Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “reactive transport”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 253 records · Page 14

International Collaborations Activities on Disposal in Argillite R&D: Characterization Studies and Modeling Investigations

This interim report is an update of ongoing experimental and modeling work on bentonite material described in Jové Colón et al. (2019, 2020) from past international collaboration activities. As noted in Jové Colón et al. (2020), work on international repository science activities such as FEBEX-DP and DECOVALEX19 is either no longer continuing by the international partners. Nevertheless, research activities on the collected sample materials and field data are still ongoing. Descriptions of these underground research laboratory (URL) R&D activities are described elsewhere (Birkholzer et al. 2019; Jové Colón et al. 2020) but will be explained here when needed. The current reports recent reactive-transport modeling on the leaching of sedimentary rock.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

GDSA PFLOTRAN Development (FY2021)

The Spent Fuel & Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Spent Fuel & Waste Disposition (SFWD) is conducting research and development (R&D) on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). A high priority for SFWST disposal R&D is to develop a disposal system modeling and analysis capability for evaluating disposal system performance for nuclear waste in geologic media. This report describes fiscal year (FY) 2021 advances of the PFLOTRAN Development group of the SFWST Campaign. The mission of this group is to develop a geologic disposal system modeling capability for nuclear waste that can be used to probabilistically assess the performance of generic disposal concepts. In FY 2021, development proceeded along three main thrusts: software infrastructure, code performance, and process model advancement. Software infrastructure improvements included implementing an Agile software development framework and making improvements to the QA Test Suite. Code performance improvements included development of advanced linear and nonlinear solvers as well as design of flexible smoothing algorithms for capillary pressure functions. Process modeling advancements included the addition of flexible thermal conductivity function definitions and refinement of multi-continuum reactive transport to support Sandia’s participation in DECOVALEX

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Investigating the Roughness and Advance Rate of the Weathering Interface (Final Report)

To understand geological systems that are important to our national well-being -- such as nuclear waste repositories or hydraulically fractured rocks -- requires the ability to make quantitative projections of the evolution of rock-water systems forward in time. A fundamental goal of much of our geochemical research was focused on development of numerical models of reactive transport to simulate the evolution of natural water-rock systems. The geochemical community has provided such models and they are rapidly being improved with field-model cross-testing. This project was especially impactful in field-model testing for well-constrained weathering systems to provide new conceptual understanding of how these systems function.

04 OIL SHALES AND TAR SANDS↗

Foundational Science to Accelerate Nuclear Energy Innovation [Brochure]

The foundational science gaps inhibiting the advancement of nuclear energy technologies are identified and tackled in five priority research opportunities. These opportunities pave the way to accelerate the development and ultimately the adoption of new nuclear energy systems. They include the fundamental aspects of ion-electron interactions; novel properties of next-generation coolants and solvents; interfacial dynamics, not only in solids, but in other aspects of nuclear reactors; novel operando and in-situ monitoring and sensing; and artificial intelligence to accelerate condensed phases discovery. Building on the foundation established by previous BES workshops, these opportunities encompass recent advances in fundamental knowledge and focus on the experimental and computational methods needed to resolve major technical challenges for nuclear energy technologies. Through developing fundamental scientific insight as well as pushing the frontiers of modeling complex systems and probing the operation of materials and chemical systems in extreme environments, research motivated by the priorities identified here will further develop the promise, potential, and utilization of nuclear energy for a clean energy future. The PROs are as follows: (1) Master complex electronic structures to tailor thermochemical reactivity, transport, and microstructural evolution; (2) Interrogate and direct the physics and chemistry underpinning next-generation coolants and solvents; (3) Elucidate and control the underlying physics and chemistry of interfaces in complex nuclear environments; (4) Bridge multi-fidelity multi-resolution experiments, computational modeling, and data science to control dynamic behavior; and (5) Harness artificial intelligence to design inherently resilient condensed phases.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Innovative Strategies for Long-Term Monitoring of Complex Groundwater Plumes at DOE’s Legacy Sites (Workshop Report)

Most remaining Department of Energy (DOE) sites will require extended periods of institutional control, especially at complex groundwater sites where attenuation-based strategies have been implemented to facilitate closure. The current practice of monitoring—obtaining and analyzing contaminant concentration in groundwater samples at numerous wells—will account for a large portion of the projected life-cycle at these DOE sites unless a new approach is adopted. State-of-the-art technologies are being developed, including in situ sensors, geophysics, radiation mapping, numerical modeling and AI/ML. These technologies can optimize monitoring strategies in space and time, provide spatially extensive information at vulnerable regions and/or provide more continuous monitoring at lower cost. As part of DOE’s Office of Environmental Management (DOE-EM’s) efforts to advance long-term monitoring systems, an in-person/virtual hybrid workshop was hosted by Savannah River National Laboratory (SRNL) on January 24 and 25, 2023, in Augusta, Georgia. Because DOE-EM’s complex sites will eventually be transferred to DOE’s Office of Legacy Management (DOE-LM), representatives of DOE-LM were important participants in the workshop. The purpose of the workshop was to identify challenges and opportunities for deploying advanced technologies for long-term monitoring at DOE sites. The key questions during the workshop were: 1) the regulatory acceptance of replacing a process that traditionally has used laboratory sampling and analysis of groundwater samples, and 2) the application of this strategy to the southwestern arid sites that include many of the remaining DOE-EM and DOE-LM complex groundwater plumes. Characteristics common to most arid sites present both limitations and opportunities for advanced technologies. DOE-EM has funded a National Laboratory team from SRNL, Lawrence Berkeley National Laboratory (LBNL), and Pacific Northwest National Laboratory (PNNL) to establish the overarching framework of long-term monitoring by systematically combining advanced hardware and software technologies. This project is titled “Advanced Long-Term Environmental Monitoring Systems (ALTEMIS)” and is sponsored by the DOE-EM Technology Development Program. The multi-laboratory team is currently developing and testing innovative monitoring strategies, including the use of in situ groundwater sensors, geophysics, drone/satellite-based remote sensing, reactive transport modeling, and artificial intelligence/machine learning (AI/ML). The project’s demonstration testbed is at the Savannah River Site (SRS) F-Area Seepage Basins, where a well-characterized complex groundwater plume composed of uranium and other radionuclides is in the latter stages of remediation. The workshop included more than 70 participants, presentations, a field visit to F-Area, breakout working groups, and large group discussion. Participants developed recommendations on five topics: in situ sensors, spatially integrative tools, challenges to regulatory acceptance, AI/ML strategies, and transitioning sites to DOE-LM.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Management and International Sorption Model Collaboration (M4SF-23LL010302062-NEA-TDB)

This progress report (Level 4 Milestone Number M4SF-23LL010302062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline International Collaborations Activity Number SF-23LL01030206. The activity is focused on our long-term commitment of engaging our partners in international nuclear waste repository research. This includes participation in the Nuclear Energy Agency Thermochemical Database (NEA-TDB) Project and development of methodologies for integrating US and international thermodynamic databases for use in SFWST Generic Disposal System Assessment (GDSA) efforts. A continuing focus for FY23 efforts has been to support the US participation in the NEA-TDB effort (Mavrik Zavarin replaced Cindy Atkins-Duffin on the NEA-TDB Management Board (MB) and Executive Group (EG)) and developing mechanisms for integration of NEA-TDB thermochemical data with LLNL’s SUPCRTNE thermodynamic database that supports the SFWST GDSA activities. This effort is coordinated with the Argillite work package SUPCRTNE database development efforts. The goal is to provide a downloadable database that will be hosted on a LLNL website which integrates NEA-TDB data into the LLNL SUPCRTNE database where appropriate. As part of our international activities, we continue our effort to integrate international sorption databases into L-SCIE (Zavarin et al., 2022b). We presented opportunities to include sorption in the next phase of NEA-TDB efforts at the April 2023 EG meeting in Paris. FY23 efforts focused on ensuring interoperable database development across multiple international database development activities. The overall goal is to produce an open source database that can be shared and integrated with multiple nuclear waste programs internationally and harness modern data science workflows and algorithms to incorporate these new approaches into reactive transport and performance assessment models. In collaboration with our Helmholtz Zentrum Dresden Rossendorf partners, we recently demonstrated the power of FAIR open source databases by fitting iron oxide (hydrous ferric oxide, goethite, hematite, and magnetite) protolysis constants to all available L-SCIE data. The results were submitted as a manuscript to J. Colloid Interface Science. This work will inform future metal sorption studies on a variety of iron oxides in order to discern the most appropriate acidity constants and surface complexation modeling constructs to account for pH-dependent mineral surface charge behavior. This work also explored automated surface complexation model development workflows in order to generate higher throughput model input files for a more facile incorporation into GDSA activities.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Assessment of Carbonated Brine Injection as Low-risk Strategy for Geologic Carbon Storage

The main objective of this early-phase research was to evaluate the techno-economic feasibility and risk associated with combined brine and CO 2 storage in SWD wells using brine dissolution in the North Dakota portion of the Williston Basin. Three simulation studies were conducted to investigate: (1) CO 2 phases at different conditions, (2) wellbore compatibility, and (3) long-term storage fate in reservoir. (1) A simple reservoir model and injection simulations were created using data to represent the BEST (brine extraction and storage test) site, an operational SWD facility located near Watford City, North Dakota. The pressure evolution caused by CO 2 comingled in produced water injectate in a layer cake reservoir was then modeled while tracking aqueous CO 2 throughout the project. The salinity of the injection water, the salinity of the reservoir brine, and the amount of dissolved CO 2 comingled in the injection water were varied. (2) A wellbore corrosion model was performed using the CO 2 concentrations selected based on the reservoir modeling to examine the carbonated produced water impact on wellbore. (3) Reactive transport modeling was conducted with the optimal CO 2 concentration for this injection site to study the rock-fluid interactions and CO 2 fate in the reservoir. Results suggest that CO 2 dissolved in produced water can be injected without appreciably increasing subsurface pressure or leakage risks. Pressure buildup was found to vary with salinity but not with CO 2 mass fraction. Simulation results show that lower CO 2 percent mass fraction leads to a higher amount of CO 2 that can be dissolved at a higher injection salinity. Furthermore, the long-term goal of dissolution trapping in a traditional carbon storage project is accomplished from the start, mitigating risks associated with potential migration of buoyant CO 2 , so long as the reservoir pressure and temperature are used to determine the maximum mass fraction of the dissolved CO 2 .

54 ENVIRONMENTAL SCIENCES↗

Advancing a Watershed Hydro-Biogeochemical Theory: Linking Water Travel Time and Reaction Rates Under Changing Climate

The major goal of the project is to answer the question how and to what degree does a warming climate alter hydrological functioning and (biogeochemical and chemical weathering) reaction rates at the watershed scale? In particular, how does hydrological functioning (water storage, flow paths, and travel time) change responding to a warming climate? What are the corresponding alterations in biogeochemical and chemical weathering rates at the watershed scale? What is the general watershed-scale reaction rate law that causally links reaction rates to metrics of hydrological functioning that are determined by external hydroclimatic conditions and internal watershed structure characteristics? To answer these questions, we have used field measurements and reactive transport modeling. We have found that: 1) stream chemistry has altered tremendously in warmer years; 2) In this water-limited environment, hydrology is the dominant driver for soil respiration and carbon lateral export at the watershed scale; 3) deeper carbon respiration plays an essential role in regulating the patterns of stream carbon in low and high flow conditions, and deeper groundwater will become increasingly important as warming intensifies. This indicates in mountain streams, a warming climate will modify not only the timing and magnitude of streamflow as expected, but also the chemistry and quality of stream water.

54 ENVIRONMENTAL SCIENCES↗

Carbonated Brine Injection Pilot Plan

This is a three-year effort to develop a plan for carbonated brine injection, with an end goal of a path for pilot scale implementation. Carbonated brine injection (CBI) strategy was planned for a potential pilot site through simulation study. Methods include geology model, reservoir modeling, wellbore materials compatibility and corrosion modeling, reactive transport modeling.

Xiong, Wei↗

Carbonated Brine Injection for a Pilot Site as a Low-Risk Geologic Carbon Storage Strategy: A Simulation Study

This technical report presents a preliminary study for CBI implementation in the Pena Creek pilot site in Dimmit County, Texas, targeting the Edwards Limestone Formation for SWD, in collaboration with NGL Energy Partners. The objective of this study is to find the conservative CO 2 molality for safe storage and potential risks for CBI at this pilot site. Geomodel was performed to get site-specific reservoir geology information. Reservoir modeling was performed to investigate dissolved CO 2 molality and pressure changes at relevant injection conditions. Wellbore corrosion and compatibility was discussed with corrosion modeling. Dissolved CO 2 long-term fate in the reservoir was examined with reactive transport modeling. This plan would set the scientific foundation as the initial step for future implementation in the field.

58 GEOSCIENCES↗

FY24: LEMMs: Long-term, Electrochemical Materials degradation Models

FY24 progress for LEMMs: Long-term, Electrochemical Materials degradation Models LDRD project are presented. Significant progress toward creating validated corrosion models was made in this FY paving success in future FY’s for success with battery model development and validation. Specifically, models for various forms of corrosion were probed for sensitivities showing a significant influence of reactive transport parameters for hydroxide species on the run time of the models. Further, cryo-genic time-of-flight secondary ion mass spectroscopy was utilized to map ions in a frozen corrosion droplet showing the precipitates/precipitate species near corroding locations. Additionally, a realistic corrosion droplet was created that accounted for evaporation and condensation coupled with corrosion. This pushes the boundary of corrosion modeling and will be validated in future FY’s.

36 MATERIALS SCIENCE↗

Genomes to ecosystem function: Targeting critical knowledge gaps in methanogenesis and translation to updated global biogeochemical models

Natural freshwater temperate wetland systems currently represent the largest natural source of atmospheric methane, but are relatively understudied using systems biology tools (e.g. meta-omics) compared to other high producing methane systems (e.g. peat, tropical, or reconstructed wetlands). Using field investigations at the NOAA operated sentinel site on Lake Erie, methane producing activities and responses to geochemical conditions will be determined along seasonal and spatial gradients (Objective 1). Here, a combination of high-throughput activity and gas measurements, combined with high-resolution systems biology and analytical methods, will provide in depth knowledge of the microbiological, chemical, and physical constraints on methane production in wetlands. Using laboratory microcosms, the formation of anoxic microsites and their capacity to facilitate methane production in wetland soils will be simulated (Objective 2). This objective will validate the findings from the field investigations, offering a more controlled environment for teasing out the role of different yet interrelated variables. Lastly, these field and laboratory data will be used for multi-scale, process-level evaluation of an ecosystem biogeochemical model that accommodates these newly identified processes and parameterizes representation of these processes along relevant environmental gradients (Objective 3).This research will identify multiple interacting geochemical, ecological, and metabolic constraints that are poorly understood, oversimplified, or missing in global biogeochemical methane models. This proposal targets the role of oxygen limitation on methane processes in soil domains, to improve reactive transport models of microbial carbon cycling across terrestrial-aquatic soils and generate data on nutrient cycling activities in Great Lake wetlands. This information could provide new insights into the microbial controllers of Lake Erie eutrophication.

59 BASIC BIOLOGICAL SCIENCES↗

Interactions between molecular-scale biogeochemical processes and hyporheic exchange for understanding coupled Fe-S-C cycling in iron-rich riparian wetlands (Final Technical Report)

Riparian wetlands are dynamic interfaces that exert strong control over water quality, contaminant mobility, and greenhouse gas emissions. These systems are characterized by hyporheic exchange between oxic surface water and anoxic groundwater, which generates steep redox gradients and promotes spatially and temporally variable microbial activity. Despite growing recognition of tightly coupled iron (Fe), sulfur (S), and carbon (C) cycling in these environments, the mechanisms governing these interactions—particularly under low-sulfate freshwater conditions—remain poorly constrained. This project developed a mechanistic understanding of how hydrologic variability and microbial processes interact to control Fe–S–C cycling in iron-rich riparian wetlands. Using a multi-scale and multi-method approach integrating field observations, geochemical and spectroscopic analyses, metagenomics, and reactive transport modeling, we demonstrate that “cryptic” sulfur cycling—rapid sulfur transformations involving intermediate-valence species—plays a dominant and previously underrecognized role in freshwater wetlands. These processes persist despite low sulfate concentrations and significantly influence iron reduction, carbon mineralization, and methane dynamics. The results show that cryptic sulfur cycling enhances dissolved Fe 2+ production, regulates methane concentrations, and is strongly controlled by climate-driven hydrologic fluxes. By linking hydroclimate, subsurface flow, and biogeochemical reactions, this work provides a predictive framework for understanding how wetland systems respond to environmental change, with direct implications for water quality and carbon cycling.

54 ENVIRONMENTAL SCIENCES↗

PFLOTRAN Development FY2021

The Spent Fuel & Waste Science and Technology (SFWST) Campaign of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Spent Fuel & Waste Disposition (SFWD) is conducting research and development (R&D) on geologic disposal of spent nuclear fuel (SNF) and high-level nuclear waste (HLW). A high priority for SFWST disposal R&D is to develop a disposal system modeling and analysis capability for valuating disposal system performance for nuclear waste in geologic media. This report describes fiscal year (FY) 2021 advances of the PFLOTRAN Development group of the SFWST Campaign. The mission of this group is to develop a geologic disposal system modeling capability for nuclear waste that can be used to probabilistically assess the performance of generic disposal concepts. In FY 2021, development proceeded along three main thrusts: software infrastructure, code performance, and process model advancement. Software infrastructure improvements included implementing an Agile software development framework and making improvements to the QA Test Suite. Code performance improvements included development of advanced linear and nonlinear solvers as well as design of flexible smoothing algorithms for capillary pressure functions. Process modeling advancements included the addition of flexible thermal conductivity function definitions and refinement of multi-continuum reactive transport to support Sandia’s participation in DECOVALEX. This report fulfills the GDSA PFLOTRAN Development Work Package Level 3 Milestone – PFLOTRAN Development, FY2021, M3SF-21SN010304072.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Using Homogenized Models to Explore the Effect of Fracture Densities on Weathering

Despite its importance, only a few researchers have incorporated the effects of fracturing into models of reactive transport for rock weathering. Here we explore 2D simulations that describe weathering under conditions of diffusive and advective transport within heterogeneous media consisting of rocky blocks and fractures. In our simulations, the Darcy velocities vary in space and time and depend on weathering processes within the rock matrix. We explore simulations with saturated and unsaturated flow for weathering bedrock that consists of blocks separated by inert or weathered material. The simulations show that a simplified homogenized model can approximate exact solutions for some of the simulated columns and hills and can allow exploration of coupling between flow and reaction in fractured rock. These hillslope simulations document that, even in the presence of 2D water flow, i) an increase in fracture density results in faster weathering advance rates; and ii) the water table locates deeper for a rock system that is weathered and fractured rather than weathered and unfractured. Some of these patterns have also been observed for natural systems. But these simulations also highlight how simplified models that do not use appropriate averaging of heterogeneities can be inaccurate in predicting weathering rate for natural systems. For example, if water flows both vertically and laterally through the vadose zone of a hill, then a prediction of the depth of regolith that is based on modeling strictly unidirectional downward infiltration will be unrealistically large. Likewise, if the fracture density observed near the land surface is used in a model to predict depth of weathering for a system where the fracture density decreases downward, the model will overestimate regolith depth. Learning how to develop accurately homogenized models could thus enable better conceptual models and predictions of weathering advance in natural systems.

58 GEOSCIENCES↗

Editorial: Sorption processes in nuclear waste management: data knowledge management and new methodologies for data acquisition/prediction

A fundamental approach to Nuclear Waste Repository research involves the collection of experimental data in a laboratory setting, development of empirical and/or mechanistic numerical models representing those observations, and application of these models (or Reduced Order Models) into reactive transport and performance assessment models as predictive tools for informing society of impacts and risks associated with nuclear waste repository scenarios (Stevens et al., 2020). Therefore, the assimilation and interpretation of experimental data must take advantage of both new data and the rich historical data available in the literature and apply novel modeling approaches to improve predictive tools, particularly from the standpoint of uncertainty quantification, for nuclear waste repository performance assessment (Zavarin et al., 2022).

sorption↗

A multirate mass transfer model to represent the interaction of multicomponent biogeochemical processes between surface water and hyporheic zones (SWAT-MRMT-R 1.0)

Abstract. Surface water quality along river corridors can be modulated by hyporheic zones (HZs) that are ubiquitous and biogeochemically active. Watershed management practices often ignore the potentially important role of HZs as a natural reactor. To investigate the effect of hydrological exchange and biogeochemical processes on the fate of nutrients in surface water and HZs, a novel model, SWAT-MRMT-R, was developed coupling the Soil and Water Assessment Tool (SWAT) watershed model and the reaction module from a flow and reactive transport code (PFLOTRAN). SWAT-MRMT-R simulates concurrent nonlinear multicomponent biogeochemical reactions in both the channel water and its surrounding HZs, connecting the channel water and HZs through hyporheic exchanges using multirate mass transfer (MRMT) representation. Within the model, HZs are conceptualized as transient storage zones with distinguished exchange rates and residence times. The biogeochemical processes within HZs are different from those in the channel water. Hyporheic exchanges are modeled as multiple first-order mass transfers between the channel water and HZs. As a numerical example, SWAT-MRMT-R is applied to the Hanford Reach of the Columbia River, a large river in the United States, focusing on nitrate dynamics in the channel water. Major nitrate contaminants entering the Hanford Reach include those from the legacy waste, irrigation return flows (irrigation water that is not consumed by crops and runs off as point sources to the stream), and groundwater seepage resulting from irrigated agriculture. A two-step reaction sequence for denitrification and an aerobic respiration reaction is assumed to represent the biogeochemical transformations taking place within the HZs. The spatially variable hyporheic exchange rates and residence times in this example are estimated with the basin-scale Networks with EXchange and Subsurface Storage (NEXSS) model. Our simulation results show that (1), given a residence time distribution, how the exchange fluxes to HZs are approximated when using MRMT can significantly change the amount of nitrate consumption in HZs through denitrification and (2) source locations of nitrate have a different impact on surface water quality due to the spatially variable hyporheic exchanges.

58 GEOSCIENCES↗

Modeling commercial-scale CO 2 storage in the gas hydrate stability zone with PFLOTRAN v6.0

Abstract. Safe and secure carbon dioxide (CO2) storage is likely to be critical for mitigating some of the most dangerous effects of climate change. In the last decade, there has been a significant increase in activity associated with reservoir characterization and site selection for large-scale CO2 storage projects across the globe. These prospective storage sites tend to be selected for their optimal structural, petrophysical, and geochemical trapping potential. However, it has also been suggested that storing CO2 in reservoirs within the CO2 hydrate stability zone (GHSZ), characterized by high pressures and low temperatures (e.g., Arctic or marine environments), could provide a natural thermodynamic barrier to gas leakage. Evaluating the prospect of commercial-scale, long-term storage of CO2 in the GHSZ requires reservoir-scale modeling capabilities designed to account for the unique physics and thermodynamics associated with these systems. We have developed the HYDRATE flow mode and the accompanying fully implicit parallel well model in the massively parallel subsurface flow and reactive transport simulator PFLOTRAN to model CO2 injection into the marine GHSZ. We have applied these capabilities to a set of CO2 injection scenarios designed to reveal the challenges and opportunities for commercial-scale CO2 storage in the GHSZ.

carbon storage↗