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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

An integrated experimental–modeling approach to identify key processes for carbon mineralization in fractured mafic and ultramafic rocks

Abstract Controlling atmospheric warming requires immediate reduction of carbon dioxide (CO2) emissions, as well as the active removal and sequestration of CO2 from current point sources. One promising proposed strategy to reduce atmospheric CO2 levels is geologic carbon sequestration (GCS), where CO2 is injected into the subsurface and reacts with the formation to precipitate carbonate minerals. Rapid mineralization has recently been reported for field tests in mafic and ultramafic rocks. However, unlike saline aquifers and depleted oil and gas reservoirs historically considered for GCS, these formations can have extremely low porosities and permeabilities, limiting storage volumes and reactive mineral surfaces to the preexisting fracture network. As a result, coupling between geochemical interactions and the fracture network evolution is a critical component of long-term, sustainable carbon storage. In this paper, we summarize recent advances in integrating experimental and modeling approaches to determine the first-order processes for carbon mineralization in a fractured mafic/ultramafic rock system. We observe the critical role of fracture aperture, flow, and surface characteristics in controlling the quantity, identity, and morphology of secondary precipitates and present where the influence of these factors can be reflected in newly developed thermo-hydro-mechanical–chemical models. Our findings provide a roadmap for future work on carbon mineralization, as we present the most important system components and key challenges that we are overcoming to enable GCS in mafic and ultramafic rocks.

58 GEOSCIENCES↗
DOE OSTI2024

Water foraging with dynamic roots in E3SM; The role of roots in terrestrial ecosystem memory on intermediate timescales (Final Technical Report)

Terrestrial ecosystems can show sustained responses to stress events that may last for years after the initial perturbation. This phenomenon is referred to as legacy or memory and it emerges from a set of ecosystem processes that are poorly captured by Earth System and Land Surface Models. Consequently, these models struggle to predict the impact that extreme climate events have on surface energy, carbon and hydrological exchange once a stressor such as drought has relaxed or in response to repeated exposure to stress. In this project, we set out to test how the addition of dynamic root profiles in land surface models impact the capacity for Earth System Models, such as the Department of Energy’s E3SM, to capture realistic legacy effects. Observations have shown that vegetation shifts their root profiles during stress events to forage for water and these altered root profiles may take years to relax back to the initial state. We hypothesized that the alteration of the belowground root structures may be a source of terrestrial ecosystem legacy that is missing from models. To test this idea we undertook three core activities. (1) We developed a global-scale analysis of the impact of dynamic roots on ecosystem legacy building from a recently developed dynamic root module. (2) We developed new root dynamics in the DOE’s Energy Land Model (ELM) that allowed not only root profiles to shift their profile but also simultaneously alter carbon allocation to fine root pools. We then tested the impact of these new dynamics with intensive sensitivity analysis at four long-term AmeriFlux sites. (3) We undertook detailed isotopic analysis of tree rings from these AmeriFlux sites to assess ecophysiological and ecohydrological legacy to stress events that can be used to benchmark the sensitivity experiments with ELM. From these core activities, we report the following key findings. Firstly, on a global scale, the addition of dynamic roots led to chronically water-stressed ecosystems recovering faster to climate stress while wetter ecosystem showed enhanced legacy. This is because across ecosystems, stress events were almost universally associated with water shortages that led to the development of deeper root profiles. These deeper root profiles proved beneficial for recovery from drought stress. While the root dynamics did not universally improve the modeled representation of legacy it showed complex transient dynamics that emerge from the addition of dynamic roots. Secondly, the sensitivity analysis illustrated long term shifts in rooting depths away from the prescribed default profile suggesting that initializing of root profiles could benefit from spin-up simulations that converge on locally optimized root profiles. In addition, by enabling dynamic allocation some of the sites predicted unrealistically low allocation to roots (and high allocation to leaves). While these changes did not dramatically alter modeled gross primary productivity, they illustrated that without more sophisticated root processes in models, there is little penalty to dramatically disinvest in roots. Thirdly, the isotopic analysis of tree rings showed highly distinct legacy responses across species and sites. For example, T. canadensis showed reduced transpiration the year after stress events illustrated by sustained elevated $\delta^{18}$O. In contrast, A saccharum displayed elevated $\delta^{13}$C associated with reduced stomatal conductance in response to the previous years’ stress event. These geochemical signatures of legacy were present despite tree growth returning to normal the year after the stress. The results show the importance of species-level dynamics in legacy that are absent in modeling that assumes common traits within plant functional types. In summary, the work here established new avenues to explore root dynamics in models while illustrating how additional root processes are needed before dynamic carbon allocation can be implemented. Lastly, this project provided mentorship to a postdoctoral fellow, training for an early career scientist and multiple undergraduate students recruited from a minority serving institution.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Quantifying pH buffering capacity in acidic, organic-rich Arctic soils: Measurable proxies and implications for soil carbon degradation

Dynamic pH change promoted by biogeochemical reactions in Arctic tundra soils can be a major control on the production and release of CO 2 and CH 4 , which contribute to rising global temperatures. Large quantities of soil organic matter (SOM) in these soils are susceptible to microbial decomposition, leading to pH changes during permafrost thaw. Soil pH buffering capacity (β) modulates the extent of pH change but has not been thoroughly studied and represented in predictive ecosystem scale biogeochemical models in Arctic tundra soils. In this study, we generated titration curves for 21 acidic tundra soils from three Arctic sites across northern Alaska, United States of America. Geochemical and hydrological soil properties were evaluated, and correlations with β were developed. Strong correlations between β and both gravimetric water content (Θ g ) (R 2 = 0.847, p < 0.001) and soil water retention (SWR) (R 2 = 0.849, p = 0.001) indicate that the ability of soil to retain water could be associated with its buffering properties. Correlations between β and soil organic carbon (SOC) and cation exchange capacity (CEC) were also explored, and relationships to SWR are discussed. These correlations were then used with existing soil databases reporting SOC, CEC, and SWR to estimate β across Alaska soils. We further demonstrated the quantitative relationships between β and the simulated rates of biogeochemical reactions and show that lower β leads to higher soil pH and more CH 4 production. Overall, our study provides simple proxies for β in Arctic soils and highlights the importance and implications of representing soil buffering in predictive models, thereby enabling quantitative coupling between pH dynamics associated with biogeochemical reactions. Integrating β into predictive models of Arctic biogeochemical cycling may reduce model uncertainty and further our understanding of permafrost SOM degradation accelerated by warming.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Surface Complexation/Ion Exchange Hybrid Model for Radionuclide Sorption to Clay Minerals (M4SF-23LL010301062)

This progress report (Level 4 Milestone Number M4SF-23LL010301062) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Argillite International Collaborations Activity Number SF-23LL01030106. The activity is focused on our long-term commitment to engaging our partners in international nuclear waste repository research. The focus of this milestone is the establishment of international collaborations for surface complexation modeling and the associated impacts of unlocking larger, community-based datasets. More specifically, we are developing a database framework for Spent Fuel and Waste and Science Technology (SFWST) that is aligned with the Helmholtz Zentrum Dresden Rossendorf (HZDR) sorption database development group in support of the database needs of the SFWST program. In our FY22 effort, we described a detailed analysis of U(VI) sorption to quartz through both traditional surface complexation modeling and through a hybrid ML framework. In FY23, effort was placed on publication of these results and expansion of the LLNL surface complexation and ion exchange database (L-SCIE) in order to assess mineral-based radionuclide retardation under a wider variety of geochemical conditions (e.g., ionic strength, varying electrolyte compositions). Efforts were initiated to expand L-SCIE to include radionuclide surface complexation and ion exchange to clays that are relevant to subsurface geochemical processes occurring at nuclear waste repositories. In particular, a large source of sorption data for clays resides at the Paul Scherrer Institute (PSI) (work primarily by Bradbury and Baeyens) and we initiated discussions on how to retrieve those data and apply FAIR principles to those datasets. In addition to L-SCIE development, two hybrid models that incorporate AI/ML were investigated and compared to discern the most promising approaches for accurate and precise estimations of radionuclide retardation. Key considerations for future model development include (1) the ability to reduce computational burden on determining retardation coefficients for PA and (2) the ability to quantify and predict radionuclide-mineral partitioning at a more efficient, rapid pace due to automated workflows. Upon the careful consideration of the most effective modeling approaches, we are identifying ways to implement these approaches into PA. Ultimately, the data science-based workflows will provide a major incentive for other institutions to adopt a FAIR-formatted, interoperable database. LLNL will play a key role in disseminating sorption data and acting as good data stewards by updating the database in a consistent format and assessing the quality of the newly assimilated data in an organized fashion. To this end, all data and workflows are open access and made available on the LLNL Seaborg research website (https://seaborg.llnl.gov/resources/geochemical-databases-modeling-codes).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Multistage nucleation pathway in LiF molten salt mirrors the crystal–melt interface structure

Despite over a century of studies, fundamental questions remain about the processes governing crystal nucleation from melts or solutions. Research over the past three decades has presented mounting evidence for kinetic pathways of crystal nucleation that are more complex than envisioned by the simplest forms of classical theory. Such observations have been presented for colloidal and elemental systems with covalent and metallic bonding. Despite the technological and geochemical importance of molten salts, similar studies for these ionically bonded systems are currently lacking. Here we develop a machine learning interatomic potential for a model ionic system: LiF. The potential features quantum-level accuracy for both liquid and multiple solid polymorphs over wide temperature and pressure ranges and accurately reproduces experimentally measured properties. Thanks to the efficiency of the potential, which enables microsecond-scale molecular dynamics simulations, induction times for nucleation of LiF solids from their melts are computed over a range of undercoolings. With the aid of a set of robust local order parameters established here, the simulations reveal that homogeneous crystal nucleation in undercooled melts preferentially initiates from liquid regions showing slow dynamics and high bond orientational order simultaneously, and the second-shell order of both precritical nuclei and the surface of postcritical nuclei is dominated by hexagonal close packing and body-centered cubic local structure, even though the nucleus core is dominated by face-centered cubic structure corresponding to the stable rocksalt crystal structure. Finally, we establish a connection between the crystallization pathway and the equilibrium crystal-melt interface structure.

Applied Physical Sciences↗
DOE OSTI2022

A Brief Overview of Reactive Transport Codes Used in CO 2 Applications

Reactive transport modelling consists of computational and numerical models that describe the coupled physical, chemical, mechanical, and biological processes interacting with each other over a broad range of spatial and temporal scales. This report reviews some of the reactive transport codes available in the literature for carbon dioxide (CO 2 ) applications and can assist the scientific community with the applicability of each code to solve a specific problem. Approaches implemented in these codes can be categorized in three groups: (i) continuum-scale, (ii) pore-scale, and (iii) hybrid-scale approaches. Theoretical foundations, numerical implementations, and application examples using the models are described. In the continuum approach, flow and transport are formulated in terms of a representative control volume of the medium and coupled with geochemical reactions. The medium is characterized by bulk parameters such as porosity, permeability, or reactive surface area. In the pore-scale approach, each point of space in the pore network is occupied by either a fluid or solid phase. The pore-scale approach requires an exact knowledge of the spatial and temporal phase distribution. In the hybrid-scale approach, media are described by multiple characteristic length-scales, with some regions using a pore-scale approach while others used a continuum approach.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2022

Stability of mineral-organic matter associations under varying biogeochemical conditions

It is well-recognized and documented in the literature that a considerable fraction of the soil organic matter (SOM) is associated with Fe-oxide minerals. Recent studies have also showed that the persistence of various classes of SOM may depend on soil Fe mineralogy. Other laboratory studies with model mineral-associated organic matter (MAOM) moieties, which were primarily focused on ferrihydrite, either coated or coprecipitated with natural organic matter (NOM), have suggested that the mineral phase transformation and adsorption-desorption of SOM is rather complex but appears to be largely controlled by the C/Fe ratio of the MAOM moiety and geochemical conditions. It is also clear from multiple recent studies that the nature or type of SOM (microbial vs. plant-derived) adsorbed on mineral surfaces and the rate and extent of SOM biodegradation depend on the type of mineral, and/or metal ions, that are associated with the SOM. Modeling studies that are primarily centered on achieving a better understanding of the effect of mineral type on SOM interactions with minerals and degradation are also reported. These studies have improved the understanding of the nature and stability of MAOM in soils of varying types and under different conditions, positioning researchers to better predict the properties and stabilities of organo-mineral associations in soils.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Emergent Behavior at the Calcite–Water Interface during Reactive Transport in a Simple Microfluidic Channel

Geochemical reactive transport processes in natural mineral-fluid systems may produce a wide array of emergent phenomena that are difficult to predict from basic principles and to reproduce in model systems. In this study, we present experimental results obtained from a simple microfluidic system with which we explored the consequences of reacting the calcite (104) cleavage surface with an acidic Pb-bearing solution (pH = 3.5, [Pb] total = 5 mM) as a function of flow rate. This system is relevant to passive remediation systems for Pb-rich acid mine drainage. We observed periodic banding in the amounts of Pb sorption at flow velocities ≥ 926 μm s -1 , where the band spacing was spatially correlated with the amount of calcite dissolution and the development of micropyramidal topography on the calcite (104) surface. The equivalent coverage of Pb deposited in these Pb-rich bands was at least several monolayers per unit cell, yet there was no evidence for precipitation of any secondary Pb phase implying incorporation of Pb within the near-surface calcite lattice. We also observed spatial variations in nucleation and growth of euhedral secondary Pb-carbonate minerals hydrocerusite and cerussite at flow rates ≤ 278 μm s -1 ,. These findings demonstrate potential for exploiting the rich phenomenology afforded by the interplay among transport phenomena and chemical kinetics in experimental systems designed to yield deeper insights into geochemical self-organization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Electrical Resistivity Tomography based monitoring of stress perturbations to optimize placement of high-precision strain meters

The Center for Understanding Subsurface Signals and Permeability is a new U.S. Department of Energy Earthshot Center focused on understanding and predicting the long-term evolution of permeability in enhanced geothermal systems. The center will use a highly instrumented testbed within the Sanford Underground Research Facility to conduct field scale experiments that elucidate and test capabilities to simulate geochemical-geomechanical interactions and permeability evolution. Here we demonstrate initial developments using previously collected electrical resistivity tomography (ERT) monitoring data with high-performance multi-physics modelling advancements to inform the optimal location of two new monitoring boreholes. Specifically, ERT monitoring data collected during shear stimulation testing shows marked responses to changes in stress during borehole pressurization. We demonstrate how the same response is being simulated, ultimately to train a machine-learning algorithm to estimate rock properties and enable enhanced prediction of stress and strain responses anticipated during future testing campaigns.

Stress, EGS, CUSSP, 3D Electrical Imaging↗
DOE OSTI2025

Single rhenium atoms on nanomagnetite: Probing the recharge process that controls the fate of rhenium in the environment

Understanding the redox transitions that control rhenium geochemistry is central to paleoredox and geochronology studies, as well as predicting the fate of chemically similar hazardous oxyanions in the environment such as pertechnetate. However, detailed mechanistic information regarding rhenium redox transitions in anoxic systems is scarce. Here, we performed a comprehensive laboratory study of rhenium redox transitions on variably oxidized magnetite nanoparticle surfaces. Through high-end spectroscopic and microscopic tools, we propose an abiotic transition pathway in which aqueous iron(II) ions in the presence of pure or preoxidized magnetite serve as an electron source to reduce rhenium(VII) to individual rhenium(IV) atoms or small polynuclear species on nanoparticle surfaces. Notably, iron(II) ions recharged preoxidized magnetite nanoparticles exhibit a maghemite core and a magnetite shell, challenging the traditional core-shell magnetite-maghemite model. This study provides a fundamental understanding of redox processes governing rhenium fate and transport in the environment and enables an improved basis for predicting its speciation in geochemical systems.

Science & Technology - Other Topics↗
DOE OSTI2025

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↗
DOE OSTI2022

Volcanology, Geochemistry, and Petrology Perspectives on Integrated, Coordinated, Open, Networked (ICON) Science

This article is composed of a commentary about the state of Integrated, Coordinated, Open, and Networked (ICON) principles in Volcanology, Geochemistry, and Petrology (VGP), and discussion on the opportunities and challenges of adopting them. VGP encompasses a broad field that addresses volcanic, magmatic, hydrothermal, geomicrobial systems; process investigations that span the physical, geochemical and biological realms, including planetary geology; and one that is extensively supported by state-of-the-art research facilities. We suggest that an open, inclusive, collaborative and evolving model of an international coordinated network is critical to answering the most pressing challenges in VGP. In this commentary piece, we begin to discuss the elements of, challenges to, and path forward in developing such a model. For this team, ICON means collaboration, equitable access to data for the entire scientific community, and forging of partnerships that potentially contribute to more innovative ways of coordinating and sharing research. It also means bringing more equity to science, by implementing effective measures which consider access to funding, analytical equipment, resources, and mentors. More importantly, ICON to us means having important conversations around what we value in the advancement of science, perhaps exploring outside the idea of meritocracy and evaluating what individual traits can contribute to science outside what has traditionally been considered the norm.

58 GEOSCIENCES↗
DOE OSTI2024

Carbon Mineralization in Fractured Mafic and Ultramafic Rocks: A Review

Mineral carbon storage in mafic and ultramafic rock masses has the potential to be an effective and permanent mechanism to reduce anthropogenic CO 2 . Several successful pilot-scale projects have been carried out in basaltic rock (e.g., CarbFix, Wallula), demonstrating the potential for rapid CO 2 sequestration. However, these tests have been limited to the injection of small quantities of CO 2 . Thus, the longevity and feasibility of long-term, large-scale mineralization operations to store the levels of CO 2 needed to address the present climate crisis is unknown. Moreover, CO 2 mineralization in ultramafic rocks, which tend to be more reactive but less permeable, has not yet been quantified. In these systems, fractures are expected to play a crucial role in the flow and reaction of CO 2 within the rock mass and will influence the CO 2 storage potential of the system. Therefore, consideration of fractures is imperative to the prediction of CO 2 mineralization at a specific storage site. In this review, we highlight key takeaways, successes, and shortcomings of CO 2 mineralization pilot tests that have been completed and are currently underway. Laboratory experiments, directed toward understanding the complex geochemical and geomechanical reactions that occur during CO 2 mineralization in fractures, are also discussed. Experimental studies and their applicability to field sites are limited in time and scale. Many modeling techniques can be applied to bridge these limitations. We highlight current modeling advances and their potential applications for predicting CO 2 mineralization in mafic and ultramafic rocks.

25 ENERGY STORAGE↗
DOE OSTI2026

Innovations in underground hydrogen storage with multiphysics simulations, optimization, and monitoring: A review

Underground Hydrogen Storage (UHS) is a promising solution for large-scale energy storage and a critical component in advancing low-carbon energy system. Ensuring the safety and efficiency of UHS necessitates a comprehensive understanding of multiphysical interactions driven by cyclic pore fluid pressure fluctuations and coupled physicochemical processes. Here, this review examines the key geomechanical responses in UHS, including rock property variations under cyclic loading, fracture evolution and propagation, reservoir stress sensitivity, and fault stability. It also explores the impact of geochemical and microbial reactions on geomechanical characteristics. We provide an in-depth analysis of Thermal-Hydraulic-Mechanical-Chemical (THMC) coupled numerical simulations, highlighting their potential for future multi-scale modeling. Limitations of current machine learning (ML) approaches in addressing UHS challenges are highlighted, emphasizing the need for innovative ML-based methodologies. Operational strategies for hydrogen injection and production are reviewed, focusing on safety, efficiency, and economic viability. The necessity for multi-objective optimization (MOO) to balance storage efficiency, risk mitigation, and cost-effectiveness is also discussed. Current monitoring technologies are evaluated to ensure safe and efficient UHS operations. Finally, this review identifies critical knowledge gaps and underscores the importance of advancing geomechanical understanding under multiphysics-coupling. We highlight the need for ML-driven multiphysics theories, enhanced modeling techniques, and robust optimization strategies to improve UHS performance. This study serves as a comprehensive reference for future research and the large-scale implementation of UHS systems.

25 ENERGY STORAGE↗
DOE OSTI2023

A compendium of bacterial and archaeal single-cell amplified genomes from oxygen deficient marine waters

Oxygen-deficient marine waters referred to as oxygen minimum zones (OMZs) or anoxic marine zones (AMZs) are common oceanographic features. They host both cosmopolitan and endemic microorganisms adapted to low oxygen conditions. Microbial metabolic interactions within OMZs and AMZs drive coupled biogeochemical cycles resulting in nitrogen loss and climate active trace gas production and consumption. Global warming is causing oxygen-deficient waters to expand and intensify. Therefore, studies focused on microbial communities inhabiting oxygen-deficient regions are necessary to both monitor and model the impacts of climate change on marine ecosystem functions and services. Here we present a compendium of 5,129 single-cell amplified genomes (SAGs) from marine environments encompassing representative OMZ and AMZ geochemical profiles. Of these, 3,570 SAGs have been sequenced to different levels of completion, providing a strain-resolved perspective on the genomic content and potential metabolic interactions within OMZ and AMZ microbiomes. Hierarchical clustering confirmed that samples from similar oxygen concentrations and geographic regions also had analogous taxonomic compositions, providing a coherent framework for comparative community analysis.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Development of Scalable Reactive Transport Framework for PFAS

Research on PFAS chemicals is extensive and covers all aspects, including analytical quantification, determination of properties, toxicology, ex situ treatment, and in situ remediation. PFAS chemicals are very stable and thus persistent/recalcitrant in the environment. Although there are many unknowns about PFAS chemicals, degradation pathways, reaction rates, etc., many different sorption, oxidation, reduction, biological, and innovative treatment approaches are being developed. Sorption with activated carbon is currently the only fully available in situ treatment technology for PFAS-impacted groundwater. Given the wide array of PFAS chemicals and transformation products, remediation may need multi-step treatment trains to fully address the PFAS contamination. The work here provides kinetic reaction modules that represent an initial cut at functionality representing PFAS migration and reaction in groundwater aquifer flow and transport models. One reaction kinetics module provides a method to model kinetically limited adsorption using a mass transfer model. The second reaction module represents biological transformation of 8:2 FTOH and daughter species, illustrating how a complex reaction pathway network can be represented. Both reaction modules allow for spatially variable parameter values so that a variety of remediation approaches (e.g., a PRB or volumetric treatment or variations in geochemical conditions) can be simulated. The intent with these PFAS reaction modules is to provide tools for practitioners to aid in the selection, design, and assessment of potential in situ PFAS remediation strategies. It is anticipated that, as PFAS remediation technologies and scientific understanding advances, these modules would be refined or replaced to match new knowledge.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Can we safely go to 200 °C? An integrated approach to assessing impacts to the engineered barrier system in a high-temperature repository

Abstract. This presentation gives on overview of the complex thermo-hydro-mechanical-chemical (THMC) processes occurring during the disposal of heat-producing high-level radioactive waste in geologic repositories. A specific focus is on the role of compacted bentonite, which is commonly used as an engineered backfill material for emplacement tunnels because of its low permeability, high swelling pressure, and radionuclide retention capacity. Laboratory and field tests integrated with THMC modeling have provided an effective way to deepen our understanding of temperature-related perturbations in the engineered barrier system; however, most of this work has been conducted for maximum temperatures around 100 ∘C. In contrast, some international disposal programs have recently started investigations to understand whether local temperatures in the bentonite of up to 200 ∘C could be tolerated with no significant changes to safety relevant properties. Raising the maximum temperature is attractive for economical and safety reasons but faces the challenge of exposing the bentonite to significant temperature increases. Strong thermal gradients may induce complex moisture transport processes while geochemical processes, such as cementation and perhaps also illitization effects may occur, all of which could strongly affect the bentonite and near-field rock properties. Here, we present initial investigations of repository behavior exposed to strongly elevated temperatures. We will start discussing our current knowledge base for temperature effects in repositories exposed to a maximum temperature of 100 ∘C, based on data and related modeling analysis from a large heater experiment conducted for over 18 years in the Grimsel Test Site in Switzerland. We then show results from coupled THMC simulations of a nuclear waste repository in a clay formation exposed to a maximum temperature of 200 ∘C. We also explore preliminary data from a bench-scale laboratory mock-up experiment, which was designed to represent the strong THMC gradients occurring in a “hot” repository, and we finally touch on a full-scale field heater test to be conducted soon in the Grimsel Test Site underground research laboratory in Switzerland (referred to as HotBENT).

Birkholzer, Jens T. (ORCID:0000000279891912)↗
DOE OSTI2023

Noble gas insights into early impact delivery and volcanic outgassing to Earth's atmosphere: A limited role for the continental crust

Earth's atmosphere, crust and mantle have evolved together through continuous geochemical exchange throughout Earth's history. Constraints on the transport of volatile elements and compounds between these reservoirs are crucial for understanding how Earth could have stayed habitable for extended periods of time. In this work, we present a new forward model of He, Ne and Ar in the mantle, crust and atmosphere. We explore concentrations of noble gases at the end of accretion, bulk silicate Earth K/U ratios, crustal growth scenarios, and upper mantle processing rates throughout Earth's history. We search for parameter combinations that simultaneously satisfy observational constraints on present-day mantle 4 He/ 3 He and 40 Ar/ 36 Ar (sensitive to mantle outgassing and continental crust growth, which depletes the mantle of U, Th and K), atmospheric 20 Ne/ 22 Ne (which tracks the mix of outgassed vs. delivered Ne in the atmosphere), and atmospheric 40 Ar/ 36 Ar in the past and today (sensitive to volatile delivery, mantle outgassing and crustal growth). Leveraging this intertwined set of noble gas abundances and isotopic compositions yields new constraints on initial noble gas abundances in the mantle and on the proportions of atmospheric volatiles originating from delivery by impact degassing, mantle outgassing, and degassing of the continental crust. We find that atmospheric Ar isotopic evolution is primarily sensitive to the mantle processing rate history; the atmospheric Ar isotopic record should therefore not be used to reconstruct continental crust growth, but instead provides valuable insights into mantle processing rates. Our model predicts a measurably low 20 Ne/ 22 Ne ratio of ~9.7 in Archean atmospheric samples. Most of atmospheric primordial 36 Ar was directly delivered by chondritic bodies and not transferred to the atmosphere during an intense early episode of mantle outgassing. Nitrogen delivered by impact degassing could account for the present-day atmospheric nitrogen inventory.

58 GEOSCIENCES↗