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DOE OSTI2025

Colloidal Behavior of Plutonium Oxide in Concentrated Electrolyte Solutions

The Hanford Site in Washington State manages legacy high-level radioactive waste streams that display major chemistry and engineering challenges, including the high salt levels and pH values that correspond to conditions under which many classical concepts describing chemical reactivity cannot be applied. One particular challenge that needs to be tackled at Hanford is that Pu concentrations, [Pu], in the soluble phases of the tank wastes are higher than expected based on the solubility of crystalline PuO2, which is widely accepted to be caused by the formation of PuO2 colloid, consisting of nano- to submicron-sized particles (PuO2 NPs). Fundamental research underpinning the behavior of PuO2 NPs under conditions not only relevant to the Hanford tank waste but at high ionic strength in general is needed to reliably predict the chemical reactivity of PuO2 NPs and develop engineering solutions to safely and efficiently process high-level radioactive waste into forms suitable for long-term storage. In this work, we study the behavior of PuO2 NPs (particle size ~100 nm) under high ionic strength conditions by reacting it with highly concentrated (up to 5 M) salt solutions. We explore different electrolyte compositions to elucidate the impact of different anions (NO3-, Cl-, ClO4-, SO42-, C2O42-, CO32-) on the stability of PuO2 NP in the acidic and alkaline pH regime. PuO2 NP aggregation and precipitation as function electrolyte concentration is tracked by a combination of liquid scintillation counting, dynamic light scattering for determination of particle size distributions, and zeta potentials as a proxy for particle charge. At acidic pH, electrolytes containing non-coordinating anions, such as NaNO3, NaCl, and NaClO4 mostly stabilize PuO2 NPs over a large electrolyte concentration range, showing only subtle differences in their reactivity. Other electrolyte anions show a more pronounced effect on the PuO2 NP stability: SO42-, binds directly to the particles’ surface, reverses the particle charge, and precipitates the PuO2 NPs efficiently even at intermediate sulfate concentrations (>0.1 M). In contrast, C2O42- is found to lead to high [Pu] in solution, in the milli-molar range, even at mildly acidic pH (~4). Thermodynamic modeling of the dissolved Pu concentrations using PHREEQC is unable to predict the observed [Pu] in the acidic pH regime, supporting the influence of colloids in maintaining elevated [Pu]. It is noteworthy that the current thermodynamic databases do not include constants for colloidal Pu phases and cannot accurately predict many of the high ionic strength solutions relevant to this work. The mechanisms and models responsible for these observations will need further investigation in the future. At high pH values (~12), PuO2 NPs exhibits classical sol-gel chemistry, meaning that upon destabilization of the colloidal sol, for example by addition of concentrated NaOH, highly porous and viscid PuO2 coagulates are formed that consist of a three-dimensional network likely held together by physical interactions. The PuO2 NP coagulate shows no significant reversibility of the aggregation when contacted with concentrated brines; however, PuO2 NPs can be efficiently resuspended in solution by addition of diluted electrolytes, alkaline solutions containing high amounts of carbonate, or simple addition of water. Especially carbonate is shown to stabilize PuO2 NPs in solution at high pH, characterized by stable colloidal suspensions that are resistant against sedimentation during centrifugation. Thermodynamic modeling of the carbonate system was able to predict an increasing dissolved Pu concentration with increasing carbonate concentration. However, the model was profoundly sensitive to the fixed redox potential and does not include any thermodynamic constants for colloidal Pu species.

Neumann, Julia↗

DOE OSTI2025

Dome-like pressure-temperature phase diagram of the cooperative Jahn–Teller distortion in NaNiO 2

NaNiO 2 is a Ni 3+ -containing layered material consisting of alternating triangular networks of Ni and Na cations, separated by octahedrally-coordinated O anions. At ambient pressure, it features a collinear Jahn–Teller distortion below $T^{JT}_{onset} ≈ 480$ K, which disappears in a first-order transition on heating to $T^{JT}_{onset} ≈ 500$ K, corresponding to the increase in symmetry from monoclinic to rhombohedral. It was previously studied by variable-pressure neutron diffraction (Nagle-Cocco et al 2022 ACS Inorg. Chem. 61 4312) and found to exhibit an increasing $T^{JT}_{onset}$ with pressure up to ∼5 GPa. In this work, powdered NaNiO 2 was studied via variable-pressure synchrotron x-ray diffraction up to pressures of ∼67 GPa at 294 K and 403 K. Suppression of the collinear Jahn–Teller ordering is observed via the emergence of a high-symmetry rhombohedral phase, with the onset pressure occurring at ∼18 GPa at both studied temperatures. Further, a discontinuous decrease in unit cell volume is observed on transitioning from the monoclinic to the rhombohedral phase. These results taken together suggest that in the vicinity of the transition, application of pressure causes the Jahn–Teller transition temperature, $T^{JT}_{onset}$, to decrease rapidly. We conclude that the pressure-temperature phase diagram of the cooperative Jahn–Teller distortion in NaNiO 2 is dome-like.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

AmeriFlux FLUXNET-1F US-xDC NEON Dakota Coteau Field School (DCFS)

This is the AmeriFlux Management Project (AMP) created FLUXNET-1F version of the carbon flux data for the site US-xDC NEON Dakota Coteau Field School (DCFS). This is the FLUXNET version of the carbon flux data for the site US-xDC NEON Dakota Coteau Field School (DCFS) produced by applying the standard ONEFlux (1F) software. Site Description - The Dakota Coteau Field School (DCFS) and Prairie Lake (PRLA) field sites are co-located in an agricultural area used primarily for cattle grazing, just a few miles east of the Woodworth and Prairie Pothole sites at the Chase Lake National Wildlife Refuge. DCFS covers 7.8 km2 (3 square miles) of grazing land in Stutsman County, ND, between the tiny communities of Pingree and Woodworth. The population here is sparse, but the land has been transformed by agricultural activities over the last 150 years. The field site has been used only for grazing, but other land in the surrounding area has been converted to corn and soybean production. DCFS is located in an area known as the "Prairie Pothole Region," a band of tall and mixed prairie that stretches across parts of North and South Dakota, Minnesota and the Canadian provinces of Alberta, Saskatchewan and Manitoba. Historically, this area supported tall to mid-height prairie grasses, including blue gamma and green needlegrass. The land here is pocked by thousands of depressions left behind by glaciers 10,000 years ago, resulting in a series of small lakes and wetland areas known as prairie potholes. These potholes receive most of their water from spring snowmelt and are a primary source of groundwater recharge for the region. NEON data will help researchers monitor the effects of climate change on the Northern Plains ecosystem. Over the last 30 years, the hydrological cycle in the plains has changed dramatically, trending wetter overall and diverging from the historical ten-year cycles. Temperatures are also rising, leading to changes in plant phenology cycles and species distribution that could negatively impact migratory bird populations and other animal species.

Network), NEON (National Ecological Observatory↗

DOE OSTI2020

Integrating field observations and process-based modeling to predict watershed water quality under environmental perturbations

Watersheds play a critical role in supplying water resources needed for human use and ecosystem health. Understanding and predicting how, when, and where changes in the quantity and quality of water resources occur under different environmental stresses including extreme events is crucial for sustainable management of water resources under a changing environment. However, few studies have attempted to quantify or identify the factors and process interactions controlling the impact of extreme events across water-shed systems. Only few large-scale studies include coordinated monitoring and modeling efforts, which limits our ability to assess the large-scale impact of extreme events on water supply and quality. Methods are lacking to propagate uncertainty in process understanding through an integrated hydro-biogeochemical model framework and evaluate its importance, thus failing to take full advantage of the information potentially available through transformative advances in characterization technologies from high-resolution mass spectrometry to airborne and satellite-based remote sensing. There are consequent risks to our nations water security and to human and ecosystem health that may become exacerbated with the increasing frequency of extreme events that is projected for the coming decades. This paper reviews the current status of watershed science for both water quantity and quality and identifies critical gaps in our current knowledge and modeling capability in addressing the emergent needs in predicting watershed hydrologic and biogeochemical responses (i.e., water quantity and quality) under natural and anthropogenic perturbations. We highlight the need to (1) understand how environmental perturbations including extreme events like floods and droughts propagate through watershed systems and assess their short- and long-term impacts on watershed biogeochemistry, water quality and their recovery pathways; (2) develop and improve a watershed water quality model that reflects the state of scientific understanding gained from observations; and (3) construct a data-model fusion system for watershed characterization, process identification, and mechanistic model parameterization. A large base of modeling, monitoring and data capabilities have been built by various federal government agencies given the relevance of water to their critical missions. An emerging need is to build an integrated national capability for watershed water availability and quality that can address water-related missions across multiple federal agencies.

13 HYDRO ENERGY↗

DOE OSTI2020

Final Reports of the 2020 Los Alamos National Laboratory Computational Physics Student Summer Workshop

For the past ten years, the workshop has been bringing a highly talented and diverse group of student every summer. Students work in teams of two, alongside typically two mentors, on research projects reflecting a broad range of topics within computational physics. In addition, students attend a series of lectures on topics within computational physics, facility tours, and networking events. The program lasts ten weeks, with this year’s workshop running from June 8 to August 14. At the end of the summer, students give a final presentation, along with a written report. Those reports are what make up the remaining sections of this document. Admission to the workshop is by a competitive process, with the mentors forming the selection committee. One of the important accomplishments of the workshop has been to create a student pipeline from diverse schools that sometimes are not normally tapped by LANL recruiting. Many workshop students maintain a continuing relationship with LANL, returning as students interns, post-doctoral researchers, and staff members. Additionally, workshop alumni act as ambassadors for LANL. The result is a wider awareness both of LANL as a potential employer, and of the technical work that happens at LANL. This year, the workshop format was changed in several ways, in order to accommodate the off-site, virtual format. Students worked on LANL virtual desktop systems remotely, also accessing LANL HPC resources. In order to facilitate communication, student were given accounts on both Webex, a video teleconferencing platform, and Mattermost, an online team collaboration and chat platform, similar to Slack. Daily communication between students and mentors was primarily on Mattermost, with Webex conferencing as needed. The lectures were all done on Webex. Given the difficulty of the virtual format, and a concern that students might have video teleconferencing burn-out after an academic semester largely moved to that format, all lectures were optional this year. In spite of this, the attendance was generally high. Lecturers were asked to try to move to a more high-level, ”What is it?,” format. Once again, the students did a tremendous job. Over the course of ten weeks, they did important research across a staggering array of disciplines. The following pages contain the final report for each team’s research efforts. We hope you will find reading them as exciting as it was for us to produce them.

36 MATERIALS SCIENCE↗

DOE OSTI2020

The Influence of Aqueous Dispersivity on Transport of Radiological Material at LANL MDA G - 20450

Aqueous dispersivity is a phenomenon by which a solute moving in groundwater mixes with water that does not contain the solute and becomes diluted. Solutes take paths of varying lengths through pore networks or experience slower velocities due to interactions with pore walls. Aqueous dispersivity leads to breakthrough curves with earlier arrival than expected in purely advective systems and persistent 'tails,' or late-arriving, dilute concentrations of the solute. Dispersivity can be longitudinal (in the direction of flow) or transverse (orthogonal to flow). LANL has disposed of radioactive material at Material Disposal Area (MDA) G since the late 1950's. Most of the disposed materials at MDA G are low-level waste (LLW), but other types of radioactive wastes are disposed or stored at the site. For example, there is a collection of remote-handled transuranic waste (RH-TRU) waste in 33 shafts, which were intended to be stored retrievably. Aqueous-phase radionuclides included in models of contaminant transport at MDA G are subject to dispersive processes in porous media of the vadose zone and saturated zone. To model dispersivity at MDA G probabilistically, we created site-specific distributions of aqueous dispersivity. First, we performed a comprehensive review of peer-reviewed publications, reports from other performance assessments of MDA G, and documentation from sites that were considered similar based on expert opinion, such as Yucca Mountain. Data were included from a wide range of sources, so that distributions developed based on the data reflect the current state of knowledge in properties of the subsurface environment. Data were grouped based on value type (e.g., determined via experiment or used in a different model), rock type, zone type (saturated or unsaturated), and site, and were weighted in the distributions according to their relevance to the site and zone type. We combined Monte Carlo simulation and bootstrapping techniques to produce approximate distributions of mean aqueous dispersivity. Distributions of dispersivity for saturated and unsaturated zone transport are differentiated by data weight and the length scales over which transport occurs. We find that underestimating or disregarding transverse dispersivity may lead to overstating simulated well capture in the saturated zone at MDA G. Neglecting transverse dispersivity is a common assumption due in part to use of one-dimensional transport models that do not consider solute spreading orthogonal to flow. Also, we find that variability in longitudinal dispersivity is associated with substantial travel time alterations in the MDA G unsaturated zone and in simulated contaminant breakthrough times at a downstream observation plane in the MDA G saturated zone. Finally, at large scales (>1000 m), a linear trend between the dispersivity coefficient and length over which transport occurs may overestimate the dispersivity coefficient. Future modeling work with application to solute spreading could include interacting advective and diffusive zones in the highly fractured basalt below MDA G. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

DECOVALEX-2023: Task F1 Final Report

DECOVALEX-2023 Task F is a comparison of models and methods for post-closure performance assessment (PA) of a deep geologic repository for radioactive waste. The general aims of Task F are to build confidence in the models, methods, and software used for PA and to stimulate additional research and development in PA methodologies. The task objectives are to motivate development of PA modelling skills and capabilities, to examine the influence of model choices on calculated repository performance, and to compare the uncertainties introduced by model choices to other sources of uncertainty. Task F involves no actual experiment or site. It is a PA modelling exercise that requires the conceptual development of hypothetical repository designs and geologic settings. Because three of the teams were interested in salt and the rest of the teams were interested in crystalline rock, Task F was split into two branches: Task F1 for crystalline rock and Task F2 for salt. This report is for Task F1, crystalline rock. Teams from seven countries (Canada, Czech Republic, Germany, Korea, Sweden, Taiwan, and United States) participated in Task F1. The teams worked together to define the features, events, and processes of the reference case repository and established a set of performance measures. In addition, they defined a set of benchmark problems designed to test and compare modelling capabilities for fracture flow and transport at different scales. The repository design and benchmark problems are documented in a Task Specification that evolved over time as the group honed the specifications. The benchmark problems verified that each team can aptly model flow and transport in fractured media in 1-, 2-, and 3-dimensions. Two general approaches were used for the 3-dimensional benchmarks: discrete fracture network (DFN) and equivalent continuous porous medium (ECPM). DFN modelling involves explicit meshing of each fracture while ECPM modelling aims to capture the effective porosity and directional permeability of each cell in a space-filling mesh as affected by intersecting fractures. In some models, a combination of the two is used, i.e., DFN for large known fractures and ECPM for the rest of the domain. Transport is solved by using either the advection-dispersion equation or particle tracking. Although some variation is observed among model breakthrough curves in the benchmark problems, there is strong agreement in breakthrough behaviour up to at least the 75 th percentile for all benchmarks. At the 90 th percentile, breakthrough results show larger differences, suggesting several models retain substantially higher fractions of tracer in regions of slower moving water. In addition to the flow and transport benchmarks, several teams completed the source term benchmark, verifying capabilities for modelling radionuclide decay and ingrowth, waste package breach, instant release fractions, fuel matrix degradation rates, and radionuclide solubility limitations. The reference case is conceptualized as a generic spent fuel repository at a depth of 450 m in fractured crystalline rock. The repository has 50 parallel backfilled drifts, each with 50 deposition holes 6 m apart. Each deposition hole contains a 4-PWR waste package and bentonite buffer. The rock domain is 5 km in length, 2 km in width, and 1 km in depth. It has 6 deterministic fractured deformation zones and a multitude of stochastic fractures. Teams generally used the ECPM approach for the entire rock or a hybrid approach in which the deterministic fracture zones are modelled with a DFN and the rest of the rock is modelled by ECPM. Of the reference case problems specified, only the results of the initial reference case problem are compared in this report. The initial problem focuses on transport from the deposition holes to the surface, i.e., it neglects waste package performance. Tracers are released at all waste package locations at time zero and tracked for their releases to the near field and ground surface. The water fluxes calculated at the ground surface entry and exit regions of the domain are similar for all models except for two that have considerably lower fluxes. For tracer transport, large differences are observed among models in the magnitude of tracer transported. Much of the difference appears to be due to how the repository is implemented and hence the different degrees of repository simplification. Models that exclude the drifts, buffer, and backfill from the domain tend to show greater release of tracers and radionuclides from the repository. The initial study presented here indicates that major differences in modelling important processes within the repository (e.g., diffusion through buffer and backfill) can produce broadly different release and transport results, especially when those processes are excluded. Even for the models that included all specified features, events, and processes, the results show significant differences and demonstrate the importance of examining multiple modelling approaches in performance assessment. The differences in results observed in this study are expected to motivate teams to either increase complexity in future versions of the reference case models or to improve methods to account for the effects of simplified features and processes. Either way, future improvements in these models are expected to produce results that more closely agree.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Advancing ocean monitoring and knowledge for societal benefit: the urgency to expand Argo to OneArgo by 2030

The ocean plays an essential role in regulating Earth’s climate, influencing weather conditions, providing sustenance for large populations, moderating anthropogenic climate change, encompassing massive biodiversity, and sustaining the global economy. Human activities are changing the oceans, stressing ocean health, threatening the critical services the ocean provides to society, with significant consequences for human well-being and safety, and economic prosperity. Effective and sustainable monitoring of the physical, biogeochemical state and ecosystem structure of the ocean, to enable climate adaptation, carbon management and sustainable marine resource management is urgently needed. The Argo program, a cornerstone of the Global Ocean Observing System (GOOS), has revolutionized ocean observation by providing real-time, freely accessible global temperature and salinity data of the upper 2,000m of the ocean (Core Argo) using cost-effective simple robotics. For the past 25 years, Argo data have underpinned many ocean, climate and weather forecasting services, playing a fundamental role in safeguarding goods and lives. Argo data have enabled clearer assessments of ocean warming, sea level change and underlying driving processes, as well as scientific breakthroughs while supporting public awareness and education. Building on Argo’s success, OneArgo aims to greatly expand Argo’s capabilities by 2030, expanding to full-ocean depth, collecting biogeochemical parameters, and observing the rapidly changing polar regions. Providing a synergistic subsurface and global extension to several key space-based Earth Observation missions and GOOS components, OneArgo will enable biogeochemical and ecosystem forecasting and new long-term climate predictions for which the deep ocean is a key component. Driving forward a revolution in our understanding of marine ecosystems and the poorly-measured polar and deep oceans, OneArgo will be instrumental to assess sea level change, ocean carbon fluxes, acidification and deoxygenation. Emerging OneArgo applications include new views of ocean mixing, ocean bathymetry and sediment transport, and ecosystem resilience assessment. Implementing OneArgo requires about $100 million annually, a significant increase compared to present Argo funding. OneArgo is a strategic and cost-effective investment which will provide decision-makers, in both government and industry, with the critical knowledge needed to navigate the present and future environmental challenges, and safeguard both the ocean and human wellbeing for generations to come.

ARGO↗

DOE OSTI2025

Pantex Plant Ogallala Aquifer and Perched Groundwater Contingency Plan

The Pantex Plant Ogallala Aquifer and Perched Groundwater Contingency Plan has been developed in accordance with the requirements identified in the: • Interagency Agreement for the Pantex Superfund Site, Article 8.5 Work to be Performed, • Compliance Plan Provision of Hazardous Waste Permit No. 50284, and • Record of Decision for Groundwater, Soil, and Associated Media, Pantex Plant. A Long‐Term Monitoring System Design has been designed to monitor conditions in the perched groundwater including changes in the perched aquifer as a result of implementing the response actions. Monitoring is required for verifying the effectiveness of perched groundwater response actions (i.e., conditions in the perched aquifer are being affected as intended) and for confirming that the perched aquifer and Ogallala Aquifer characterization as defined in the Resource Conservation and Recovery Act Facility Investigation Report and the Corrective Measure Studies/Feasibility Study remains accurate. If monitoring results obtained through the monitoring network identify an unexpected condition or deviation, contingent actions will be considered and implemented as necessary to ensure continued protection of the Ogallala Aquifer and human health and the environment. Potential deviations to expected technology performance may be encountered for each of the four primary response actions that compose the selected remedy for perched groundwater; Playa 1 Pump and Treat System, Southeast Area Pump and Treat System, Southeast Area In‐Situ Bioremediation System (comprised of the Southeast In‐Situ Bioremediation System Original System, Southeast Area In‐Situ Bioremediation System Extension System, Offsite In‐Situ Bioremediation System, Perchlorate/Chromium ISB, Northeast ISB and County Road 8 ISB), and Zone 11 In‐Situ Bioremediation System. Monitoring will also be conducted to determine if there are deviations to the expected characterization, e.g., contaminants not expected as a result of the RCRA Facility Investigation characterization. Deviations to expected conditions in the Ogallala Aquifer could also be encountered if the response actions in the perched groundwater are not performing as expected, i.e., preventing contaminants from migrating to the Ogallala Aquifer. Currently, Pantex has begun investigation of detections of high explosives above groundwater protection standards in wells on the Texas Tech University property and a plume that is moving to the northeast from that area. Due to those detections, this Plan recognizes the fact that future detections in the Ogallala will be focused on first‐ time detections of analytes. After a remedy is determined, this Plan will require modification to address-deviations and contingent actions. This Plan was developed to identify the contingent actions necessary to mitigate impacts resulting from deviations to site conditions or response action performance. The Plan defines the environmental problem being addressed by the response actions, clarifies the expected conditions and objectives of the response actions, and identifies the potential deviations to the response actions (due to site conditions or technology performance) that could be encountered. The deviations were evaluated to determine the likelihood of occurrence, potential impact, and time to respond to avoid impact. The Plan also identifies the monitoring outlined in the Long‐Term Monitoring System Design Report (Consolidated Nuclear Security, 2024) and Sampling Analysis Plan (PanTeXas Deterrence, 2024) that will be used to detect the deviations. Lastly, the Plan specifies the contingent actions that could be implemented in response to the deviations. Because each response focuses on a discrete portion of the perched aquifer and contaminant plume, each response action has a different set of expected conditions, and therefore differing impacts from deviations to the site and technology expectations. As a result, the contingent actions are identified for each response action and potential deviation including specific constituents, location, and conditions. If deviations are encountered that impact the ability of the response action to meet performance objectives, the contingent actions will be focused on ensuring the response action can meet the performance objective. Contingent actions may be implemented as interim actions (ISMs/removal actions) in accordance with the Record of Decision, Interagency Agreement, and Hazardous Waste Permit‐50284, if warranted by the specific circumstances. For deviations to site characterization expected conditions, the contingent action will focus on determination of the source of the deviation, determination of the appropriate response, and evaluation of additional work to be completed. However, if the deviation to characterization impacts the performance of the response action, the contingent action will again focus on ensuring performance objectives can be met. Early source term removals and cleanup actions have been implemented to protect the Ogallala Aquifer. Because of these actions and based on modeling results, the expected conditions in the Ogallala Aquifer are that constituents of concern will not be detected above the Groundwater Protection Standards (GWPSs) nor will they reach potential points of exposure above the GWPS. The primary deviation of concern for the Ogallala is if constituents are detected in the Ogallala Aquifer near or above GWPSs. If it occurs, this change in expected conditions would require further evaluation of site and contaminant characteristics to determine an appropriate course of action. The evaluation would include additional monitoring, source identification, implementation of interim protective measures (if necessary), and delineation of extent. These evaluations are necessary to determine an appropriate response action for the Ogallala. The primary goal of the Plan is to provide for the continued protection of the Ogallala Aquifer and the health of its consumers. In recognition, this Plan presents a flexible and rational approach for making future decisions associated with confirming the change in perched and Ogallala aquifer conditions and identifying a response (technical activities, changes to response actions, regulatory oversight, and public involvement).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗