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At least 145 records · Page 8

Application of a Null-Space Monte Carlo Flow Model Set to the Composite Analysis Base Case Fate and Transport Modeling

The Plateau-to-River (P2R) Model is a groundwater flow and contaminant fate and transport (F&T) simulation model used to support remedial activities conducted by Central Plateau Cleanup Company (CPCCo) at the Hanford Site in Washington State. Figure 1 illustrates the P2R Model extents, discretization, and boundary conditions. The P2R Model is utilized in the composite analysis (CA) for the Hanford Site as the computational engine for computing F&T predictions as described in CP-60406, Hanford Site Composite Analysis Technical Approach Description: Groundwater. The model simulates contaminants of concern within the saturated zone of the uppermost aquifer beneath the Central Plateau and downgradient to the Columbia River. CP-57037, Model Package Report for the Plateau to River Model Version 8.3 documents the current version of the P2R Model including a description of the conceptual site model, model development and calibration, and limitations to the model application.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Application of a Null-Space Monte Carlo Flow Model Set to the Composite Analysis Base Case Fate and Transport Modeling

The Plateau to River Groundwater Model (P2R Model) is a groundwater flow and contaminant fate and transport (F&T) simulation model used to support remedial activities conducted by CH2M HILL Plateau Remediation Company at the Hanford Site in Washington State. Figure 1-1 illustrates the P2R Model extents, discretization, and boundary conditions. The P2R Model is utilized in the Composite Analysis (CA) for the Hanford Site as the computational engine for computing F&T predictions as described in CP-60406, Hanford Site Composite Analysis Technical Approach Description: Groundwater. The model simulates contaminants of concern within the saturated zone of the uppermost aquifer beneath the Central Plateau and downgradient to the Columbia River. CP-57037, Model Package Report for the Plateau to River Model Version 8.3, documents the current version of the P2R Model including a description of the conceptual site model, model development and calibration, and limitations to the model application. The overall objective of the saturated zone modeling effort is to provide a basis for making informed remedial action decisions based on descriptions of current and expected future contaminant concentrations in groundwater at decision points within and downgradient of the Central Plateau of the Hanford Site. Specifically, the purpose of this environmental calculation is to describe the application of the hydraulic property fields and recharge parameters documented in ECF-HANFORD-20-0027, Null Space Monte Carlo Evaluation of the Plateau to River Model, to the CA flow and fate and transport simulation results to quantify the uncertainty in the simulated results due to input parameter selection. Use of numerical groundwater models is always accompanied with uncertainty in the results produced by a model because models are approximations of reality. Thus, by definition, models lack the detail to fully represent observed behavior. Use of numerical techniques, such as a NSMC analysis, can help in identifying and quantifying the potential uncertainties associated with a numerical model such as the P2R Model. The result of NSCM analysis is a set of F&T simulations that provide an estimate of the range of possible outcomes that are used to quantify the uncertainty in simulated concentrations produced using the base case simulations. The simulated concentrations from all simulations will support calculation of the uncertainty of the total dose calculated in a separate calculation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Spatial Mapping of Riverbed Grain-Size Distribution Using Machine Learning

Recent alluvial sediments in riverbeds play a significant role in controlling hydrologic exchange flows (HEFs) in river systems. The alluvial layer is usually associated with strong heterogeneity in physical properties (e.g., permeability and hydraulic conductivity), which affects local HEFs and therefore biogeochemical processes. The spatial distribution of these physical properties needs to be determined to inform the numerical models used to reveal the realistic hydro-biogeochemical behaviors. Such information can be obtained based on the intrinsic link between sediment grain-size distribution and hydraulic properties where sediment texture information is available. However, grain-size measurements are usually spatially sparse and do not have adequate coverage and resolution, particularly for a relatively large domain such as the Hanford Reach of the Columbia River. In this paper, we adopted machine learning (ML) approaches for categorizing and mapping the spatial distributions of riverbed substrate grain size and filling in missing areas of substrate data using the ML models along the reach. Such ML models for substrate size mapping were trained at 13,372 locations using measured substrate sizes along with observed and simulated attributes, including bathymetric attributes (e.g., elevation, slope, and aspect ratio) from LIDAR and bathymetric surveys, and hydrodynamic properties (e.g., water depth, velocity, shear stress, and their statistical moments). An ensemble bagging-based ML technique, Random Forest, was adopted to identify the most influential factors as predictors to develop the predictive models with over-fitting issues addressed. The models were evaluated with respect to each individual substrate size class and the lumped group, and then used to generate the final substrate size maps covering all the grid cells in the numerical modeling domain.

54 ENVIRONMENTAL SCIENCES↗

Modeling of streamflow in a 30 km long reach spanning 5 years using OpenFOAM 5.x

Abstract. Developing accurate and efficient modeling techniques for streamflow at the tens-of-kilometers spatial scale and multi-year temporal scale is critical for evaluating and predicting the impact of climate- and human-induced discharge variations on river hydrodynamics. However, achieving such a goal is challenging because of limited surveys of streambed hydraulic roughness, uncertain boundary condition specifications, and high computational costs. We demonstrate that accurate and efficient three-dimensional (3-D) hydrodynamic modeling of natural rivers at 30 km and 5-year scales is feasible using the following three techniques within OpenFOAM, an open-source computational fluid dynamics platform: (1) generating a distributed hydraulic roughness field for the streambed by integrating water-stage observation data, a rough wall theory, and a local roughness optimization and adjustment strategy; (2) prescribing the boundary condition for the inflow and outflow by integrating precomputed results of a one-dimensional (1-D) hydraulic model with the 3-D model; and (3) reducing computational time using multiple parallel runs constrained by 1-D inflow and outflow boundary conditions. Streamflow modeling for a 30 km long reach in the Columbia River (CR) over 58 months can be achieved in less than 6 d using 1.1 million CPU hours. The mean error between the modeled and the observed water stages for our simulated CR reach ranges from −16 to 9 cm (equivalent to approximately ±7 % relative to the average water depth) at seven locations during most of the years between 2011 and 2019. We can reproduce the velocity distribution measured by the acoustic Doppler current profiler (ADCP). The correlation coefficients of the depth-averaged velocity between the model and ADCP measurements are in the range between 0.71 and 0.83 at 75 % of the survey cross sections. With the validated model, we further show that the relative importance of dynamic pressure versus hydrostatic pressure varies with discharge variations and topography heterogeneity. Given the model's high accuracy and computational efficiency, the model framework provides a generic approach to evaluate and predict the impacts of climate- and human-induced discharge variations on river hydrodynamics at tens-of-kilometers and decadal scales.

58 GEOSCIENCES↗

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↗

Null Space Monte Carlo Evaluation of the Plateau to River Model

The Plateau to River Groundwater Model (P2R Model) is a groundwater flow and contaminant fate and transport (F&T) simulation model used to support remedial activities conducted by CH2M HILL Plateau Remediation Company at the Hanford Site in Washington State. Figure 1-1 illustrates the P2R Model extents, discretization, and boundary conditions. The P2R Model provides a computational framework to simulate the F&T of contaminants in groundwater associated with the 200-PO-1, 200-UP-1, 200-BP-5, and 200-ZP-1 Groundwater Operable Units (OUs) in the Hanford Site Central Plateau. In addition, the model includes adjacent areas and facilities (e.g., the State Approved Land Disposal Site). Intended and anticipated uses of the model include calculating water levels, hydraulic gradients, and groundwater flows throughout the model domain (encompassing the 200 West and 200 East Areas) for use in subsequent F&T calculations for contaminants of concern and developing scale-appropriate, telescopic-mesh refinement models for detailed evaluation of areas within the model domain where required. The overall objective of the modeling effort is to provide a basis for making informed remedial action decisions based on descriptions of current and expected future contaminant concentrations in groundwater at decision points within the OU boundaries. The objective for the model development phase is to create a common modeling platform that can be used for investigations of the Central Plateau groundwater OUs and areas downgradient toward the Columbia River. The P2R Model calibration to historical data observed at the Hanford Site is documented in CP-57037, Model Package Report for the Plateau to River Model Version 8.3. The purpose of this environmental calculation is to describe a null space Monte Carlo (NSMC) evaluation was conducted with the historic calibration of the P2R model. Use of numerical groundwater models is always accompanied with uncertainty in the results produced by a model because models are approximations of reality. Thus, by definition, lack the detail to fully represent observed behavior. Use of numerical techniques, such as a NSMC analysis, can help in identifying and quantifying the potential uncertainties associated with a numerical model such as the P2R Model. Use of the NSMC approach results in 100 groundwater flow models that are variants of the calibrated P2R Model. These variant models can be used to evaluate uncertainty in model predictions made by the calibrated P2R Model for other analyses. A secondary purpose of the environmental calculation is to establish these variant models for use with other applications.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Estimating carrying capacity for juvenile salmon using quantile random forest models

Abstract Establishing robust methods and metrics to evaluate habitat quality is critical for the recovery of endangered Pacific salmonids ( Oncorhynchus spp.). A variety of modeling approaches are used for status and trend monitoring of anadromous species throughout the Pacific Northwest, USA, but current methods may fail to capture the complex relationship between fish and habitat and are often limited in predictive power beyond specific watersheds. Further, the focus on species distribution and abundance is not easily manipulated to predict carrying capacity and traditional stock‐recruitment analyses are reliant on long‐term data which are not always available. In this study, we developed a quantile random forest model to provide estimates of habitat carrying capacity for Chinook salmon ( O. tshawytscha ) parr during the summer months, at both the site and watershed scale. Quantile random forest models allow for the consideration of noisy data, correlated variables, and non‐linear relationships: common features in fish–habitat datasets. We leveraged Columbia Habitat Monitoring Program data to select habitat co‐variates and predict capacity at those sites. We also identified a set of globally available attributes to extrapolate capacity estimate predictions throughout wadeable streams within the Columbia River basin. Total capacity estimates for watersheds closely matched estimates from alternative fish productivity models. Carrying capacity estimates based on quantile random forest models, like those presented here, provide managers a framework to guide the identification, prioritization, and development of habitat rehabilitation actions to recover salmon populations.

See, Kevin E.↗

Predation probabilities and functional responses: How piscivorous waterbirds respond to pulses in fish abundance

Abstract How predators respond to changes in prey abundance (i.e., functional responses) is foundational to consumer–resource interactions, predator–prey dynamics, and the stability of predator–prey systems. Predation by piscivorous waterbirds on out‐migrating juvenile steelhead trout ( Oncorhynchus mykiss ) is considered a factor affecting the recovery of multiple Endangered Species Act‐listed steelhead populations in the Columbia River basin. Waterbird functional responses, however, may vary by predator species and location, with important implications to predator management strategies. We used a 13‐year dataset on waterbird abundance across seven breeding colonies (three Caspian tern [ Hydroprogne caspia ], two double‐crested cormorant [ Nannopterum auritum ], and two California and ring‐billed gull [ Larus californicus and Larus delawarensis ] colonies) and steelhead tag‐recovery data (>645,000 tagged and >32,000 recovered steelhead) to quantify weekly predation probabilities and functional responses across waterbird species, colonies, and years. Weekly predation probabilities were highly variable, ranging from 0.01 to 0.30 at tern colonies, 0.01 to 0.20 at cormorant colonies, and 0.03 to 0.13 at gull colonies. Per capita predation probabilities were an order of magnitude higher at inland tern and cormorant colonies relative to estuary colonies of the same species. Terns displayed Type II functional responses across colonies and years, where predation probabilities peaked at low steelhead abundances and declined as steelhead abundance increased (i.e., predator swamping). Cormorants nesting at the large estuary colony (several thousand birds) displayed a Type III functional response, but cormorants nesting at the smaller inland colony (several hundred birds) displayed a Type II response. Consumption probabilities of steelhead by gulls remained consistent across a large range of steelhead availability, suggesting a Type I or a Type III functional response, but a lack of colony abundance data prevented quantifying functional responses. The level of tern predation combined with Type II functional responses indicate possible population‐level impacts that could destabilize small or declining prey populations. Conversely, the apparent Type III functional responses of gulls and estuary nesting cormorants are indicative of prey switching behaviors targeted at periods of high steelhead abundance. Our results illustrate the complexity of predator–prey interactions and the importance of quantifying predator‐ and location‐specific functional responses when predicting the efficacy of management strategies to enhance prey populations.

Hostetter, Nathan J.↗

Applying cumulative effects to strategically advance large-scale ecosystem restoration

Programs restoring large terrestrial-aquatic ecosystems are expected to increase in area and number over the next decade. Factors ensuring long-term effectiveness at the program scale differ from those at the individual restoration project scale, necessitating a new synthesis. Here we contextualize hydrological, geomorphological, and biological effects of large-scale ecosystem restoration activities within a cumulative-effects paradigm. Evidence of eight modes of cumulative effects benefiting species and ecosystems was elucidated by reviewing restoration efforts in the greater Florida Everglades, Gulf Coast, lower Columbia River and estuary, Puget Sound estuary, Missouri River, northeastern coastal states, San Francisco Bay and Sacramento Delta. Additive and nonlinear cumulative effects of interacting restoration projects propagated across landscape and regional geographic scales, and throughout trophic levels, affecting population structures. Applying a cumulative-effects paradigm to planning, implementing, and evaluating large-scale restoration will avoid countervailing effects and capitalize on positive feedback, advancing evidence-based programs to recover priority species and ecosystems.

54 ENVIRONMENTAL SCIENCES↗

A Review of Factors Affecting the Susceptibility of Juvenile Salmonids to Avian Predation

Abstract We reviewed studies of piscivorous colonial waterbird predation on juvenile salmonids to synthesize current knowledge of factors affecting fish susceptibility to avian predators. Specifically, we examined peer-reviewed publications and reports from academic, governmental, and nongovernmental agencies to identify commonalities and differences in susceptibility of salmonids to avian predation, with a focus on mark–recovery studies in the Columbia River basin. Factors hypothesized to influence salmonid susceptibility to avian predation were grouped into four general categories: (1) salmonid species and populations, (2) environmental factors, (3) prey density, predator density, and migration timing, and (4) prey characteristics. Our review focused on predation by Caspian terns Hydroprogne caspia, double-crested cormorants Nannopterum auritum, and gull species Larus spp. as these are the most well-studied avian predators of salmonids. Results indicated that predator–prey interactions varied across salmonid species and populations and species of avian predator. Inferences across studies supported multiple hypotheses regarding predator–prey dynamics, including environmental factors that influence prey exposure to predators (e.g., river flows, turbidity, alternative prey), variation in predator and prey abundances, predator characteristics (e.g., foraging behavior, colony location), and prey characteristics (e.g., fish length, condition). Mark–recovery studies of avian predation on fish populations have greatly improved our understanding of the factors affecting fish susceptibility to avian predation, the relative contributions of abiotic and biotic factors to predation susceptibility, and the extent to which avian predation affects fish survival and the viability of prey populations. Future studies that jointly model predation and survival and the factors affecting those processes will further broaden our understanding of predator–prey dynamics and directly evaluate the effects of predation on prey population dynamics.

Hostetter, Nathan J. (ORCID:0000000160752157)↗

Advances in hexagon mesh-based flow direction modeling

Watershed delineation and flow direction representation are the foundations of streamflow routing in spatially distributed hydrologic modeling. A recent study showed that hexagon-based watershed discretization has several advantages compared to the traditional Cartesian (latitude–longitude) discretization, such as uniform connectivity and compatibility with other Earth system model components based on unstructured mesh systems (e.g., oceanic models). Despite these advantages, hexagon-based discretization has not been widely adopted by the current generation of hydrologic models. One major reason is that there is no existing model that can delineate hexagon-based watersheds while maintaining accurate representations of flow direction across various spatial resolutions. In this study, we explored approaches such as spatial resampling and hybrid breaching-filling stream burning techniques to improve watershed delineation and flow direction representation using a newly developed hexagonal mesh watershed delineation model (HexWatershed). We applied these improvements to the Columbia River basin and performed 16 simulations with different configurations. The results show that (1) spatial resampling modulates flow direction around headwaters and provides an opportunity to extract subgrid information; and (2) stream burning corrects the flow directions in mountainous areas with complex terrain features.

58 GEOSCIENCES↗

Isotopic discrimination of natural and anthropogenic perchlorate sources in groundwater in a semi-arid region of northeastern Oregon (USA)

Perchlorate (ClO 4 - ) has synthetic and natural sources. Synthetic ClO 4 - is released to the environment from its use as an oxidant in military and aerospace applications, and from its presence in a variety of common commercial products, such as safety flares, chlorate herbicides, and fireworks. Natural sources of ClO 4 - in the environment include imported nitrate fertilizers derived from salt deposits in the Atacama Desert of Chile and indigenous natural ClO 4 - that accumulates in unsaturated soils and groundwaters in other arid and semi-arid environments, largely from atmospheric deposition. The stable isotope ratios of chlorine ( 37 Cl/ 35 Cl) and oxygen ( 18 O/ 16 O, 17 O/ 16 O) and the isotopic abundance of radioactive 36 Cl in ClO 4 - can be used to discriminate these different sources. Perchlorate was previously detected at relatively high concentrations (3.8–34.7 μg/L) in groundwater from many wells in the Boardman-Umatilla area near the Columbia River in northeastern Oregon, which is a semi-arid, highly agricultural, heavily irrigated area that includes several past and current military installations. Eight representative groundwater wells were sampled throughout this region and isotopic characteristics of ClO 4 - collected from each well were measured along with other chemical and isotopic parameters including tritium and other groundwater age indicators. We report isotopic data indicate that indigenous natural ClO 4 - was present in groundwater from all sampled wells and was the predominant source in five of the wells. Synthetic ClO 4 - was present in the three remaining wells with natural ClO 4 - , and a minor fraction of Atacama-fertilizer-derived ClO4- was indicated in one of the wells. Data from this study expand the geographic area of the USA in which indigenous natural ClO 4 - has been detected to include the semi-arid northwest. This study also illustrates the role of irrigation recharge as a mechanism for producing relatively high concentrations of indigenous natural ClO 4 - in groundwater by flushing accumulated salts from the unsaturated zone.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Validating simulated mountain wave impacts on hub-height wind speed using SoDAR observations

The ascent of stably stratified air over a mountain barrier can trigger the generation of mountain waves. Mountain waves occur frequently over the Columbia River Gorge in western North America and can impact wind power generation over the area. Therefore, predicting the details of mountain waves events (e.g., dominant wavelength, timing, and duration) can be very valuable for the wind energy community. In this study, the ability of the Weather Research and Forecasting (WRF) model to simulate mountain waves and their impact on hub-height wind speed is investigated. Our results suggest that the WRF model has moderate skill in simulating observed mountain wave. Further, given WRF predictions of wavelength range and wave period, the Fast Fourier Transform can calculate the simulated mountain wave impact on hub-height wind speed. The resulting wind speeds agree well with SoDAR observations in terms of both magnitude and pattern. Finally, for the simulated cases, WRF consistently predicts impacts of significant mountain wave events about an hour earlier than the actual observations. Overall, in this work, the sensitivities as well as uncertainties associated with our methodology are discussed in detail.

17 WIND ENERGY↗

Parts-Per-Million Carbonate Mineral Quantification with Thermogravimetric Analysis–Mass Spectrometry

Mitigating the deleterious effects of climate change requires the development and implementation of carbon capture and storage technologies. To expand the monitoring, verification, and reporting (MRV) capabilities of geologic carbon mineralization projects, we developed a thermogravimetric analysis–mass spectrometry (TGA–MS) methodology to enable quantification of <100 ppm calcite (CaCO 3 ) in complex samples. We extended TGA–MS calcite calibration curves to enable a higher measurement resolution and lower limits of quantification for evolved CO 2 from a calcite–corundum mixture. We demonstrated <100 ppm carbonate mineral quantification with TGA–MS for the first time, an outcome applicable across earth, environmental, and materials science fields. We applied this carbonate quantification method to a suite of Columbia River Basalt Group (CRBG) well cuttings recovered in 2009 from Pacific Northwest National Laboratory’s Wallula #1 Well. Our execution of this new combined calcite and calcite–corundum calibration curve TGA–MS method on our CRBG sample suite indicated average carbonate contents of 0.050 wt % in flow interiors (caprocks) and 0.400 wt % in interflow zones (reservoirs) in the upper 1250 m of the Wallula #1 Well. Finally, by advancing our knowledge of continental flood basalt-hosted carbonates in the mafic subsurface and reaching new TGA–MS quantification limits for carbonate minerals, we expand MRV capabilities and support the commercial-scale deployment of carbon mineralization projects in the Pacific Northwest United States and beyond.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantification of CO 2 Mineralization at the Wallula Basalt Pilot Project

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

54 ENVIRONMENTAL SCIENCES↗

Exotic Carbonate Mineralization Recovered from a Deep Basalt Carbon Storage Demonstration

Mitigating climate change require transformational advances for carbon dioxide removal, including geologic carbon sequestration in reactive subsurface environments. The Wallula Basalt Carbon Storage Pilot Project demonstrated that CO 2 injected into >800 m deep Columbia River Basalt Group flow top reservoirs mineralizes on month-year timescales. Herein, we present new optical petrography, micro-computed X-ray tomography, and electron microscopy results sidewall cores collected two years after CO 2 injection. As no other anthropogenic carbonates from geologic carbon storage field studies have been recovered, this world-unique sample suite provides unparalleled insight for subsurface carbon mineralization products and paragenesis. Chemically-zoned nodules with Ca/Mn-rich cores and Fe-dominant outer rims are prominent examples of the neoformed carbonate assemblages with ankerite-siderite compositions and exotic divalent cation correlations. Further, paragenetic insights for the timing of aragonite, silica, and fibrous zeolites are clarified based on mineral texture and spatial relationships, along with time-resolved downhole fluid sampling. Collectively, these results clarify the mineralogy, chemistry, and paragenesis of carbon mineralization, providing insight into the ultimate fate and transport of CO 2 in reactive mafic-ultramafic reservoirs

54 ENVIRONMENTAL SCIENCES↗

Facile Metal Release from Pore-Lining Phases Enables Unique Carbonate Zonation in a Basalt Carbon Mineralization Demonstration

Carbon-negative strategies such as geologic carbon sequestration in continental flood basalts offers a promising route to the removal of greenhouse gases, such as CO 2 , via safe and permanent storage as stable carbonates. This potential has been successfully demonstrated at a field scale at the Wallula Basalt Carbon Storage Pilot Project where supercritical CO 2 was injected into the Columbia River Basalt Group (CRBG). Here, we analyze recovered post-injection sidewall core cross-sections containing carbonate nodules using μ-XRF chemical mapping techniques that revealed compositional zonation within the nodules. The unique nature of the subsurface anthropogenic carbonates is highlighted by the near absence of Mg in an ankerite-like composition. Furthermore, a comparison between pre- and post-injection sidewall cores along with an in-depth chemical mapping of basalt pore lining cements provides a better understanding into the source and fate of critical cationic species involved in the precipitation of carbon mineralization products. Collectively, these results provide crucial insights into carbonate growth mechanisms under a time-dependent pore fluid composition. Finally, as such, these findings will enable parameterization of predictive models for future CO 2 sequestration efforts in reactive reservoirs around the world.

54 ENVIRONMENTAL SCIENCES↗

3D Quantification of Pore Networks and Anthropogenic Carbon Mineralization in Stacked Basalt Reservoirs

Basalt formations are promising candidates for the geologic storage of anthropogenic CO 2 due to their storage capacity, porosity, permeability, and reactive geochemical trapping ability. The Wallula Basalt Carbon Storage Pilot Project demonstrated that supercritical CO 2 injected into >800 m deep Columbia River Basalt Group stacked reservoir flow tops mineralizes to ankerite-siderite-aragonite on month-year timescales, with 60% of the 977 metric tonnes of CO 2 converted within two years. The potential impacts of mineral precipitation and consequent changes on rock porosity, pore structure, pore size, and pore size distributions have likely been underestimated hitherto. Herein, we address these knowledge gaps using X-ray Micro Computed Tomography (XMT) to evaluate the pore network architecture of sidewall cores recovered two years after CO 2 injection. In the present study, we performed a detailed quantitative analysis of the CO 2 -reacted basalt cores by XMT imaging. Reconstructed 3D images were analyzed to study the distribution and volumetric details of porosity and carbonate nodules in the cores along with the various other phases, providing insight into paragenesis and carbonate growth mechanisms, including mineralogic/chemical zonation. Finally, these findings are being used to parametrize multiphase reactive transport models to predict the fate and transport of subsurface CO 2 , enabling scale-up to commercial-scale geologic carbon storage in basalts and other reactive mafic-ultramafic formations.

54 ENVIRONMENTAL SCIENCES↗