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

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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Quantification of CO 2 Mineralization at the Wallula Basalt Pilot Project

In 2013, the Pacific Northwest National Laboratory led a geologic carbon sequestration field demonstration where ~1000 tonnes of CO 2 was injected into several deep Columbia River Basalt zones near Wallula, Washington. Rock core samples extracted from the injection zone two years after CO 2 injection revealed nascent carbonate mineralization that was qualitatively consistent with expectations from laboratory experiments and reactive transport modeling. In this study, we report on a new detailed analysis of the 2012 pre-injection and 2015 post-injection hydrologic tests that capitalizes on the difference in fluid properties between scCO 2 and water to assess changes in near-field, wellbore, and reservoir conditions that are apparent approximately two years following the end of injection. This comparative hydrologic test analysis method provides a new way to quantify the amount of injected CO 2 that was mineralized in the field test. Modeling results indicate that approximately 60% of the injected CO 2 was sequestered via mineralization within two years, with the resulting carbonates occupying ~4% of the available reservoir pore space. The method presented here provides a new monitoring tool to assess the fate of CO 2 injected into chemically reactive basalt formations but could also be adapted for long-term monitoring and verification within more traditional subsurface carbon storage reservoirs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Antecedent Hydrologic Conditions Reflected in Stream Lithium Isotope Ratios During Storms

Antecedent hydrological conditions are recorded through the evolution of dissolved lithium isotope signatures (δ 7 Li) by juxtaposing two storm events in an upland watershed subject to a Mediterranean climate. Discharge and δ 7 Li are negatively correlated in both events,but mean δ 7 Li ratios and associated ranges of variation are distinct between them. We apply a previously developed reactive transport model (RTM) for the site to these event-scale flow perturbations, but observed shifts in stream δ 7 Li are not reproduced. To reconcile the stability of the subsurface solute weathering profile with our observations of dynamic stream δ 7 Li signatures, we couple the RTM to a distribution of fluid transit times that evolve based on storm hydrographs. The approach guides appropriate flux-weighting of fluid from the RTM over a range of flow path lengths, or equivalently fluid residence times. This flux-weighted RTM approach accurately reproduces dynamic storm δ 7 Li-discharge patterns distinguished by the antecedent conditions of the watershed.

58 GEOSCIENCES↗
DOE OSTI2020

Relating the depth of the water table to the depth of weathering

Weathering of bedrock creates and occludes permeability, affecting subsurface water flow. Often, weathering intensifies above the water table. On the other hand, weathering can also commence below the water table. To explore relationships between weathering and the water table, a simplified weathering model for an eroding hillslope was formulated that takes into account both saturated and unsaturated subsurface water flow (but does not fully account for changes in dissolved gas chemistry). The phreatic line was calculated using solutions to mathematical treatments for both zones. In the model, the infiltration rate at the hill surface sets both the original and the eventual steady-state position of the water table with respect to the weathering reaction front. Depending upon parameters, the weathering front can locate either above or below the water table at steady state. Erosion also affects the water table position by changing porosity and permeability even when other hydrological conditions (e.g. hydraulic conductivity of parent material, infiltration rate at the surface) do not change. The total porosity in a hill (water storage capacity) was found to increase with infiltration rate (all else held constant). Furthermore, this effect was diminished by increasing the erosion rate. We also show examples of how the infiltration rate affects the position of the water table and how infiltration rate affects weathering advance.

58 GEOSCIENCES↗
DOE OSTI2025

Representing lateral groundwater flow from land to river in Earth system models

Lateral groundwater flow (LGF) is an important hydrologic process in controlling water table dynamics. Due to the relatively coarse spatial resolutions of land surface models, the representation of this process is often overlooked or overly simplified. In this study, we developed a hillslope-based lateral groundwater flow model. Specifically, we first developed a hillslope definition model based on an existing watershed delineation model to represent the subgrid spatial variability in topography. Building upon this hillslope definition, we then developed a physical-based lateral groundwater flow using Darcy’s equation. This model explicitly considers the relationships between the groundwater table along the hillslope and the river water table levels. We coupled this intra-grid model to the land component (E3SM Land Model: ELM) and river component (MOdel for Scale Adaptive River Transport: MOSART) of the Energy Exascale Earth System Model (E3SM). We tested both the hillslope definition model and the lateral groundwater flow model and performed sensitivity experiments using different configurations. Simulations for a single grid cell at 0.5°×0.5° within the Amazon basin show that the definition of hillslope is the key to modeling lateral flow processes and the runoff partition between surface and subsurface can be dramatically changed using the hillslope approach. Although our method provides a pathway to improve the lateral flow process, future improvements are needed to better capture the subgrid structure to account for the spatial variability in hillslopes within the simulated grid of land surface models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Evaluation of subsurface transport processes of delayed gas signatures applicable to underground nuclear explosions

Radioactive gas signatures from underground nuclear explosions (UNEs) result from gas-migration processes occurring in the subsurface. The processes considered in this study either drive or retard upward migration of gases from the detonation cavity. The relative importance of these processes is evaluated by simulating subsurface transport in a dual-permeability medium for the multi-tracer Noble Gas Migration Experiment (NGME) originally intended to study some aspects of transport from a UNE. For this experiment, relevant driving processes include weak two-phase convection driven by the geothermal gradient, over pressuring of the detonation cavity, and barometric pumping while gas sorption, dissolution, radioactive decay, and usually diffusion represent retarding processes. From deterministic simulations we found that over-pressuring of the post-detonation chimney coupled with barometric pumping produced a synergistic effect amplifying the tracer-gas reaching the surface. Bounding simulations indicated that the sorption and dissolution of gases, tending to retard transport, were much smaller than anticipated by earlier laboratory studies. The NGME observations themselves show that differences in gas diffusivity have a larger effect on influencing upward transport than do the combined effects of tracer-gas sorption and dissolution, which is consistent with a Sobol’ sensitivity analysis. Both deterministic simulations and those considering parametric uncertainties of transport-related properties predict that the excess in concentration of SF 6 compared to 127 Xe as might be captured in small volumetric samples should be much smaller than the order-of-magnitude contrast found in the large-volume gas samples taken at the site. While extraction of large-volume subsurface gas samples is shown to be capable of distorting in situ gas compositions, the highly variable injection rate of SF 6 into the detonation cavity relative to that of 127 Xe at the start of the field experiment is the most likely explanation for the large difference in observed concentrations.

58 GEOSCIENCES↗
DOE OSTI2024

Characterization of Most Promising Sequestration Formations in the Rocky Mountain Region

The project Characterization of Most Promising Sequestration Formations in the Rocky Mountain Region is one of 9 site characterization projects that were implemented as part of ARRA (American Recovery and Reinvestment Act). Data from this project was used to improve resolution of data in NATCARB in the area of study. Data related to this study has already been incorporated in NATCARB Atlas. The Rocky Mountain Carbon Capture and Storage (RMCCS) project investigated multiple geologic formations and characterized a local site on the Colorado Plateau for future CCS opportunities. The RMCCS project focused on the Cretaceous Dakota, Jurassic Entrada, and Pennsylvanian Weber Sandstones, the three largest regional formations. All formations in this project are potential CO2 storage resources for future power plants, natural gas processing plants, cement plants, and oil shale development projects. The area adjacent to Craig, Colorado, (Sand Wash Basin) was the area selected for detailed geologic characterization on the RMCCS project. The basin was selected in part because the geology can be extrapolated to other sites on the Colorado Plateau. Field mapping and seismic surveys were conducted to identify and evaluate the basin's structural configuration. A 9,745-foot deep characterization well was drilled to collect 131 feet of core and a suite of geophysical well log data. Petrophysical tests on samples of core were used to calibrate geophysical log data, which can be used to obtain storage resource estimates and evaluate associated uncertainty as well as simulate the hydrologic behavior of injected CO2. A detailed analysis of the primary formations (Dakota, Entrada and Weber sandstones) yielded a more accurate CO2 storage resource assessment for these formations within the Colorado Plateau; RMCCS estimates indicate a total CO2 storage resource of more than 38,000 million metric tons. The characterization of the Sand Wash Basin (2-D seismic surveys, multiple well logs and lithological, petrophysical and geochemical analyses) allowed for a detailed 3-D model to be constructed. The model served as the framework for analyses ranging from CO2 storage resource, injectivity, and subsurface flow to uncertainty estimates to evaluation of risk.

2-D seismic↗
DOE OSTI2024

Impacts of Sea‐Level Rise on Coastal Groundwater Table Simulated by an Earth System Model With a Land‐Ocean Coupling Scheme

Abstract Sea‐level rise (SLR) poses a severe threat to the coastal environment through seawater intrusion into freshwater aquifers. The rising groundwater table also exacerbates the risk of pluvial, fluvial, and groundwater flooding in coastal regions. However, current Earth system models (ESMs) commonly ignore the exchanges of water at the land‐ocean interface. To address this gap, we developed a novel land‐ocean hydrologic coupling scheme in a state‐of‐the‐science ESM, the Energy Exascale Earth System Model version 2 (E3SMv2). The new scheme includes the lateral exchange between seawater and groundwater and the vertical infiltration of seawater driven by the SLR‐induced inundation. Simulations were performed with the updated E3SMv2 for the global land‐ocean interface to assess the impacts of SLR on coastal groundwater under a high CO 2 emission scenario. By the middle of this century, seawater infiltration on the inundated areas will be the dominant component in the land‐ocean coupling process, while the lateral subsurface flow exchange will be much smaller. The SLR‐induced seawater infiltration will raise the groundwater levels, enhance evapotranspiration, and increase runoff with distinct spatial patterns globally in the future. Although the coupling process is induced by SLR, we found topography and warming temperature have more control on the coupling impacts, probably due to the relatively modest magnitude of SLR during the selected future period. Overall, our study suggests significant groundwater and seawater exchange at the land‐ocean interface, which needs to be considered in ESMs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Permafrost thermal conditions are sensitive to shifts in snow timing

Abstract Changes in snow precipitation at high latitudes can significantly affect permafrost thermal conditions and thaw depth, potentially exposing more carbon-laden soil to microbial decomposition. A fully coupled process-based surface/subsurface thermal hydrology model with surface energy balance is used to analyze the impact of intra-annual variability in snow on permafrost thermal regime and the active layer thickness. In the four numerical scenarios considered, simulations were forced by the same meteorological data, except the snow precipitation, which was systematically altered to change timing of snowfall. The scenarios represent subtle shifts in snow timing, but the snow onset/melt days, the end of winter snowpack depth, and total annual snow precipitation are unchanged among scenarios. The simulations show that small shifts in the timing of snow accumulation can have significant effects on subsurface thermal conditions leading to active layer deepening and even talik formation when snowfall arrives earlier in the winter. The shifts in snow timing have a stronger impact on wetter regions, especially soil underneath small ponds, as compared to drained regions. This study highlights the importance of understanding potential changes in winter precipitation patterns for reliable projections of active-layer thickness in a changing Arctic climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

The stable isotopes of natural waters at the Marcell Experimental Forest

Here, we present a new data set from the Marcell Experimental Forest (MEF) that compiles water isotope measurements from multiple research catchments, some of which have been studied since the 1960s. The MEF is located in northern Minnesota, USA, and is home to heavily studied and monitored forests, streams, bogs, and fens. Peat-forming systems (bogs and fens) are an important component of the MEF landscape and have a profound impact on the water cycle in these catchments. Within the last decade, analysis of stable isotopes of water (expressed as δD and δ 18 O) has been implemented to characterize the different components of the water budget, and to allow researchers to look at catchment and peatland-specific hydrologic effects in the watershed. This δD and δ 18 O data set of natural waters from MEF catchments is primarily composed of measurements from three peatlands (S1, S2, S6) during an 11-year period. More recently collection and analysis were expanded to also include samples from the Spruce and Peatland Responses Under Changing Environments (SPRUCE) project in the S1 bog, peatlands S3, S4, S5, as well as nearby lakes. We establish a local meteoric water line by analyzing the isotopic composition of precipitation, which fills a void in regional meteoric water lines for Minnesota. Furthermore, we establish baseline isotopic composition for bog outlet streams, bog porewater, aquifer groundwater, overland flow, subsurface stormflow, and snowpack, as well as runoff from the SPRUCE experimental chambers. These data are publicly available and will be expanded upon in the future.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Modeling Geologic Waste Repository Systems Below Residual Saturation

The heat generated by high-level radioactive waste can pose numerical and physical challenges to subsurface flow and transport simulators if the liquid water content in a region near the waste package approaches residual saturation due to evaporation. Here, residual saturation is the fraction of the pore space occupied by liquid water when the hydraulic connectivity through a porous medium is lost, preventing the flow of liquid water. While conventional capillary pressure models represent residual saturation using asymptotically large values of capillary pressure, here, residual saturation is effectively modeled as a tortuosity effect alone. Treating the residual fluid as primarily dead-end pores and adsorbed films, relative permeability is independent of capillary pressure below residual saturation. To test this approach, PFLOTRAN is then used to simulate thermal-hydrological conditions resulting from direct disposal of a dual-purpose canister in unsaturated alluvium using both conventional asymptotic and revised, smooth models. Importantly, while the two models have comparable results over 100 000 years, the number of flow steps required is reduced by approximately 94%.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

EBS Task Force: Task 9/FEBEX Modeling Final Report: Thermo-Hydrological Modeling with PFLOTRAN

This report outlines Sandia National Laboratories modeling studies applied to Stage 1 and Stage 2 of the Full-scale Engineered Barriers Experiment in Crystalline Host Rock (FEBEX) in situ test for the SKB EBS Task Force Task 9. The FEBEX test was a full-scale test conducted over ~18 years at the Grimsel, Switzerland Underground Research Laboratory (URL) managed by NAGRA. It involved emplacing simulated waste packages, in the form of welded cylindrical heaters, inside a tunnel in crystalline granitic rock and surrounded by a bentonite barrier and cement plug. Sensors emplaced within the bentonite monitored the wetting-up, heating, and drying out of the bentonite barrier, and the large resulting data set provides an excellent opportunity for validation of multiphysics Thermal-Hydrological (TH), Thermal-Hydrologic-Chemical (THC), and Thermal-Hydrological-Mechanical (THM) modeling approaches for underground nuclear waste storage and the performance of engineered bentonite barriers. The present status of the EBS Task Force is finalizing Task 9, which follows years of modeling studies of the FEBEX test, by many notable modeling teams (Gens et al., 2009; Sanchez et al. 2010; 2012; Samper et al., 2018). These modeling studies generally use two-dimensional axisymmetric meshes, ignoring threedimensional effects, gravity and asymmetric wetting and dry out of the bentonite engineered barrier. This study investigates these effects with use of the PFLOTRAN THC code with massively parallel computational methods in modeling FEBEX Stage 1 and Stage 2 results. The PFLOTRAN numerical code is an open source, state-of-the-art, massively parallel subsurface flow and reactive transport code operating in a high-performance computing environment (Hammond et al., 2014). Section 2 describes the applied partial differential equations describing mass, momentum and energy balance used in this study, considerations derived by assuming phase equilibrium between gas and liquid phases, constitutive equations for granite, cement plug, and bentonite domains, and specific approaches for use inthe PFLOTRAN code. Section 3 describes the geometry, meshing, and model set-up. Section 4 describes modeling results, Section 5 compares modeling results to field testing data, and Section 6 gives conclusions. The Appendix provides detailed information required by the EBSTask Force for final reporting.

42 ENGINEERING↗
DOE OSTI2021

Modeling Terrestrial Dissolved Organic Carbon Loading to Western Arctic Rivers

The mobilization and land-to-ocean transfer of dissolved organic carbon (DOC) in Arctic watersheds is intricately linked with the region's climate and water cycle, and furthermore at risk of changes from climate warming and associated impacts. This study quantifies model-simulated estimates of runoff, surface and active layer leachate DOC concentrations and loadings to western Arctic rivers, specifically for basins that drain into coastal waters between and including the Yukon and Mackenzie Rivers. Model validation leverages data from other field measurements, synthesis studies, and modeling efforts. The simulations effectively quantify DOC leaching in surface and subsurface runoff and broadly capture the seasonal cycle in DOC concentration and mass loadings reported from other studies that use river-based measurements. A marked east-west gradient in simulated spring and summer DOC concentrations of 24 drainage basins on the North Slope of Alaska is captured by the modeling, consistent with independent data derived from river sampling. Simulated loadings for the Mackenzie and Yukon show reasonable agreement with estimates of DOC export for annual totals and four of the six seasonal comparisons. Nearly equivalent loading occurs to rivers which drain north to the Beaufort Sea and west to the Bering and Chukchi Seas. The modeling framework provides a basis for understanding carbon export to coastal waters and for assessing impacts of hydrological cycle intensification and permafrost thaw with ongoing warming in the Arctic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Data for Machado-Silva et al. (2024), "Short-Term Groundwater Level Fluctuations Drive Subsurface Redox Variability"

This dataset contains the analytical data reported in Machado-Silva et al. (2024) as part of the COMPASS-FME project, which seeks to advance a scalable, predictive understanding of the fundamental biogeochemical processes, ecological structure, and ecosystem dynamics that distinguish coastal terrestrial-aquatic interfaces from the purely terrestrial or aquatic systems to which they are coupled. The dataset consists of water quality parameters as well as redox potential, water content, and electrical conductivity. These data were collected in 2022 in Crane Creek (CRC), Portage River (PTR), and Old Woman Creek (OWC). Each of these sites included uplands (UP), transitions (TR), wetland-transition edge (WTE), and wetland (W) zones. The sites represent replicates of the Lake Erie terrestrial-aquatic interface under fluctuating water levels and are located in well-preserved areas with natural or restored marsh and forest cover.This dataset consists of a single data file (Machado_Silva_et_al_2024_EST_data.csv) that is in comma-separated value (CSV) format. No special software is required to read it.This dataset uses the ESS-DIVE Hydrologic Monitoring Reporting Format 1.0.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Community-Informed Urban Flood Modeling for Impact Mitigation

The intensification of the hydrologic cycle due to climate change poses a threat to aging and under-designed water infrastructure systems which cannot adequately manage intense storm events. Developing a comprehensive plan for managing rain-driven flooding events is challenging due to uncertainties in the magnitude and frequency of future storm events and conflicting stakeholder objectives. In the City of Baltimore, Maryland, stormwater infrastructure is struggling to keep up with rainfall-driven (pluvial) flooding events, which regularly damage housing and disrupt transportation for residents. In this study, a hybrid of community engagement, numerical modeling, and artificial intelligence techniques are employed to explore prospective urban flooding adaptations. Community engagement drives the development of an urban flooding model (EPA Storm Water Management Model) for the Baltimore Harbor watershed. The model integrates complex surface and subsurface stormwater infrastructure data from the City, high-resolution spatial data, insights from local public works experts, and the lived experiences of City residents. This co-developed model simulates adaptations of interest to stakeholders in the city, including green and grey infrastructure and operational management strategies. Stormwater management scenarios focused on inlet cleaning and spatially concentrated green infrastructure are found to be the most effective in reducing flood depths in community priority locations. Together, these adaptations can reduce the duration of intersection inundation by more than twenty minutes, allowing for quicker emergency response and restoration of typical transportation systems. Future work will combine this community engaged flooding model with the Deep Uncertainties Pathways framework to explore tradeoffs between adaptations and develop dynamic adaptations which align with community objectives, enhance climate resilience in Baltimore, and can be adjusted in response to changing future conditions.

Ava, Spangler [Pennsylvania State University]↗
DOE OSTI2022

Conservative solute transport processes and associated transient storage mechanisms: Comparing streams with contrasting channel morphologies, land use and land cover

Abstract Land use within a watershed impacts stream channel morphology and hydrology and, therefore, in‐stream solute transport processes and associated transient storage mechanisms. This study evaluated transport processes in two contrasting stream sites where channel morphology was influenced by the surrounding land use, land cover, climate and geologic controls: Como Creek, CO, a relatively undisturbed, high gradient, forested stream with a gravel bed and complex channel morphology, and Clear Creek, IA, an incised, low‐gradient stream with low‐permeability substrate draining an agricultural landscape. We performed conservative stream tracer injections at these sites to address the following questions: (1) How does solute transport vary between streams with differing morphologies? and (2) How does solute transport at each stream site change as a function of discharge? We analysed in‐stream tracer time series data and compared results quantifying solute attenuation in surface and subsurface transient storage zones. Significant trends were observed in these metrics with varying discharge conditions at the forested site but not at the agricultural site. There was a broad range of transport mechanisms and evidence of substantial exchange with both surface and hyporheic transient storage in the relatively undisturbed, forested stream. Changing discharge conditions activated or deactivated different solute transport mechanisms in the forested site and greatly impacted advective travel time. Conversely in the simplified agricultural stream, there was a narrow range of solute transport behaviour across flows and predominantly surface transient storage at all measured discharge conditions. These results demonstrate how channel simplification inhibits available solute transport mechanisms across varying discharge conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Soil frost controls streamflow generation processes in headwater catchments

The relationship between snowmelt and spring streamflow is changing under warming temperatures and diminishing snowpack. At the same time, the hydrologic connectivity across catchment landscape elements, such as snowpack and surface wetlands, can play a critical role in controlling the routing of snowmelt to streams. The role of hydrologic connectivity is important in headwater regions of the continental northern latitudes, where catchments have low topographic relief and seasonally frozen ground. Nevertheless, the effects of soil frost on the sequence, timing, and magnitudes of hydrologic events that drive the movement of water from a snowpack to a stream are not fully understood. Therefore, we examine two questions: First, what is the flowpath that snow melt and precipitation from spring rain events takes to generate spring streamflow, and second, what hydrologic, climatic, or landscape variables exert the most control on the magnitude of streamflow? In this work, we use long-term hydrological records from the two reference basins at the Marcell Experimental Forest in northern Minnesota to analyze the cascading effects across precipitation, snow, water table elevation, soil frost, and streamflow in peatland-dominated headwater catchments. We identify a sequence of fill-and-spill effects across the landscape that control the timing of spring streamflow generation. Then, we use stepwise regression to show that soil frost is a key supporting predictor for both the magnitude of streamflow in the spring as it adds significantly to the predictive power of precipitation and water table elevation. Our results highlight the importance of recognizing the role of soil frost, when present, on the partitioning of snowmelt between overland runoff and water table recharge during the critical snowmelt period, as well as the later partitioning between evapotranspiration and subsurface flows.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Integrated Effects of Site Hydrology and Vegetation on Exchange Fluxes and Nutrient Cycling at a Coastal Terrestrial‐Aquatic Interface

Abstract The complex interactions among soil, vegetation, and site hydrologic conditions driven by precipitation and tidal cycles control the biogeochemical transformations and bi‐directional exchange of carbon and nutrients across the terrestrial–aquatic interfaces (TAIs) in coastal regions. This study uses a highly mechanistic model, Advanced Terrestrial Simulator (ATS)‐PFLOTRAN, to explore how these interactions affect exchanges of materials and carbon and nitrogen cycling. We used a transect in the Chesapeake Bay region that spans zones of open water, coastal wetland, transition, and upland forest. We designed several simulation scenarios to parse the effects of the individual controlling factors and the sensitivity of carbon cycling to reaction rate parameters derived from laboratory experiments. Our simulations reveal an active zone for carbon cycling under the transition zones between the wetland and the upland. Evapotranspiration is found to enhance the exchange fluxes between the surface and subsurface domains, resulting in a higher dissolved oxygen concentration in the TAIs. The transport of organic carbon derived from plant leaves and roots provide an additional source of organic carbon needed for the aerobic respiration and denitrification processes in the TAIs. The variability in reaction rate parameters associated with microbial activities is also found to play a dominant role in controlling the heterogeneity and dynamics of the simulated redox conditions. This modeling‐focused exploratory study enabled us to better understand the complex interactions among soil, water and microbes that govern the hydro‐biogeochemical processes at the TAIs, which is an important step toward representing coastal ecosystems in larger‐scale Earth system models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Influence of physical and chemical hydrology on bioremediation of a U-contaminated aquifer informed by reactive transport modeling incorporating 238 U/ 235 U ratios

Microbially-catalyzed reductive immobilization of aqueous uranium (U) as a solid phase has been proposed as a U remediation technique. Both laboratory and field experiments have demonstrated that this reduction reaction alters the 238 U/ 235 U ratio, producing a 238 U-enriched U(IV) solid. In contrast, other major U reactive transport processes fractionate these isotopes much less. This suggests the potential to quantify the extent of bioreduction occurring in groundwater containing U using the 238 U/ 235 U ratio, which would substantially improve upon current practices largely relying on U concentration measurements alone. Current reactive transport models for uranium dynamics include only concentration measurements, which are strongly influenced by highly coupled reactive transformation and aqueous transport processes. The complex physical and chemical behavior of U potentially compromises such quantitative analysis of U storage and release. Here we report the first numerical reactive transport model which explicitly incorporates variations in the 238 U/ 235 U ratio of U and demonstrates improved interpretation of the principal chemical reactions and groundwater transport processes affecting the subsurface mobility and distribution of this widespread contaminant. Recent U bioreduction studies performed in a contaminated aquifer in Rifle, Colorado, USA applied Rayleigh distillation models to interpret U stable isotope fractionation observed as a result of acetate amendment. These simplified models were unable to resolve the spatiotemporal pattern of U isotope fractionation recorded in the aqueous solutes. Here, we employ the multi-component, isotope-enabled CrunchTope reactive transport software to interpret these measured U isotope ratios, and demonstrate accurate reproduction of observed trends in both geochemistry and 238 U/ 235 U ratios for two consecutive years of field experiments. Overall, our results indicate that accurately modeling both the U concentration and isotope ratio distributions greatly constrains the parameter space of the model. We find that the transport properties of U in the Rifle aquifer are governed by the presence of low-permeability regions, which the isotopes are uniquely sensitive to. When U reduction is spatially constrained by these low-permeability regions, the shift in the 238 U/ 235 U ratio becomes more muted. Accurate modeling of observed U isotope ratios thus provides a powerful means to better understand bioremediation, and the current study serves to advance the application of this novel method.

238U/235U↗