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DOE OSTI2012

Independent Confirmatory Survey Results of Soils Associated with the Argyle Street Sewer Line at the United Nuclear Corporation Naval Products Site, New Haven, Connecticut (Letter Report)

Oak Ridge Institute for Science and Education (ORISE) personnel visited the United Nuclear Corporation (UNC) Naval Products site on three separate occasions during the months of October and November 2011. The purpose of these visits was to conduct confirmatory surveys of soils associated with the Argyle Street sewer line that was being removed. Soil samples were collected from six different, judgmentally determined locations in the Argyle Street sewer trench. In addition to the six soil samples collected by ORISE, four replicate soil samples were collected by Cabrera Services, Inc. (CSI) for analysis by the ORISE laboratory. Replicate samples S0010 and S0011 were final status survey (FSS) bias samples; S0012 was an FSS systematic sample; and S0015 was a waste characterization sample. Six soil samples were also collected for background determination. Uranium-235 and uranium-238 concentrations were determined via gamma spectroscopy; the spectra were also reviewed for other identifiable photopeaks. Radionuclide concentrations for these soil samples are provided. In addition to the replicate samples and the samples collected by ORISE, CSI submitted three soil samples for inter-laboratory comparison analyses. One sample was from the background reference area, one was from waste characterization efforts (material inside the sewer line), and one was a FSS sample. The inter-laboratory comparison analyses results between ORISE and CSI were in agreement, except for one sample collected in the reference area. Smear results For Argyle Street sewer pipes are tabulated.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

The Nature and State of Groundwater Contamination at the Nevada National Security Site: What Have We Learned from Decades of Groundwater Analysis? - 20337

The regulatory framework for remediating radionuclide contamination from underground nuclear testing at the Nevada National Security Site (NNSS) is based on a combination of characterization and modeling studies, monitoring, and institutional controls [1]. Currently, tritium is the largest contributor (∼90%) to the estimated 44.6 million-curie radionuclide inventory resulting from underground testing [2]. Because of its short half-life (12.32 years), its relative contribution reduces below 10% of the total radiologic inventory over the next 120 years as a result of radioactive decay. Although tritium levels are observed well above the Safe Drinking Water Act (SDWA) maximum contaminant levels (MCLs) in groundwater, other radionuclides are well below their MCLs except within the nuclear test near-field (nuclear test cavity and chimney) environment. In fact, most device-derived radionuclides are below their MCL in groundwater even in samples collected from this near-field environment. The distribution of radionuclides following the nuclear detonation greatly influences the availability of potential contaminants for groundwater transport. Tritium is initially distributed in the gas phase, later as tritiated water in steam, and finally as liquid water, and is available to groundwater transport away from the near-field environment. Other radionuclides that are mobile in groundwater are {sup 14}C, {sup 36}Cl, {sup 99}Tc, and {sup 129}I though their radiologic inventory is small when compared to tritium. Many radionuclides (e.g. U, Pu, Am) are incorporated to a significant extent into the melt glass at the bottom of the cavity and are accessible to groundwater primarily through the slow process of glass dissolution. These radionuclides are also adsorbed to the surfaces of the crushed rock within the cavity and chimney which limits their migration in groundwater. Although colloid facilitated transport of radionuclides at the NNSS has been observed [3], radionuclide concentrations decrease with time and migration distances due to desorption and colloid filtration processes. Current studies indicate that radionuclides associated with colloids are unlikely to migrate downgradient from NNSS underground nuclear tests at concentrations above the SDWA MCL [4][5]. The results of over 50 years of sampling, along with an understanding of these post detonation processes, indicate that tritium is the only contaminant of concern downgradient of testing and that even tritium will not exceed its MCL in groundwater after ∼120 years. Although other longer-lived radionuclides may continue to be released slowly from the near-field environment they will likely never reach levels exceeding their MCLs in groundwater downgradient of the NNSS. Groundwater monitoring will continue to verify these observations. (authors)

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DOE OSTI2012

Influence of nutrients and currents on the genomic composition of microbes across an upwelling mosaic

Metagenomic data sets were generated from samples collected along a coastal to open ocean transect between Southern California Bight and California Current waters during a seasonal upwelling event, providing an opportunity to examine the impact of episodic pulses of cold nutrientrich water into surface ocean microbial communities. The data set consists of B5.8 million predicted proteins across seven sites, from three different size classes: 0.1–0.8, 0.8–3.0 and 3.0–200.0 lm. Taxonomic and metabolic analyses suggest that sequences from the 0.1–0.8 lm size class correlated with their position along the upwelling mosaic. However, taxonomic profiles of bacteria from the larger size classes (0.8–200 lm) were less constrained by habitat and characterized by an increase in Cyanobacteria, Bacteroidetes, Flavobacteria and double-stranded DNA viral sequences. Functional annotation of transmembrane proteins indicate that sites comprised of organisms with small genomes have an enrichment of transporters with substrate specificities for amino acids, iron and cadmium, whereas organisms with larger genomes have a higher percentage of transporters for ammonium and potassium. Eukaryotic-type glutamine synthetase (GS) II proteins were identified and taxonomically classified as viral, most closely related to the GSII in Mimivirus, suggesting that marine Mimivirus-like particles may have played a role in the transfer of GSII gene functions. Additionally, a Planctomycete bloom was sampled from one upwelling site providing a rare opportunity to assess the genomic composition of a marine Planctomycete population. The significant correlations observed between genomic properties, community structure and nutrient availability provide insights into habitat-driven dynamics among oligotrophic versus upwelled marine waters adjoining each other spatially.

marine↗

DOE OSTI2013

Shifting the Paradigm for Long Term Monitoring at Legacy Sites to Improve Performance while Reducing Cost

A major issue facing many government and private industry sites that were previously contaminated with radioactive and chemical wastes is that often the sites cannot be cleaned up enough to permit unrestricted human access. These sites will require long-term management, in some cases indefinitely, leaving site owners with the challenge of protecting human health and environmental quality in a cost effective manner. Long-term monitoring of groundwater contamination is one of the largest projected costs in the life cycle of environmental management at the Savannah River Site (SRS), the larger DOE complex, and many large federal and private sites. Currently, most monitoring strategies are focused on laboratory measurements of contaminants measured in groundwater samples collected from wells. This approach is expensive, and provides limited and lagging information about the effectiveness of cleanup activities and the behavior of the residual contamination. Over the last twenty years, DOE and other federal agencies have made significant investments in the development of various types of sensors and strategies that would allow for remote analysis of contaminants in groundwater, but these approaches do not promise significant reductions in risk or cost. Scientists at SRS have developed a new paradigm to simultaneously improve the performance of long term monitoring systems while lowering the overall cost of monitoring. This alternative approach incorporates traditional point measurements of contaminant concentration with measurements of controlling variables including boundary conditions, master variables, and traditional plume/contaminant variables. Boundary conditions are the overall driving forces that control plume movement and therefore provide leading indication to changes in plume stability. These variables include metrics associated with meteorology, hydrology, hydrogeology, and land use. Master variables are the key variables that control the chemistry of the groundwater system, and include redox variables (ORP, DO, chemicals), pH, specific conductivity, biological community (breakdown/decay products), and temperature. A robust suite of relatively inexpensive tools is commercially available to measure these variables. Traditional plume/contaminant variables are various measures of contaminant concentration including traditional analysis of chemicals in groundwater samples. An innovative long term monitoring strategy has been developed for acidic or caustic groundwater plumes contaminated with metals and/or radionuclides. Not only should the proposed strategy be more effective at early identification of potential risks, this strategy should be significantly more cost effective because measurement of controlling boundary conditions and master variables is relatively simple. These variables also directly reflect the evolution of the plume through time, so that the monitoring strategy can be modified as the plume 'ages'. This transformational long-term monitoring paradigm will generate significant cost savings to DOE, other federal agencies and industry and will provide improved performance and leading indicators of environmental management performance.

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DOE OSTI2013

Shifting the Paradigm for Long Term Monitoring at Legacy Sites to Improve Performance while Reducing Costs - 13422

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2011

RESULTS FOR THE SECOND QUARTER 2011 TANK 50 WAC SLURRY SAMPLE: CHEMICAL AND RADIONUCLIDE CONTAMINANT RESULTS

The Saltstone Facility is designed and permitted to immobilize and dispose of low-level radioactive and hazardous liquid waste (salt solution) remaining from the processing of radioactive material at the Savannah River Site. Low-level waste (LLW) streams from the Effluent Treatment Project (ETP), H-Canyon, the DDA (Deliquification, Dissolution, and Adjustment) process, and the decontaminated salt solution product from the Actinide Removal Process/Modular Caustic Side Solvent Extraction (CSSX) Unit (ARP/MCU) process are stored in Tank 50 until the LLW can be transferred to the Saltstone Facility for treatment and disposal. The LLW must meet the specified waste acceptance criteria (WAC) before it is processed into saltstone. The specific chemical and radionuclide contaminants and their respective WAC limits are listed in the current Saltstone WAC. Waste Solidification Engineering (WSE) requested that Savannah River National Laboratory (SRNL) perform quarterly analysis on saltstone samples. The concentrations of chemical and radionuclide contaminants are measured to ensure the saltstone produced during each quarter is in compliance with the current WAC. This report documents the concentrations of chemical and radionuclide contaminants for the 2011 Second Quarter samples collected from Tank 50 on April 4, 2011 and discusses those results in further detail than the previously issued results report. The following conclusions are drawn from the analytical results provided in this report: (1) The concentrations of the reported chemical and radioactive contaminants were less than their respective WAC targets or limits unless noted in this section. (2) The reported detection limit for {sup 59}Ni is above the requested limit from Reference 2 but below the established limit in Reference 3. (3) The reported detection limit for {sup 94}Nb is above the requested limit from Reference 2; however, it is below the established limits in Reference 3. (4) The reported concentration of {sup 242m}Am is above the target in Listed in Attachment 8.4 of the Saltstone WAC. (5) {sup 247}Cm and {sup 249}Cf are above the requested limits from Reference 2. However, they are below the limits established in Reference 3. (6) The reported detection limit for Norpar 13{sup 5} is greater than the limit from Table 4 and Attachment 8.2 of the WAC. (7) The reported detection limit for Isopar L is greater than the limit from Table 3 of the WAC. (8) Isopar L and Norpar 13 have limited solubility in aqueous solutions making it difficult to obtain consistent and reliable sub-samples. The values reported in this memo are the concentrations in the sub-sample as detected by the instrument; however, the results may not accurately represent the concentrations of the analytes in Tank 50.

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DOE OSTI2021

Nitrate, ammonium, and DON mass time series output for East River stream, vadose zone and groundwater subwatersheds from HAN-SoMo model

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. This dataset contains model output from 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. Six 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, from 2014-2018. The files in this dataset are named according to which calibration scenario they represent (1, 2, 3, NM1, NM2, and NC), and include daily time series model output of nitrate, ammonium and dissolved organic nitrogen concentrations for all six calibration scenarios described in Maavara et al., 2021, "Modeling geogenic and atmospheric nitrogen through the East River Watershed, Colorado Rocky Mountains," PLOS One (in press), for the stream, vadose zone, and groundwater in the five discretized subwatersheds: Rustlers Gulch, Copper Creek, East above Quigley (EAQ), the Middle East River (ME), and Lower Triangle (LT) from Gothic to the Pumphouse. The READ_ME.txt file includes details on units and naming conventions in each of these files. Model files are in .mat format, to be opened in MATLAB.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Virulence factors and antimicrobial resistance profiles of Campylobacter isolates recovered from consecutively reused broiler litter

ABSTRACT Campylobacterinfections are a leading cause of bacterial diarrhea in humans globally. Infections are due to consumption of contaminated food products and are highly associated with chicken meat, with chickens being an important reservoir forCampylobacter. Here, we characterized the genetic diversity ofCampylobacter jejuni(C. jejuni) andCampylobacter coli(C. coli) detected in broiler chicken litter over three consecutive flocks and determined their antimicrobial resistance (ARM) and virulence factor (VF) profiles.Campylobacterwas detected in 9.38% (27/288) of litter samples collected. Antimicrobial susceptibility testing and whole genome sequencing were performed onC. jejuni(n= 39) andC. coli(n= 5) isolates.Campylobactervirulence factors differed within and across broiler houses but were explained by the broiler flock cohort raised on litter,Campylobacterspecies andCampylobactermultilocus sequence type (MLST). Virulence factors involved in the ability to invade and colonize host tissues and evade host defenses were present inC. jejuniisolates (ST-464) from flock cohorts 1 and 2 but absent inC. jejuniisolates (ST-48) from flock cohort 3.C. jejuniisolates from house three harbored a significantly higher proportion of virulence genes with functions related to glycosylation and immune evasion thanC. jejuniisolates from houses 1 and 2 (P< 0.01). AllC. jejuniisolates were susceptible to all antibiotics tested whileC. coli(n= 4) were resistant to tetracycline and harbored the tetracycline resistant ribosomal protection protein (TetO). Our results suggest that house environment and broiler management practices imposed selective pressures on virulence factors and antimicrobial resistance genes ofCampylobacter. IMPORTANCE Campylobacteris a leading cause of foodborne illness in the United States due to consumption of contaminated or mishandled food products, often associated with chicken meat.Campylobacteris common in the microbiota of avian and mammalian gut; however, acquisition of antimicrobial resistance genes (ARGs) and virulence factors (VFs) may result in strains that pose significant threat to public health. Although there are studies investigating the genetic diversity ofCampylobacterstrains isolated from post-harvest chicken samples, there are limited data on the genome characteristics of isolates recovered from preharvest broiler production. Here, we show thatCampylobacter jejuniandCampylobacter colidiffer in their carriage of antimicrobial resistance and virulence factors may also differ in their ability to persist in litter during consecutive grow-out of broiler flocks. We found that presence/absence of virulence factors needed for evasion of host defense mechanisms and gut colonization played an integral role in differentiatingCampylobacterstrains.

Microbiology↗

DOE OSTI2014

Examination of lead concentrations in new decorative enamel paints in four countries with different histories of activity in lead paint regulation

Paints with high lead concentrations (ppm) continue to be sold around the world in many developing countries and those with economies in transition representing a major preventable environmental health hazard that is being increased as the economies expand and paint consumption is increasing. Prior lead paint testing had been performed in Brazil and India and these countries were selected to examine the impact of a new regulatory limit in Brazil and the impact of efforts of non-governmental organizations and others to stop the use of lead compounds in manufacturing paints. Armenia and Kazakhstan, in Central Asia, were selected because no information on lead concentration in those regions was available, no regulatory activities were evident and non-governmental organizations in the IPEN network were available to participate. Another objective of this research was to evaluate the lead loading (µg/cm{sup 2}) limit determined by X-Ray Fluorescence (XRF) for areas on toys that are too small to obtain a sample of sufficient size for laboratory analysis. The lead concentrations in more than three-fourths of the paints from Armenia and Kazakhstan exceeded 90 ppm, the limit in the United States, and 600 ppm, the limit in Brazil. The percentages were about one-half as high in Brazil and India. The average concentration in paints purchased in Armenia, 25,000 ppm, is among the highest that has been previously reported, that in Kazakhstan, 15,700 ppm, and India, 16,600, about median. The average concentration in Brazil, 5600 ppm, is among the lowest observed. Paints in Brazil that contained an average of 36,000 ppm before the regulatory limit became effective were below detection (<9 ppm) in samples collected in the current study. The lack of any apparent public monitoring of paint lead content as part of regulatory enforcement makes it difficult to determine whether the regulation was a major factor contributing to the decline in lead use in these paints. Using data from the current study and those available from other studies 24 of 28 paints from major brands in India decreased from high concentrations to 90 ppm or lower. Since lead concentrations in golden yellow paints from these brands were found to decrease to ≤90 ppm, it is possible that all 28 of these paints now contain ≤90 ppm since yellow paints usually have the highest lead concentrations. Other brands in Brazil and India that have been analyzed only one time had lead concentrations up to 59,000 ppm and 134,000 ppm, respectively. Less than one-third of the paints had notations on their labels with information about lead content and these were sometimes inaccurate. The label from one brand indicating “no added lead” contained paint with 134,000 ppm lead, the highest found in this study. Three percent (3 of 98) of the paints with surface lead loading that did not exceed 2 µg/cm{sup 2}, the limit established by the Consumer Product Safety Improvement Act for small areas on toys, contained greater than 90 ppm lead and thus were false negatives. Of the new paint samples that contained ≤600 ppm, 88% contained ≤90 ppm. Of the samples that contained ≤90 ppm, 97% contained ≤45 ppm and 92% contained ≤15 ppm. Based on these data it appears to be technically feasible to manufacture paints containing ≤90 ppm and in many cases to produce paints that have lead concentrations that do not exceed 15 ppm. - Highlights: • Brazilian paints with high lead (avg. 36,000 ppm) contained <9 ppm after regulation. • Lead in major Indian paint brands decreased to low levels by efforts of NGOs/others. • Most paints with lead ≤600 ppm also are ≤90 ppm and many also ≤15 ppm. • At the CPSIA limit of 2 µg Pb/cm{sup 2} for small areas on toys, 3% exceeded 90 ppm lead. • Most paint brands in Armenia and Kazakhstan based/manufactured outside the country.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

National Virtual Biotechnology Laboratory: Report on Rapid R&D Solutions to the COVID-19 Crisis

With funding from the CARES Act, the U.S Department of Energy (DOE) established the National Virtual Biotechnology Laboratory (NVBL) in March 2020 to address key challenges associated with the COVID-19 crisis. NVBL brought together the broad scientific and technical expertise and resources of DOE’s 17 national laboratories to help tackle medical supply short ages, discover potential drugs to fight the virus, develop and validate COVID-19 testing methods, model disease spread and impact across the nation, and understand virus transport in buildings and the environment. National laboratory resources leveraged for this effort include a suite of world-leading user facilities broadly available to the research community, such as light and neutron sources, nanoscale science research centers, sequencing and biocharacterization facilities, and high-performance computing facilities. Within months, NVBL teams produced innovations in materials and advanced manufacturing that mitigated shortages in test kits and personal protective equipment (PPE), creating nearly 1,000 new jobs. They used DOE’s high-performance computers and light and neutron sources to identify promising candidates for antibodies and antivirals that universities and drug companies are now evaluating. NVBL researchers also developed new diagnostic targets and sample collection approaches, and supported U.S. Food and Drug Administration (FDA), Centers for Disease Control and Prevention (CDC), and U.S. Department of Defense (DoD) efforts to establish national guidelines used in administering millions of tests. Researchers used artificial intelligence and high-performance computing to produce near-real-time data analysis to forecast disease transmission, stress on public health infrastructure, and economic impact, which supported decision-makers at the local, state, and national levels. NVBL teams also studied how to control indoor virus movement to minimize uptake and protect human health. NVBL’s accomplishments demonstrate not only the powerful resource represented by DOE’s national laboratories working together to meet national needs, but also the effectiveness of the integrated NVBL framework for rapidly responding to emergencies with research and development (R&D) solutions. As the fight against COVID continues, sustained efforts are needed to confront this pandemic as well as future threats. Examples include: 1) Establishing “supply chains on demand” to meet emergency production needs by leveraging the materials and manufacturing expertise of DOE national laboratories and developing advances in electronics, sensing, robotics, and automation capabilities; 2) Improving the speed and robustness of drug discovery by integrating experimental platforms with DOE’s computational and experimental user facilities, which provide unique resources to support the discovery of high-potential therapeutic agents; 3) Protecting public, environmental, and animal health by developing new testing protocols and instrumentation adaptable to diverse sample types (both physiological and environmental) to quickly detect a wide range of pathogens and monitor other biorisks; 4) Supporting near-real-time data needs of decision-makers at the local, regional, state, and national levels by advancing data curation, analysis, and modeling using artificial intelligence and new data science tools for managing and evaluating large diverse datasets; 5) Harnessing DOE’s expertise in environmental modeling to design rooms and air handling for offices, classrooms, restaurants, and other structures to minimize biorisk transmissions. Going forward, NVBL is poised to apply the unique capabilities and expertise of the national laboratory complex to future national and international emergencies, both natural and engineered. Through this framework, the Office of Science will continue to be an integral component of agency wide efforts to prepare for and respond to biorisks and other crises.

42 ENGINEERING↗

DOE OSTI2013

Grout long radius flow testing to support Saltstone disposal Unit 5 design

The Saltstone Facility, located within the Savannah River Site (SRS) near Aiken, South Carolina, consists of two facility segments: The Saltstone Production Facility (SPF) and the Saltstone Disposal Facility (SDF). The SPF receives decontaminated legacy low level sodium salt waste solution that is a byproduct of prior nuclear material processing. The salt solution is mixed with cementitious materials to form a grout slurry known as “Saltstone”. The grout is pumped to the SDF where it is placed in a Saltstone Disposal Unit (SDU) to solidify. SDU 6 is referred to as a “mega vault” and is currently in the design stage. The conceptual design for SDU 6 is a single cell, cylindrical geometry approximately 114.3 meters in diameter by 13.1 meter high and is larger than previous cylindrical SDU designs, 45.7 meters in diameter by 7.01 meters high (30 million gallons versus 2.9 million gallons of capacity). Saltstone slurry will be pumped into the new waste disposal unit through roof openings at a projected flow rate of about 34.1 cubic meters per hour. Nine roof openings are included in the design to discharge material into the SDU with an estimated grout pour radius of 22.9 to 24.4 meters and initial drop height of 13.1 meters. The conceptual design for the new SDU does not include partitions to limit the pour radius of the grout slurry during placement other than introducing material from different pour points. This paper addresses two technical issues associated with the larger diameter of SDU 6; saltstone flow distance in a tank 114.3 meters in diameter and quality of the grout. A long-radius flow test scaled to match the velocity of an advancing grout front was designed to address these technology gaps. The emphasis of the test was to quantify the flow distance and to collect samples to evaluate cured properties including compressive strength, porosity, density, and saturated hydraulic conductivity. Two clean cap surrogate mixes (saltstone premix plus water) were designed to simulate slurry with the reference saltstone rheology and a saltstone with extra water from the process flushing operation. Long-radius flow tests were run using approximately 4.6 cubic meters of each of these mixes. In both tests the pump rate was 0.063 liters/second (1 gpm). A higher pump rate, 0.19 liters/second (3 gpm), was used in a third long-radius flow test. The angle of repose of the grout wedges increased as a function of time in all three tests. The final angles of repose were measured at 3.0º, 2.4º, and 0.72º. The pump rate had the largest effect on the radial flow distance and slope of the grout surface. The slope on the pour placed at 0.19 liters/second (3 gpm) was most representative of the slope on the grout currently being pumped into SDU 2 which is estimated to be 0.7º to 0.9º. The final grout heights at 1/3 of a meter from the discharge point were 115, 105, and 38 cm. Entrapped air (≥ 0.25 cm bubbles) was also observed in all of the mixes. The entrapped air appeared to be released from the flows within about 3.1 meters (10 feet) of the discharge point. The bleed water was clear but had a thin layer of floating particulates. The bleed water should be retrievable by a drain water collection system in SDU 6 assuming the system does not get clogged. Layering was observed and was attributed to intervals when the hopper was being cleaned. Heat from the hydration reactions was noticeable to the touch.

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DOE OSTI2013

Grout Long Radius Flow Testing to Support Saltstone Disposal Unit 6 Design - 13352

The Saltstone Facility, located within the Savannah River Site (SRS) near Aiken, South Carolina, consists of two facility segments: The Saltstone Production Facility (SPF) and the Saltstone Disposal Facility (SDF). The SPF receives decontaminated legacy low level sodium salt waste solution that is a byproduct of prior nuclear material processing. The salt solution is mixed with cementitious materials to form a grout slurry known as 'Saltstone'. The grout is pumped to the SDF where it is placed in a Saltstone Disposal Unit (SDU) to solidify. SDU 6 is referred to as a 'mega vault' and is currently in the design stage. The conceptual design for SDU 6 is a single cell, cylindrical geometry approximately 114.3 meters in diameter by 13.1 meter high and is larger than previous cylindrical SDU designs, 45.7 meters in diameter by 7.01 meters high (30 million gallons versus 2.9 million gallons of capacity). Saltstone slurry will be pumped into the new waste disposal unit through roof openings at a projected flow rate of about 34.1 cubic meters per hour. Nine roof openings are included in the design to discharge material into the SDU with an estimated grout pour radius of 22.9 to 24.4 meters and initial drop height of 13.1 meters. The conceptual design for the new SDU does not include partitions to limit the pour radius of the grout slurry during placement other than introducing material from different pour points. This paper addresses two technical issues associated with the larger diameter of SDU 6; Saltstone flow distance in a tank 114.3 meters in diameter and quality of the grout. A long-radius flow test scaled to match the velocity of an advancing grout front was designed to address these technology gaps. The emphasis of the test was to quantify the flow distance and to collect samples to evaluate cured properties including compressive strength, porosity, density, and saturated hydraulic conductivity. Two clean cap surrogate mixes (Saltstone premix plus water) were designed to simulate slurry with the reference Saltstone rheology and a Saltstone with extra water from the process flushing operation. Long-radius flow tests were run using approximately 4.6 cubic meters of each of these mixes. In both tests the pump rate was 0.063 liters/second (1 gpm). A higher pump rate, 0.19 liters/second (3 gpm), was used in a third long-radius flow test. The angle of repose of the grout wedges increased as a function of time in all three tests. The final angles of repose were measured at 3.0 deg., 2.4 deg., and 0.72 deg.. The pump rate had the largest effect on the radial flow distance and slope of the grout surface. The slope on the pour placed at 0.19 liters/second (3 gpm) was most representative of the slope on the grout currently being pumped into SDU 2 which is estimated to be 0.7 deg. to 0.9 deg. The final grout heights at 1/3 of a meter from the discharge point were 115, 105, and 38 cm. Entrapped air (≥ 0.25 cm bubbles) was also observed in all of the mixes. The entrapped air appeared to be released from the flows within about 3.1 meters (10 feet) of the discharge point. The bleed water was clear but had a thin layer of floating particulates. The bleed water should be retrievable by a drain water collection system in SDU 6 assuming the system does not get clogged. Layering was observed and was attributed to intervals when the hopper was being cleaned. Heat from the hydration reactions was noticeable to the touch. (authors)

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DOE OSTI2023

Schneider Springs Fire Study 2023 for Ecosystem Respiration Rates: Surface Water Chemistry and Hydrologic Sensor Data across the Yakima River Basin, Washington, USA (v2)

This dataset supports a broader study examining the drivers of spatial variability in wildfire impacts across the Yakima River Basin. Data provided within this dataset were generated from sample collection across 17 total sites (8 sites affected by a recent wildfire, 9 sites unaffected by a recent wildfire) within multiple rivers throughout the Yakima River Basin in Washington, USA from May-July 2023. Fire affected sites are defined as those affected by the 2021 Schneider Springs Fire, based on the drainage area of the streams being within the 2021 Schneider Springs Fire burn perimeter or not (Figure 1, below). The contents include surface water geochemistry data (dissolved organic carbon; total dissolved nitrogen; total suspended solids); short-term sonde data (specific conductivity; turbidity; pH; chlorophyll A; temperature); stream depth data; stream velocity; manual chamber open channel respiration data; sensor time-series data (oxygen; water pressure; barometric pressure); field metadata (including qualitative information on in stream and river corridor characteristics); and environmental context photos taken in the field. The dataset also includes a summary file of the sensor data and plots of the sensor data. Sensors were only recovered at 15 out of the 17 sites, and not all sensors were recovered at all 15 sites (see Methods section for more details), therefore all data does not exist at all sites. Data from a 2022 study at the same sites, as well as additional sites, can be found at https://data.ess-dive.lbl.gov/view/doi:10.15485/1969566. The data package was originally published in November 2023. It was updated in June 2025 (v2; modified files). See the change history section in the readme for more details. For details on how to navigate data packages generated by this project, see https://data.ess-dive.lbl.gov/portals/PNNLRiverCorridorSFA/About. This dataset is comprised of one folder with field photos and one main data folder with two subfolders. The main data folder consists of (1) file-level metadata; (2) data dictionary; (3) field metadata; (4) field protocol; (5) readme; (6) international generic sample number (IGSN) mapping file; and (7) stream depth and averages. The sensor data subfolder consists of (1) sensor installation methods summary; (2) stream velocity; and (3) six subfolders. The BarotrollAtm (barometric pressure; temperature), DepthHOBO (water pressure; temperature), MantaRiver (specific conductivity; turbidity; pH; chlorophyll A; temperature), EXO (specific conductivity; pH; temperature), miniDOT (dissolved oxygen; temperature), and miniDOTManualChamber (dissolved oxygen; temperature) contain time-series data, plots, and summary files. The sample data subfolder consists of (1) total suspended solids (TSS) data; (2) dissolved organic carbon (DOC, measured as non-purgeable organic carbon, NPOC) data and averages; (3) total dissolved nitrogen (TN) data and averages; and (4) methods codes. All files are .csv, .pdf, .jpg, .jpeg, or .mov.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Success Using A Granular-Activated Carbon Filtration Swab to Rehabilitate Westbay{sup R} Multi-level Groundwater Monitoring Wells at the INL - 20544

In November 2015, tetrachloroethylene (PCE) was discovered in groundwater samples collected from a Westbay{sup R} multi-level groundwater monitoring well at the Idaho National Laboratory (INL).a Subsequent investigation determined that PCE was not present in the groundwater. The detected PCE was instead due to inadvertent contamination of the internal tubing fluid in the Westbay well-monitoring system, which is isolated from the surrounding groundwater. Further investigation showed that three of the 11 Westbay wells at the INL contained PCE-contaminated tubing fluid at concentrations above the U.S. Environmental Protection Agency's maximum contaminant level for drinking water (5 μg/L). Loose sediment at the bottom of some Westbay wells was also found to contain PCE; the three wells were then identified for rehabilitation as part of the INL well maintenance program. The unique construction of the Westbay wells - i.e., the small diameter (5.72 cm [2.25 in.]) and the depths of the tubing fluid ranging from 144.8 to 419 m (475 to 1,376 ft) below ground surface - posed unique challenges to the rehabilitation. Because the tubing fluid provides structural integrity, the fluid cannot be removed and then replaced without damaging the integrity of the Westbay well. Additionally, the small diameter of the systems and the associated depths limit the availability of equipment that can be used for the rehabilitation. After an evaluation of potential methods, it was determined that the use of an in-well, custom-fabricated, granular-activated-carbon filtration swab deployed via a wire line would provide the safest and most cost-effective method for rehabilitation. Westbay well rehabilitation started at well MIDDLE-2051 in late June 2018 and paused in December 2018 for the season. The PCE concentration in the tubing fluid at MIDDLE-2051 was initially reduced to a maximum concentration of 3.81 μg/L from a maximum of 642 μg/L, while the concentration of PCE in the sediment had been reduced from 5,360 to 2,270 μg/kg. Sampling was performed at MIDDLE-2051 again in August 2019, and the tubing fluid increased to a maximum concentration of 45.4 μg/L, while the concentration in the sediment decreased further to 1,890 μg/kg due to desorption of PCE from the sediment to the tubing fluid. Rehabilitation resumed at well MIDDLE-2050A in late August 2019, and the PCE concentration in the tubing fluid had been reduced to a maximum concentration of 19.0 μg/L. Although the method has been shown to be time-consuming, it has proven to be effective and safe for personnel performing the work and to the integrity of the well. Future sample data results at all wells will help determine an estimated completion of the rehabilitation. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Use of an Alternative Conceptual Model of Vadose Zone Heterogeneity to Evaluate Past Tank Leaks and Other Unplanned Releases within a Tank Farm at the Hanford Site - 20061

Washington State Department of Ecology (Ecology) requested that U.S. Department of Energy (DOE)-Office of River Protection (ORP) consider an evaluation of effects of fine-grained thin sediment layers on transport with a separate alternative conceptual model in its evaluation of the potential impact of tank leaks and other unplanned releases within the tank farm at the Hanford Site. For this alternative model, Ecology recommended that the model be developed based on the general framework of fine-grained units identified by a stakeholder group in their interpretations of variability in moisture content data collected in the vicinity of Waste Management Area (WMA) C. In discussions with DOE-ORP, Ecology acknowledged that the underlying data and interpretations of the occurrence and lateral continuity of the fine-grained thin layers identified by a stakeholder group are uncertain. However, DOE-ORP agreed to Ecology's recommendation and has provided support for the requested evaluation that involved development of an alternative model based on the general framework of the unpublished report by the stakeholder. DOE-ORP considered this evaluation to be a hypothetical evaluation of vadose zone heterogeneities at WMA C. General observations from the range of simulation cases examined in the evaluation of the effects of hypothetical vadose zone heterogeneities at WMA C are as follows. - The movement of the center of mass of the simulated plumes was generally vertically downward below the source for all simulations, including those that incorporated the hypothetical fine-grained units. - All simulations that incorporated hypothetical heterogeneity produced additional plume spreading over what was produced in simulations using Equivalent Homogeneous Media (EHM) model(s)a. The spreading resulted in a broadening of the fringes of the plume, resulting in a wider region of low concentration, but lower peak concentrations associated with the center of mass of the plume. - Simulations that used the silty-sand hydraulic properties, suggested by Ecology for the hypothetical fine-grained units, generally produced similar spreading and slightly lower peak mass flux at the water table when compared to the EHM modeling results. a The EHM-based models used at WMA C do not explicitly include small-scale fine-grained heterogeneities used in the model advocated by Ecology. - Simulations that used the silty-sand hydraulic properties, suggested by Ecology for the hypothetical fine-grained units, generally produced less spreading and an earlier arrival of mass flux at the water table when compared to the use of another set of hydraulic properties from a silty-sand sample collected at a nearby disposal facility. - The EHM representation of the vadose zone generally produced higher peak mass flux and an earlier occurrence of peak fluxes at the water table compared to all analyses incorporating additional hypothetical heterogeneity. Results of this alternative model evaluation of past leaks provided some insight into the transport effects of vadose zone heterogeneities at WMA C that helped resolve Ecology's comments and issues related to the effects of vadose zone heterogeneities on past leaks and losses from the WMA C tank farms area. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Subtask 1.1 – Advanced Characterization of Unconventional Oil and Gas Reservoirs to Enhance CO2 Storage Resource Estimates

The Energy & Environmental Research Center (EERC) developed methods and approaches for advanced characterization of unconventional oil and gas reservoirs to enhance CO2 storage resource estimates using samples collected from organic-rich shales of the Bakken Formation. The project was funded under U.S. Department of Energy (DOE) Cooperative Agreement No. DE-FE0024233, with nonfederal cost share provided by Hitachi High Technologies America. The project participants included the EERC, Hitachi High Technologies America, the team at the National Energy Technology Laboratory’s (NETL’s) computed tomography (CT) scanning laboratory in Morgantown, West Virginia, and several NETL staff who have worked on CO2 storage resource estimation. Investigations on the use of subsurface geologic formations for CO2 storage have been ongoing for many years. In the last decade, improvements in directional drilling technology and hydraulic fracturing of organic-rich shale and other tight rock formations have opened new opportunities for CO2 storage, with the potential cobenefit of enhancing gas and oil recovery. Gas-bearing, organic-rich shales have been of particular interest as a carbon storage target because their ability to store large volumes of CO2 is implied by their ability to store methane; however, estimating the CO2 storage resource of organic-rich shales and other unconventional reservoirs is challenging because of the lack of detailed geologic and petrophysical data that are needed to develop improved volumetric equations. According to NETL’s method for estimating regional-scale CO2 storage resources, the key factors that control CO2 storage in geologic formations include void space within induced fractures, natural fractures and matrix pores, as well as the occurrence and distribution of organic matter (OM) and clay minerals. A key goal of this effort was to use field emission scanning electron microscopy (FESEM) analysis of fine-grain unconventional reservoir rocks coupled with advanced image analysis and machine learning techniques to quantify the occurrence and distribution of porosity, OM, and clay minerals. By better understanding the potential migration pathways of CO2 within tight rocks and quantifying the occurrence of sorptive components (OM and clays) along potential flow pathways, methods to estimate the CO2 storage resource of such rocks can be refined. The Bakken petroleum system (Bakken) was used as the source of rock samples for this effort because it includes organic-rich shales with contrasting degrees of thermal maturity as well as tight, nonshale clastic rocks with varying clay mineral content. To better understand the key components of interest in tight rock samples, the EERC worked closely with Hitachi to optimize the FESEM settings necessary to resolve the sample mineralogy, porosity and OM content at micro- to nanoscale resolution. The EERC also worked closely with Hitachi to apply and improve its advanced mineral identification and characterization system (AMICS) software so that it is better suited for mineral identification at the high resolution necessary to resolve features of interest in fine-grained rocks such as organic-rich shales. The EERC also applied advanced image analysis software packages, including Ilastik, to classify and quantify the key components of interest within the samples using FESEM imagery. These advanced techniques allowed for quantification and differentiation of the void space within fractures, pores and OM, as well as a technique to determine and quantify the key mineral and OM components surrounding pore spaces. Being able to better quantify the void space and the potential accessibility of CO2 to sorptive minerals or OM within tight rocks allows for improved estimation of the CO2 storage resource potential of organic-rich shales and other unconventional formations. The information derived from the image analysis techniques was used to refine NETL’s method for estimating regional-scale CO2 storage resources in collaboration with staff from NETL. An additional goal of this work was to better understand rates of CO2 permeation, flow pathways, and sorption in organic-rich shales and nonshale reservoir rocks and to evaluate potential changes in CO2 flow over time. The EERC conducted long-duration (several weeks) CO2 flow-through testing at reservoir conditions using Bakken shale and nonshale samples to assess CO2 permeation rates and retention/sorption within core plugs to represent bulk matrix behavior. Conventional isothermal adsorption testing over a range of pressure conditions was also performed on pulverized Bakken samples to better assess potential maximum sorptive capacity of the samples. The results of this testing illustrated the higher sorptive capacity of the Bakken shales when compared to the sorptive capacity of the nonshale reservoir rock, which contains very little OM when compared to the Bakken shales. The results also illustrate the differences in permeation behavior as a function of fracture flow versus matrix flow. In an attempt to visualize CO2 permeation and flow behavior in Bakken shale samples over time, the EERC collaborated with NETL’s CT Lab in Morgantown, West Virginia. A variety of tests were performed at the NETL lab on unfractured and fractured samples of the Bakken shale. The unfractured Bakken shale samples did not result in CO2 migration within the samples over the testing duration; thus imagery of CO2 migration pathways within the matrix of Bakken samples was not obtained. The results of the flow-through testing within fractured samples illustrate changes in CO2 permeation rates over time, with a trend of decreasing CO2 flow over time. The results of this effort suggest that FESEM analysis coupled with advanced image analysis and machine learning techniques are effective in characterizing and quantifying the mineralogy, porosity, fractures, and OM content of 2-D imagery at the high resolution needed to identify features of interest in tight rocks. In addition, the image analysis techniques allow for identification and quantification of different porosity types as well as the key mineral components and/or OM that CO2 would contact in the reservoir as it migrates through pores and fracture networks. This is key information needed to better estimate the CO2 storage resource potential of organic-rich shales and other tight reservoirs. Additional work is needed to determine the sorptive capacity of the individual sample components (OM and clay minerals) at reservoir conditions so that this approach and the refined CO2 storage resource equation can be applied to other shale and unconventional reservoirs. In addition, subsequent work should be performed to better understand the number of images needed to use stereological approaches to estimate the volume of sample components using 2-D imagery, to explore machine learning techniques to differentiate between induced vs. natural fractures, and to estimate the connectivity of pores and fracture networks using 2-D imagery. Being able to derive this information at the microscale would facilitate scaling up of the sample characterization data used for reservoir modeling and simulation to estimate the CO2 storage resource potential of tight formations.

03 NATURAL GAS↗

DOE OSTI2014

Colloid Rates of Radionuclides in Cooling Water of the 120-GeV Proton Accelerator Facilities at Fermilab - Paper 58

Cooling water systems for high-energy accelerators are typically equipped with a deionizer to keep water pure for accelerator materials and to remove radionuclides for radioactivity control. Although the deionizers are expected to collect the entire radionuclides, more radioactivity than expected remains in the cooling water in typical cooling water operations at J-PARC and the Tsukuba Campus of High Energy Accelerator Research Organization (KEK), Japan. For example, specific activity of {sup 7}Be in the cooling water for magnetic horns at the J-PARC Neutrino Experimental Facility was observed to be comparable to the limit of {sup 7}Be activity for drain (30 Bq/mL) after enough deionization duration. Removing this activity from the cooling water is an important problem that must be solved before the water can be released into the environment. In our previous study, it was found that some radionuclides had weak retention on ion-exchange resins in the cooling water deionizer system for the K2K target and magnetic horns at the 12-GeV proton accelerator in KEK, Japan. Incomplete adsorption in the deionizer was attributed to colloid formation. Therefore, understanding the colloid formation of radionuclides in cooling water is important for understanding the activity remaining in the cooling water. Colloid formation in water under high-intensity radiation fields has been investigated by previous irradiation experiments. Under 120-GeV proton irradiation of Cu foils in water, it was found that the colloid formation rates of Mg, Mn, Co, Ni, and Cu isotopes and those of {sup 7}Be, {sup 24}Na, {sup 42}K, and {sup 43}K were approximately 30% and 1.8-3.9%, respectively. Sc, Cr, and Fe isotopes were missing from the water. In the photon irradiation of water in a Cu tube using Bremsstrahlung from an electron linear accelerator and a {sup 60}Co γ-ray source at Kyoto University Research Reactor Institute, we observed Cu colloid formation in consequence of the corrosion of Cu. It is possible that radionuclides attach to the colloids formed by the corrosion of accelerator materials and pass through the deionizer. To enhance the understanding of the behavior of radionuclides in cooling water in a high-energy accelerator environment, we investigated the colloid formation of radionuclides in cooling waters at the 120-GeV proton accelerator facilities at Fermilab, USA. We have already reported the previous results of specific activities of γemitting radionuclides and {sup 3}H in water samples collected from eight cooling water systems. Following the previous study, this paper is concerned with the measurement of colloid formation rates of radionuclides in cooling waters. (authors)

43 PARTICLE ACCELERATORS↗

DOE OSTI2015

Technologies for pre-screening IAEA swipe samples

During the course of International Atomic Energy Agency (IAEA) inspections, many samples are taken for the purpose of verifying the declared facility activities and identifying any possible undeclared activities. One of these sampling techniques is the environmental swipe sample. Due to the large number of samples collected, and the amount of time that is required to analyze them, prioritizing these swipes in the field or upon receipt at the Network of Analytical Laboratories (NWAL) will allow sensitive or mission-critical analyses to be performed sooner. As a result of this study, technologies were placed into one of three categories: recommended, promising, or not recommended. Both neutron activation analysis (NAA) and X-ray fluorescence (XRF) are recommended for further study and possible field deployment. These techniques performed the best in initial trials for pre-screening and prioritizing IAEA swipes. We learned that for NAA more characterization of cold elements (such as calcium and magnesium) would need to be emphasized, and for XRF it may be appropriate to move towards a benchtop XRF versus a handheld XRF due to the increased range of elements available on benchtop equipment. Promising techniques that will require additional research and development include confocal Raman microscopy, fluorescence microscopy, and infrared (IR) microscopy. These techniques showed substantive responses to uranium compounds, but expensive instrumentation upgrades (confocal Raman) or university engagement (fluorescence microscopy) may be necessary to investigate the utility of the techniques completely. Point-and-shoot (handheld) Raman and attenuated total reflectance–infrared (ATR-IR) measurements are not recommended, as they have not shown enough promise to continue investigations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗