Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Geochemical Processes”

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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Skin factor and potential formation damage from chemical and mechanical processes in a naturally fractured carbonate aquifer with implications to CO 2 sequestration

Here, in this study, we investigate formation damage due to acidization and water injection tests into the naturally fractured carbonate Middle Duperow Formation at Kevin Dome, Montana, potentially diminishing the chance of a future successful Geological Carbon Sequestration (GCS) project. Multiple well-test analytical models, correlated with core description and lithology data, are used to determine flow behavior and communication between the water injection interval and surrounding formations. An improved three-dimensional (3D) geologic model with dual-continuum matrix and fracture properties is constructed based on most recent seismic, core, and water sample measurements. Brine injection is simulated to verify the interpretation from the analytical models, followed by CO 2 injection simulation. Geochemical calculations are performed to understand the in-situ processes that led to formation damage. Our findings suggest: (1) there are two possible scenarios that could lead to a positive total effective skin factor and permeability decline: partial penetration and formation damage; (2) analytical models indicate a positive total skin factor, contradicting results of a previous study suggesting that the well was mildly stimulated; (3) numerical simulation supports the formation damage hypothesis by matching the pressure buildup observed during the latter two brine injection tests; (4) several mechanical and chemical processes may have occurred during injection to clog the matrix/fracture system: anhydrite fines migration and/or calcite precipitation. We then make preventative suggestions for future GCS projects into carbonate reservoirs and remediation recommendations for GCS operation at the Kevin Dome.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

AquaMEND: Reconciling multiple impacts of salinization on soil carbon biogeochemistry

Soil salinization, exacerbated by climate change, poses a global threat to coastal ecosystem function and soil quality. Salinity influences carbon cycling through direct effects on microbial activity and indirect alterations to soil physicochemical properties including cation exchange, pH, and soil organic carbon availability. Current models inadequately represent these complexities, relying on linear reduction functions that overlook specific physicochemical changes induced by salinity. To address this gap, we propose an integrated model framework, AquaMEND, that combines microbial-explicit carbon decomposition and geochemical models. This model allows cation exchange and surface complexation processes to capture solute chemistry and nutrient availability in soils upon saltwater intrusion. Using response functions that capture salinity impacts on both salt-sensitive and salt-resistant microbial processes, AquaMEND simulates how the abiotic and biotic mechanisms work individually and collectively to regulate organic and inorganic pools and fluxes. Here, the parallel structure of aqueous and non-aqueous phases, together with microbial functions, result in a versatile model for solving dynamic coupling of organics, minerals and microbes under various environmental settings.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

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↗
DOE OSTI2020

Tracking natural CO 2 migration through a sandstone aquifer using Sr, U and C isotopes: Chimayó, New Mexico, USA

The geochemical and isotopic characteristics of groundwaters in Chimayó, New Mexico, reflect processes that affect water quality in the Tesuque Aquifer, which overlies a leaking natural CO 2 source in a structurally complex region. In this study, select isotopes (δ 13 C, 87 Sr/ 86 Sr, 234 U/ 238 U) are applied to groundwaters to better understand CO 2 transport mechanisms and related water-rock interactions that impact Chimayó groundwater. Carbon stable isotope ratios of dissolved inorganic carbon (DIC; δ 13 CDIC = -15.10‰ to 4.50‰) identify a distinct source of upward-migrating CO 2 that interacts with the groundwater. Additionally, groundwater 87 Sr/ 86 Sr compositions (0.7098 to 0.7154) reflect intrusion of varying amounts of saline water associated with the high CO 2 source, while 234 U/ 238 U ratios corroborate presence of deep groundwater and suggest impacts from distinctive natural uranium sources are affecting groundwater. Previous work proposed two CO 2 transport mechanisms at the site: (1) dissolved in deep brine that underlies the aquifer and (2) in the gas phase; this study uses isotope mixing models to identify wells that are affected by these CO 2 transport mechanisms and demonstrates that both transport mechanisms are associated with impaired groundwaters. Overall, this study demonstrates that applying multiple isotope systems (δ 13 CDIC, 87 Sr/ 86 Sr, 234 U/ 238 U) is a dynamic tool for identifying and measuring the impact of CO 2 leakage from a sequestration site.

58 GEOSCIENCES↗
DOE OSTI2020

Pump-and-Treat Impacts on Aquifer Conditions and the Development of System-Wide Performance Strategies - 20377

The pump-and-treat (P and T) system on the Hanford Site's Central Plateau currently treats multiple contaminants within the 200-ZP-1 operable unit, including nitrate through its biological treatment processes. Although it was initially designed to support the 200-ZP-1 Remedial Action Objectives, the P and T system has evolved in use to address contaminants from other regions of the aquifer as well. The P and T influents are biogeochemically distinct, treating groundwaters with elevated concentrations of cyanide, uranium, technetium-99, and nitrate. Given the varying geochemical signatures from current and potential future sources, operational conditions, and amendments considered for treatment processes, there is a need to identify the impacts that the P and T effluent has on the aquifer, and how the aquifer affects P and T performance. To this end, laboratory efforts have focused on characterizing P and T effluent and its biogeochemical effects on the sediments through a series repacked column experiments. The P and T effluent is rich in particulate matter. A systematic inspection of this particulate matter in the P and T effluent showed significant levels of manganese/iron oxides, calcite crystals, relatively large organic matter molecules, and biomass. Therefore, the column experiments were designed and conducted for four different treatment systems: artificial groundwater, filtered P and T effluent, non-filtered P and T effluent, and chlorinated P and T effluent. Different levels of microbiologically- and geochemically-induced changes in the columns occurred and modified the flow systems. For example, physical filtration occurred in the sediments where the particulate material had accumulated in the top portion of the column. Reactive transport modeling of the laboratory experiments is being carried out so that the reaction network can be extrapolated to the field scale. These simulations will provide predictive evaluations of system performance based on P and T operational changes and aquifer mass loading and capacity estimates. This information can be used to address combined subsurface and operational challenges, such as the need for frequent well redevelopment to maintain injection capacity. This information also provides the technical basis for decisions related to the P and T system operations that support remedy optimization efforts and short- and long-term remedy decisions related to multiple operable units on the Hanford Site Central Plateau. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Elucidating the temperature and density dependence of silver chloride hydration numbers in high-temperature water vapor: A first-principles molecular simulation study

Hydration numbers of metal complexes in low-density aqueous solutions are required for developing geochemical models for ore-forming metals and for designing supercritical desalination processes. In this study, we investigate the temperature and density dependence of the hydration numbers of silver chloride at 623 K, 673 K, and 713 K and densities of 10–100 kg/m 3 . Experimental estimates of the hydration number in the literature for AgCl at these conditions are inconclusive and possibly contradictory as to the temperature and density dependence. First-principles molecular simulation presents an attractive alternative to experimental measurements. Specifically, recent work shows that machine-learning-accelerated nested Monte Carlo simulations provide reliable estimates for the hydration numbers of CuCl at 623 K from 10 to 100 kg/m 3 . Using the same technique, we find a monotonic temperature dependence, with the hydration number decreasing slightly with increasing temperature. In addition, the simulation-predicted hydration numbers steadily increase with increasing density. These temperature and density trends are in agreement with certain experimental data sets. Therefore, this work demonstrates how first-principles Monte Carlo simulations assist in resolving discrepancies between experimental data sets. Our simulation results also correctly predict that the hydration number, and thus also the solubility, of AgCl is lower than that of CuCl under the same conditions. Furthermore, the bond length and angle formed between the water complex and AgCl differ from those for CuCl, consistent with the lower solubility of AgCl.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Zn speciation and fate in soils and sediments along the ground transportation route of Zn ore to a smelter

We discuss assessment of Zn toxicity/mobility based on its speciation and transformations in soils as critical for maintaining human and ecosystem health. Zn-concentrate (56% Zn as ZnS, sphalerite) has been imported through a seaport and transported to a Zn-smelter for several decades, and smelting processes resulted in aerial deposition of Zn and sulfuric acids in two geochemically distinct territories around the smelter (mountain-slope and riverside). XAFS analysis showed that the mountain-slope soils contained franklinite (ZnFe 2 O 4 ) and amorphous (e.g., sorbed) species of Zn(II), whereas the riverside sediments contained predominantly hydrozincite [Zn 5 (OH) 6 (CO 3 ) 2 ], sphalerite, and franklinite. The mountain-slope soils had low pH and moderate levels of total Zn (~1,514 ppm), whereas the riverside sediments had neutral pH and higher total Zn (12,363 ppm). The absence of sphalerite and the predominance of franklinite in the mountain-slope soils are attributed to the susceptibility of sphalerite and the resistance of franklinite to dissolution at acidic pH. These results are compared to previous Zn analyses along the transportation routes, which showed that Zn-concentrate spilled along the roadside in dust and soils underwent transformation to various O-coordinated Zn species. Overall, Zn-concentrate dispersed in soils and sediments during transportation and smelting transforms into Zn phases of diverse stability and bioavailability during long-term weathering.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Environmental cell for in situ X-ray synchrotron micro-CT imaging with simultaneous acoustic measurements

Synchrotron radiation provides the necessary spatial and temporal resolution for non-invasive operando studies of dynamic processes under complex environmental conditions. Here a new environmental cell for simultaneous in situ dynamic X-ray imaging and measuring acoustic properties of geological samples is presented. The primary purpose of this cell is to study gas-hydrate formation in porous geo-materials and its influence on their acoustic properties. The cell is designed for cylindrical samples of 9 mm in diameter, confining and pore pressures up to 12 MPa, and temperatures from –20°C to room temperature. The cell is portable and can be easily assembled and operated at different X-ray sources. This cell enables a wide range of experiments studying physical/chemical processes in the Earth subsurface that change the mechanical properties of rocks (geochemical reactions, phase transitions, etc.).

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Biogeochemistry simulations for the Salt Marsh Accretion Response to Temperature eXperiment (SMARTX)

Coastal ecosystems have been largely ignored in Earth system models but are important zones for carbon and nutrient processing. Interactions between water, microbes, soil, sediments, and vegetation are important for mechanistic representation of coastal processes and ecosystem function. To investigate the role of these feedbacks, we used a reactive transport model (PFLOTRAN) that has the capability to be connected to the Energy Exascale Earth System Model (E3SM). PFLOTRAN was used to incorporate redox reactions and track chemical species important for coastal ecosystems as well as define simple representations of vegetation dynamics. Our goal was to incorporate oxygen flux, salinity, pH, sulfur cycling, and methane production along with plant-mediated transport of gases and tidal flux. Using porewater profile and incubation data for model calibration and evaluation, we were able to create depth-resolved biogeochemical soil profiles for saltmarsh habitat and use this updated representation to simulate direct and indirect effects of elevated CO2 and temperature on subsurface biogeochemical cycling. We found that simply changing the partial pressure of CO2 or increasing temperature in the model did not fully reproduce observed changes in the porewater profile, but the inclusion of plant or microbial responses to CO2 and temperature manipulations was more accurate in representing porewater concentrations. This indicates the importance of characterizing tightly coupled vegetation-subsurface processes for developing predictive understanding and the need for measurement of plant-soil interactions on the same time scale to understand how hotspots or moments are generated.Included in this data package are PFLOTRAN input (PFLOTRAN input files and chemical database) files for simulating single column biogeochemistry, root, and tide interactions at the Global Change Research Wetland (Kirkpatrick Marsh; Edgewater, MD). The biogeochemical network includes soil organic matter decomposition, nitrogen, iron, and sulfur cycling, and methanogenesis. Reduced species can be oxidized and plant processes include oxygen and nutrient priming, methane release, and nutrient uptake.Inputs:TAI_database.dat - geochemical database for reactions, more information on database structure and variables can be found here https://www.pflotran.org/documentation/user_guide/cards/pages/geochemical_database.htmlswamp.in - input file for biogeochemical network in PFLOTRANswamp_eCO2.in - input file for biogeochemical network in PFLOTRAN with input gas partial pressures/concentrations adjusted for elevated CO2 treatmentsOutputs:swamp_obs_0.tec - hourly porewater concentrations from from multiple depths in the soil columnswamp_eCO2_obs_0.tec - hourly porewater concentrations from multiple depths in the soil column for elevated CO2 treatmentsPFLOTRAN code access: https://github.com/fmyuan/pflotran-elm-interface.git

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

A combined experimental and modelling study of granite hydrothermal alteration

Geochemical reactions can induce significant changes of rock reservoir porosity and permeability via mineral dissolution and precipitation processes, affecting the long-term fluid behaviour within various geological systems. Here, the understanding and quantification of these reactions rely on field and experimental studies and on the predictions of reactive transport models. The present study was aimed at assessing the extent to which current geochemical models integrating available mineral dissolution/precipitation rate equations can reproduce the experimental data obtained from 4 to 17-day long hydrothermal alteration experiments of a muscovite-biotite granite and, thus, help provide an accurate description of the evolution of geothermal systems within granitic reservoirs. The experiments were conducted at a constant temperature of 180 °C and over an aqueous fluid pH range of 2 to 8.5, using both mixed-flow and static batch reactors. Modelled major element (K, Al, Si, Ca, and Mg) concentrations were generally in satisfactory agreement with the corresponding measured elemental fluxes – the differences between modelled and experimental values were generally within a factor of 5 – and the predicted identity and mass of formed secondary phases were consistent with the microscopic observations of the reacted solids. However, larger differences between measured and modelled element concentrations were observed when significant amounts of secondary phases formed, notably at pH 2 to 3, and for longer-term batch experiments. Much of this concentration difference stems from the underestimation of the amounts of Al-phases formed at acid to near-neutral pH. Although an idealized rock composition was considered, the observed mismatch between model calculations and experimental data can be attributed to inadequate mineral precipitation reaction rates and a poor description of reactive surface areas in existing geochemical modelling codes. More accurate quantification of precipitation kinetics, including nucleation and growth, and improved descriptions of the temporal change of mineral surface area would enhance the predictive capabilities of reactive transport models and benefit, particularly, the efforts aimed at increasing the sustainability of EGS reservoirs.

58 GEOSCIENCES↗
DOE OSTI2020

Conceptual Model Update of Mercury Sources and Flux at Y-12 and Upper East Fork Poplar Creek, Oak Ridge,Tennessee

The interactions between the key processes that control the fate and transport of mercury (Hg) in the sediments, groundwater, and stream water within the Y-12 National Security Complex (Y-12) in Oak Ridge, Tennessee are complex, and many aspects are not well understood. In contaminated environments such as Y-12, conceptual models are frequently developed to aid in visualizing and understanding the dynamic nature of the hydrologic, geochemical, and physical environment. These conceptual models integrate data in an internally consistent manner to understand processes that control the fate and transport of contaminants. Over the past few decades of environmental investigation at Y-12, a number of conceptual models have been developed to identify and define various technical processes at various scales. The main purpose of the activities described in this report is to update the 2011 conceptual model for Upper East Fork Poplar Creek using the most recent Hg concentration and flux data and informed scientific interpretation. Emphasis was placed on improving the previous model by implementing a more detailed spatial and temporal approach to visualize transport pathways in the watershed and trends in flux and concentration over time, and to compare baseflow and stormflow system dynamics. Detailed descriptions of historical and current Hg sources and transport pathways are also provided for the east and west ends of the facility. This conceptual model will allow the US Department of Energy to evaluate past and present remedial activities and provide a strong technical basis for prioritizing and optimizing remedial responses in a cost-effective and efficient manner. Twenty years ago, Hg flux from Outfall (OF) 200 at the headwaters of East Fork Poplar Creek represented approximately 20% of the overall flux leaving Y-12. By the time of the 2011 conceptual model report, that percentage had increased to 70%–80%. Flux estimates compiled for this report using data from 2009 to 2018 show that OF200 accounted for roughly 60% of the flux leaving Y-12. The relative role of the four storm drain conduits to OF200 appeared similar to 2011, with OF163 being the greatest contributor to downstream flux. An increase in Hg concentrations and flux occurred throughout and downstream of west end storm drains in 2011 in response to a storm drain cleanout. Leading up to the 2011 storm drain cleanout, annual baseflow flux was higher at OF200A6 than at Station 17. From 2011 to 2018, the trend reversed with concentrations and flux being higher at Station 17 than at OF200A6. A spike in concentrations occurred in July 2018, potentially due to a one-time influx of Hg that occurred during COLEX decontamination and decommissioning activities at Y-12. This report includes recommendations for improving our conceptual understanding of Hg sources, transport pathways, and flux at Y-12. Important recommendations include further evaluation of transport pathways, concurrent measurement of Hg concentration and flux under baseflow and stormflow conditions at multiple sites, and research to understand the connections among periphyton and methylmercury concentration, bioavailability, and bioaccumulation. Ongoing facility decontamination and decommissioning efforts, site characterization, remedial actions, and research are facilitating the collection of new Hg data at Y-12. The conceptual model update provided herein takes advantage of the extensive recent Hg sampling to provide an updated assessment of Hg mass balance and support a refined understanding of Hg behavior at or near Y-12. This assessment should assist in future environmental management decisions and in mitigating the impacts of Hg on the surrounding environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Data and scripts associated with “Riverine dissolved organic matter transformations increase with watershed area, water residence time, and Damköhler numbers in nested watersheds” (v2)

This data package is associated with the publication “Riverine dissolved organic matter transformations increase with watershed area, water residence time, and Damköhler numbers in nested watersheds” submitted to Biogeochemistry by Ryan et al., 2024 (DOI: https://doi.org/10.1007/s10533-024-01169-5). This study aims to investigate fundamental and transferable drivers of dissolved organic matter (DOM) diversity across five nested watersheds within the contiguous United States. DOM diversity was explored using ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). The samples and the unprocessed FTICR-MS data used in this study are publicly available on the Environmental System Science Data Infrastructure for a Virtual Ecosystem (ESS-DIVE) data repository (see DOIs below). The data for the Willamette, Gunnison, Connecticut, and Deschutes basins were collected as part of a collaboration between the Watershed Rules of Life (WROL) project and Worldwide Hydrobiogeochemistry Observation Network for Dynamic River Systems (WHONDRS). The data for the Yakima River basin (YRB) was collected by the PNNL River Corridor SFA. The raw, unprocessed FTICR-MS data with additional (meta)data can be found at doi:10.15485/1895159 for WROL samples and doi:10.15485/1898912 for YRB samples. This data package contains the processed data used in the associated manuscript. This package also contains ancillary geospatial, hydrological, and geochemical information that supports the interpretation of the FTICR-MS data within Ryan et al., 2024. This data package is associated with the GitHub repository found at https://github.com/WHONDRS-Hub/rcsfa-RC4-WROL-YRB_DOM_Diversity. This data package was originally published August 2024. It was updated January 2025 (modified files). See the change history in the readme more details. At the directory level, the data package is comprised of three folders: (1) data, (2) output, and (3) src; and five additional files including the data dictionary (file ending in "_dd.csv”) and file-level metadata (file ending in “_flmd.csv”). The “src” folder contains the scripts used to process the FTICR data, conduct the analyses, and produce the manuscript figures. The inputs for these scripts are in the “data” folder and the returned outputs in the “output” folder. Inputs include temporal and spatial metadata associated with the sampling efforts, processed FTICR data, and total and normalized putative biochemical transformations per sample. Outputs include cleaned and combined data presented as tables, descriptive statistics, and plots. The file-level metadata file lists all files contained in this data package and descriptions for each. The data dictionary describes the units and definitions for each tabular data column or row header.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Microtopography Matters: Belowground CH 4 Cycling Regulated by Differing Microbial Processes in Peatland Hummocks and Lawns

Water table depth and vegetation are key controls of methane (CH 4 ) emissions from peatlands. Microtopography integrates these factors into features called microforms. Microforms often differ in CH 4 emissions, but microform-dependent patterns of belowground CH 4 cycling remain less clearly resolved. Here, to investigate the impact of microtopography on belowground CH 4 cycling, we characterized depth profiles of the community composition and activity of CH 4 -cycling microbes using 16S rRNA amplicon sequencing, incubations, and measurements of porewater CH 4 concentration and isotopic composition from hummocks and lawns at Sallie's Fen in NH, USA. Geochemical proxies of methanogenesis and methanotrophy indicated that microforms differ in dominant microbial CH 4 cycling processes. Hummocks, where water table depth is lower, had higher porewater redox potential (Eh) and higher porewater δ 13 C-CH 4 values in the upper 30 cm than lawns, where water table depth is closer to the peat surface. Porewater δ 13 C-CH 4 and δD-CH 3 D values were highest at the surface of hummocks where the ratio of methanotrophs to methanogens was also greatest. These results suggest that belowground CH 4 cycling in hummocks is more strongly regulated by methanotrophy, while in lawns methanogenesis is more dominant. We also investigated controls of porewater CH 4 chemistry. The ratio of the relative abundance of methanotrophs to methanogens was the strongest predictor of porewater CH 4 concentration and δ 13 C-CH 4 , while vegetation composition had minimal influence. As microbial community composition was strongly influenced by redox conditions but not vegetation, we conclude that water table depth is a stronger control of belowground CH 4 cycling across microforms than vegetation.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Impact of oxidation and carbonation on the release rates of iodine, selenium, technetium, and nitrogen from a cementitious waste form

Evaluation of the long-term retention mechanisms and potential release rates for the primary constituents of potential concern (COPCs) (i.e., Tc, I, Se, and nitrate) is necessary to determine if Cast Stone, a radioactive waste form, can meet performance objectives under near-surface disposal scenarios. In this work, a mineral and parameter set accounting for the solubility of I and Se in Cast Stone was developed based on pH-dependent and monolithic diffusion leaching test results, to extend a geochemical speciation model previously developed. The impact of oxidation and carbonation as environmental aging processes on the retention properties of Cast Stone for primary COPCs was systematically estimated. Physically, the effective diffusion coefficients of 4 COPCs in Cast Stone were increased after carbonation and/or oxidation, reflecting an increase in permeability to diffusion. Chemically, i) pH & pe conditions in the original Cast Stone were favorable for the stabilization of Tc, but not for I, Se, and N; ii) oxidation (with/without carbonation) of Cast Stone changed the pe & pH conditions to be detrimental for Tc stabilization; and iii) carbonation (with/without oxidation) of Cast Stone modified the pH & pe conditions to be beneficial for the stabilization of I (in system with Ag added) and Se.

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

Reactive chemical transport simulations of geologic carbon sequestration: Methods and applications

Chemical reaction simulations are considerably used to quantitatively assess the long-term geologic carbon sequestration (GCS), such as CO 2 sequestration capacity estimations, leakage pathway analyses, enhanced oil recovery (EOR) efficiency studies, and risk assessments of sealing formations (caprocks), wellbores, and overlying underground water resources. All these require a deep understanding of the CO 2 - associated chemical reactions. To ensure long-term, safe CO 2 sequestration in the intended formations, modeling is the only way to plausibly assess the CO 2 flow, reaction, and transport over thousands of years. This review summarizes the multiple methodologies for describing homogeneous and heterogeneous chemical reaction patterns and multiscale application examples, the recent progress and current status of chemical reaction simulations for GCS, and the impact of such simulations on geological CO2 sequestration performance. Technical gaps and future challenges are also discussed for further study. The trends and challenges of such studies include: (1) the combination of coupled chemical, mechanical, and transport processes with calibrated experiments and associated uncertainty/risk assessments; (2) enhancement of the ability to simulate detailed geophysical and geochemical equations to mimic in situ conditions; and (3) characterization of multiscale subsurface systems with detailed conceptual models and assignment of suitable boundary conditions for field-scale sequestration fields. One major gap remaining is the current lack of accurate (and scale-justified) kinetic and equilibrium chemical reaction parameters under reservoir conditions. Advanced models that couple chemical, mechanical, and transport processes with scale-justified parameters, from lab to field-scale experiments, are required for quantitative assessments of sequestration capacity and the long-term safety of GCS projects.

58 GEOSCIENCES↗
DOE OSTI2023

Utah FORGE 5-2428: Fracture Permeability Impact on Reservoir Stress and Seismic Slip Behavior - Workshop Presentation

This is a presentation on the Fracture Permeability Impact on Seismic Slip Behavior project by Lawrence Livermore National Laboratory, presented by Dr. Kayla A. Kroll. The project's objective is to develop, apply and validate a holistic thermal, hydrologic, mechanical, and chemical (THMC) workflow that includes evaluation of induced seismic slip in EGS reservoirs. This presentation was featured in the Utah FORGE R&D Annual Workshop on September 8, 2023. The workshop provided a valuable opportunity to explore the progress made in each of the 17 Research and Development projects funded under Solicitation 2020-1 which aim to enhance our understanding of the crucial factors influencing the development of Enhanced Geothermal Systems (EGS) reservoirs and resources.

15 GEOTHERMAL ENERGY↗
DOE OSTI2022

Probing multiscale dissolution dynamics in natural rocks through microfluidics and compositional analysis

Mineral dissolution significantly impacts many geological systems. Carbon released by diagenesis, carbon sequestration, and acid injection are examples where geochemical reactions, fluid flow, and solute transport are strongly coupled. The complexity in these systems involves interplay between various mechanisms that operate at timescales ranging from microseconds to years. Current experimental techniques characterize dissolution processes using static images that are acquired with long measurement times and/or low spatial resolution. These limitations prevent direct observation of how dissolution reactions progress within an intact rock with spatially heterogeneous mineralogy and morphology. We utilize microfluidic cells embedded with thin rock samples to visualize dissolution with significant temporal resolution (100 ms) in a large observation window (3 × 3 mm). Here we injected acidic fluid into eight shale samples ranging from 8 to 86 wt % carbonate. The pre- and postreaction microstructures are characterized at the scale of pores (0.1 to 1 µm) and fractures (1 to 1,000 µm). We observe that nonreactive particle exposure, fracture morphology, and loss of rock strength are strongly dependent on both the relative volume of reactive grains and their distribution. Time-resolved images of the rock unveil the spatiotemporal dynamics of dissolution, including two-phase flow effects in real time and illustrate the changes in the fracture interface across the range of compositions. Moreover, the dynamical data provide an approach for characterizing reactivity parameters of natural heterogeneous samples when porous media effects are not negligible. The platform and workflow provide real-time characterization of geochemical reactions and inform various subsurface engineering processes.

58 GEOSCIENCES↗
DOE OSTI2024

Rare earth element enrichment in coal and coal-adjacent strata of the Uinta Region, Utah and Colorado

This study aims to quantify rare earth element enrichment within coal and coal-adjacent strata in the Uinta Region of central Utah and western Colorado. Rare earth elements are a subset of critical minerals as defined by the U.S. Geological Survey. These elements are used for a wide variety of applications, including renewable energy technology in the transition toward carbon-neutral energy. While rare earth element enrichment has been associated with Appalachian coals, there has been a more limited evaluation of western U.S. coals. Here, samples from six active mines, four idle/historical mines, four mine waste piles, and seven stratigraphically complete cores within the Uinta Region were geochemically evaluated using portable X-ray fluorescence ( n = 3,113) and inductively coupled plasma-mass spectrometry ( n = 145) elemental analytical methods. Results suggest that 24%–45% of stratigraphically coal-adjacent carbonaceous shale and siltstone units show rare earth element enrichment (>200 ppm), as do 100% of sampled igneous material. A small subset (5%–8%) of coal samples display rare earth element enrichment, specifically in cases containing volcanic ash. This study proposes two multi-step depositional and diagenetic models to explain the enrichment process, requiring the emplacement and mobilization of rare earth element source material due to hydrothermal and other external influences. Historical geochemical evaluations of Uinta Region coal and coal-adjacent data are sparse, emphasizing the statistical significance of this research. These results support the utilization of active mines and coal processing waste piles for the future of domestic rare earth element extraction, offering economic and environmental solutions to pressing global demands.

Coe, Haley H.↗