity in planetary surface exploration.The design reference scenario for this concept is that astronauts involved in future lunar or Mars exploration will be on the surface for weeks or months rather than days, and will be involved in regular EVA operations. It is not unreasonable to think of geologists spending several days inEVA exploration each week over a prolonged mission duration, with far more ambitious operational objectives than were typical of Apollo. In this scenario, each astronaut will be accompanied by a "BioBot", which will transport their life support system and consumables, an extended umbilical and umbilical reel, and robotic systems capable of controlling the position and motion of the umbilical. The astronaut will be connected to the robot via the umbilical, carrying only a small emergency open-loop life support system similar to those contained in every PLSS. The robotic mobility base will be designed to be capable of traveling anywhere the astronaut can walk, and will also be useful as a transport for the EVA tools, science instrumentation, and collected samples. In addition, the BioBot can potentially carry the astronaut on traverses as well. Such a system will also be a significant enhancement to public engagement in these future exploration missions, as the robotic vehicles can also support high-resolution cameras and high bandwidth communications gear to providehigh-definition video coverage of each crew throughout each EVA sortie.

Akin, David L.↗

NASA NTRS2006

MISSE PEACE Polymers Atomic Oxygen Erosion Results

Forty-one different polymer samples, collectively called the Polymer Erosion and Contamination Experiment (PEACE) Polymers, have been exposed to the low Earth orbit (LEO) environment on the exterior of the International Space Station (ISS) for nearly 4 years as part of Materials International Space Station Experiment 2 (MISSE 2). The objective of the PEACE Polymers experiment was to determine the atomic oxygen erosion yield of a wide variety of polymeric materials after long term exposure to the space environment. The polymers range from those commonly used for spacecraft applications, such as Teflon (DuPont) FEP, to more recently developed polymers, such as high temperature polyimide PMR (polymerization of monomer reactants). Additional polymers were included to explore erosion yield dependence upon chemical composition. The MISSE PEACE Polymers experiment was flown in MISSE Passive Experiment Carrier 2 (PEC 2), tray 1, on the exterior of the ISS Quest Airlock and was exposed to atomic oxygen along with solar and charged particle radiation. MISSE 2 was successfully retrieved during a space walk on July 30, 2005, during Discovery s STS-114 Return to Flight mission. Details on the specific polymers flown, flight sample fabrication, pre-flight and post-flight characterization techniques, and atomic oxygen fluence calculations are discussed along with a summary of the atomic oxygen erosion yield results. The MISSE 2 PEACE Polymers experiment is unique because it has the widest variety of polymers flown in LEO for a long duration and provides extremely valuable erosion yield data for spacecraft design purposes.

deGroh, Kim, K.↗