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Enriched Background Isotope Study (EBIS): Analysis of 14C-Enriched Carbon Cycle in Soils and Litter at Forested Oak Ridge and AmeriFlux Sites, 2001-2011

These data provide a record of the multi-year, multi-institutional Enriched Background Isotope Studies (EBIS) projects that ran from 2000 through 2011. Elevated levels of 14C enriched CO2 in the air and soil atmosphere as well as leaf, stem, and root tissues were observed on the Oak Ridge Reservations (ORR) during the summer of 1999, and were attributed to local incinerator activities on and/or near the ORR (Trumbore et al. 2002). The isolated enrichment of the background levels of 14C in local forest ecosystem represented a unique opportunity to study unresolved carbon cycling processes such as the contribution of leaf versus root litter contributions to soil carbon accumulation, the rate of vertical transport of carbon into deep soil storage pools, and the differential contribution of physicochemical versus faunal driven processes to soil carbon cycling and sequestration. Leaf litter from the local enriched forest was transplanted to selected sites on the ORR and to selected AmeriFlux study sites to study soil C cycling across a range of soils and climates. The EBIS research projects provide data on C flux from litter sources to mineral soil sinks for United States eastern hardwood forests necessary for testing process hypotheses and judging efficacy of soil C cycling models. Experimental results from this study are being used to parameterize and refine existing carbon dynamics models, the quantification of the long-term fate of ecosystem carbon inputs and as a means to judge the potential for ecosystem carbon sequestration via enhance litter inputs to soil. EBIS observations support conclusions that intra- and inter-annual soil carbon cycling in hardwood forest soils should be characterized as a least a two-compartment system where surface leaf-litter and belowground root turnover represent primary carbon sources for organic-layer and mineral-soil carbon cycles, respectively. EBIS experiments were conducted to complete enriched litterfall maniplations in upland forests on Ultisol and Inceptisol soils of the Oak Ridge Reservation, Oak Ridge, Tennessee. We also collected additional14C-enriched materials for new experimental applications, and applied those materials to multiple AmeriFlux sites over a range of climatic, edaphic and biological conditions. The research provided data for addressing DOE's goal of understanding mechanisms controlling C flux, and for the improvement of models to be applied to policy discussions regarding the safe levels of greenhouse gases for the earth's system. There are 5 data files provided in comma separated (*.csv) format for vegetation, field litter, soil and air [C] and C isotope data from the EBIS studies and associated environmental data.

54 ENVIRONMENTAL SCIENCES↗

Recent Progress on Emerging Applications of Hydrochar

Hydrothermal carbonization (HTC) is a prominent thermochemical technology that can convert high-moisture waste into a valuable product (called hydrochar) at a relatively mild treatment condition (180–260 °C and 2–10 MPa). With rapidly growing research on HTC and hydrochar in recent years, review articles addressing the current and future direction of this research are scarce. Hence, this article aims to review various emerging applications of hydrochars, e.g., from solid fuel to soil amendment, from electron storage to hydrogen storage, from dye adsorption, toxin adsorption, heavy metal adsorption to nutrient recovery, and from carbon capture to carbon sequestration, etc. This article further provides an insight in the hydrochar’s working mechanism for various applications and how the applications can be improved through chemical modification of the hydrochar. Finally, new perspectives with appropriate recommendations have been made to further unveil potential applications and its improvement through hydrochar and its modified version.

09 BIOMASS FUELS↗

On Caprock Seal Integrity of Tuscaloosa Mudstone at Cranfield, MS (USA), CO 2 Injection Site

Saline formations deep underground are among the most promising targets for large-scale geologic carbon storage. The caprock seal integrity evaluation is an important component of commercial-scale CO 2 sequestration projects. Measurements of the porosity and permeability of mudstone samples from the NETL-supported Cranfield Project were performed using a helium porosimeter and a core flow apparatus, before and after exposure in a CO 2 -saturated brine environment. The permeability of the core samples rapidly decreased with the increase in confining pressure and did not fully recover after decompression. On the other hand, exposure to CO 2 led to an increase in the permeability by at least an order of magnitude. The porosity changes after the exposure were not substantial. The post-exposure increase in permeability was subsequently offset by its rapid decrease during the higher-pressure confinement. Extrapolation of the observed permeability trends to in situ reservoir conditions suggests that Tuscaloosa mudstone can effectively serve as a natural seal.

58 GEOSCIENCES↗

Investigation of enhanced CO 2 storage in deep saline aquifers by WAG and brine extraction in the Minnelusa sandstone, Wyoming

Geological CO 2 sequestration in deep saline aquifers has been extendedly investigated to reach the goal of carbon neutral as large amount of CO 2 can be reduced in a short time. Here, this study investigates the feasibility of water-alternating-gas (WAG) injection and brine extraction on enhancing CO 2 storage in a target deep saline aquifer, Minnelusa Sandstone in the Powder River Basin (PRB) of Wyoming. An integrated numerical model is developed to account for four scenarios: (1) CO 2 continuous injection (CI) through one injection well, (2) WAG injection through one injection well, (3) CO 2 CI through one injection well and brine extraction through one producer, (4) WAG injection through one injection well and brine extraction through one producer. Simulation results suggest that WAG injection and brine extraction corporately make it possible to enhance CO 2 injectivity while securing CO 2 storage safety. For instance, WAG injection considerably reduces structural trapping contribution while enhances dissolved and residual trapping contributions. As for brine extraction, it can decrease the maximum averaged reservoir pressure by 37% and 22% for CI and WAG injection, respectively. Besides, sensitive analyses of the operational parameters for the fourth scenarios are performed. Results reveal that, when the amount of total CO 2 injection has been predetermined, CO 2 injection time and rate within each period of WAG should be small whereas it is preferable to have large water injection time and rate. This is to secure desirable dissolved and residual trapping contributions (store CO 2 with safety). Sensitive degree results confirm that CO 2 injection rate, water injection time, and CO 2 injection time of WAG injection exhibit significant effects on CO 2 storage whereas the impacts of producer bottom-hole pressure (BHP), water injection rate, and CO 2 -water injection time are relatively weaker. This study not only sheds light on achieving double-win goal: enhance CO 2 injectivity and store CO 2 with safety, but also can be a critical reference for other CO 2 storage in deep saline aquifers.

58 GEOSCIENCES↗

CO 2 /Brine/Rock Interactions in the Cedar Keys-Lawson Formation

It has been reported that among the various geologic storage options, deep saline aquifers have the largest estimated capacity for CO 2 storage. Obtaining knowledge of possible artificially geochemically induced changes to the permeability and porosity of host CO 2 storage deposits will enable us to gain insight on long-term reservoir behavior under CO 2 storage conditions. An experimental study of the interaction of CO 2 /brine/rock on saline formations was conducted in a static system under CO 2 storage conditions. Chemical interactions in the Cedar Keys-Lawson Formation carbonate during exposure to CO 2 and brine under sequestration conditions were studied. Samples were exposed to the simulated in-situ reaction conditions for one and six months. The samples were exposed to a model brine at 55 °C and CO 2 pressure of 23.8 MPa (3,500 psig). Computed tomography (CT), x-ray diffraction (XRD), scanning electron microscopy (SEM)-energy dispersive x-ray spectroscopy (EDS), brine composition, core porosity, and core permeability analyses were conducted prior to and after the exposure experiments. Preliminary permeability measurements obtained from the core samples showed changes after they were exposed to CO 2 -saturated brine for one and six months. This observation suggests that mineral dissolution and mineral precipitation could occur in the host deposit altering its characteristics for CO 2 storage over time. The 3D images of the pore space clearly illustrate the degree of dissolution that occurred during exposure. It is noted that the dissolution that occurred during the six-month exposure could have enhanced the connectivity between voids. This may contribute the increase of permeability after the CO 2 /brine exposure. In addition, the primary minerals comprising the core are dolomite and gypsum. Both minerals could dissolve in the CO 2 /brine environment resulting in the increase of permeability after the six-month exposure.

58 GEOSCIENCES↗

AssessCCUS: An Integrated Approach for Aggregating Resources to Enable Techno-Economic and Life Cycle Assessment of Carbon Management Technologies

Carbon capture, utilization, and storage (CCUS) - also sometimes known as carbon management - technologies are becoming an increasingly important part of the portfolio of technologies necessary to mitigate climate change and defossilize industrial production systems (Sick, 2021). These technologies capture carbon dioxide from industrial point sources or from the atmosphere directly and then either sequester it or use it as a carbon source in valuable products. Potential utilization pathways include, but are not limited to, concrete, fuels, and certain commodity chemicals, and sequestration pathways can include permanent geological storage or temporary storage in natural sinks ranging from forests to agricultural soil. Regardless of the pathway, assessment of the economic and environmental performance of the technologies is important for understanding their potential scalability and impact as well as developing plans to minimize life cycle costs and potential environmental trade-offs. A full discussion of potential trade-offs associated with CCUS is outside the scope of this article, but promoting assessment broadly helps to stimulate important conversations about the benefits and drawbacks of any particular technological choice.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Subsurface mafic and ultramafic rock mapping and analysis for carbon mineralization in the United States (SubMAP-CO 2 )

Achieving durable, gigaton-scale carbon dioxide (CO₂) removal will require the development of storage strategies that are both permanent and scalable. Among the available options, carbon mineralization in mafic and ultramafic rocks offers a uniquely robust pathway for long-term CO₂ sequestration, converting CO₂ into thermodynamically stable carbonate minerals. While surface exposures of these lithologies have been extensively studied, particularly in ophiolitic and volcanic settings, the potential for carbon mineralization in the subsurface remains comparatively underexplored at national scale. This gap limits the ability to assess storage capacity, accessibility, and deployment pathways for mineralization-based carbon management in the United States.

08 HYDROGEN↗

Normal or abnormal? Machine learning for the leakage detection in carbon sequestration projects using pressure field data

The international commitments for atmospheric carbon reduction will require a rapid increase in carbon capture and storage (CCS) projects. The key to any successful CCS project lies in the long term storage and prevention of leakage of stored carbon dioxide (CO 2 ). In addition to being a greenhouse gas, CO 2 leaks reaching the surface can accumulate in low-lying areas resulting in a serious health risk. Among several alternatives, some of the more promising CCS storage formations are depleted oil and gas reservoirs, where the reservoirs had good geological seals prior to hydrocarbon extraction. With more CCS wells coming online, it is imperative to implement permanent, automated monitoring tools. We apply machine learning models to automate the leakage detection process in carbon storage reservoirs using rates of (CO 2 ) injection and pressure data measured by simple harmonic pulse testing (HPT). To validate the feasibility of this machine learning based workflow, we use data from HPT experiments carried out in the Cranfield oil field, Mississippi, USA. The data consist of a series of pulse tests conducted with baseline parameters and with an artificially introduced leak. Here, in this study, we pose the leakage detection task as an anomaly detection problem where deviation from the predicted behavior indicates leaks in the reservoir. Results show that different machine learning architectures such as multi-layer feed forward network, Long Short-Term Memory, and convolutional neural network are able to identify leakages and can provide early warning. These warnings can then be used to take remedial measures.

58 GEOSCIENCES↗

Time-lapse seismic data inversion for estimating reservoir parameters using deep learning

Geologic carbon sequestration involves the injection of captured carbon dioxide ([Formula: see text]) into subsurface formations for long-term storage. The movement and fate of the injected [Formula: see text] plume is of great concern to regulators because monitoring helps to identify potential leakage zones and determines the possibility of safe long-term storage. To address this concern, we design a deep-learning framework for [Formula: see text] saturation monitoring to determine the geologic controls on the storage of the injected [Formula: see text]. We use different combinations of porosities and permeabilities for a given reservoir to generate saturation and velocity models. We train the deep-learning model with a few time-lapse seismic images and their corresponding changes in saturation values for a particular [Formula: see text] injection site. The deep-learning model learns the mapping from the change in the time-lapse seismic response to the change in [Formula: see text] saturation during the training phase. We then apply the trained model to data sets comprising different time-lapse seismic image slices (corresponding to different time instances) generated using different porosity and permeability distributions that are not part of the training to estimate the [Formula: see text] saturation values along with the plume extent. Our algorithm provides a deep-learning assisted framework for the direct estimation of [Formula: see text] saturation values and plume migration in heterogeneous formations using the time-lapse seismic data. Our method improves the efficiency of time-lapse inversion by streamlining the large number of intermediate steps in the conventional time-lapse inversion workflow. This method also helps to incorporate the geologic uncertainty for a given reservoir by accounting for the statistical distribution of porosity and permeability during the training phase. Tests on different examples verify the effectiveness of our approach.

Geochemistry & Geophysics↗

Nano-Engineered Catalyst Supported on Ceramic Hollow Fibers for the Utilization of CO 2 in Dry Reforming to Produce Syngas

The objective of this project was to develop a novel catalytic reactor containing nano-engineered catalysts for the utilization of CO 2 (captured from coal-fired power plants and other CO 2 emitting sources) in dry methane reforming (DMR) (CO 2 + CH 4 → 2 H 2 + 2 CO) to produce synthesis gas (syngas). The technology aims to reduce CO2 emissions by developing beneficial uses for CO 2 from coal-fired power plants. It also offers an alternative to mitigate CO 2 emissions in areas where geologic storage may not be an optimal solution and/or utilization could significantly offset the costs of carbon capture and sequestration. The nano-engineered Ni-based catalyst was prepared by atomic layer deposition (ALD). The Ni particles were as small as ~2-4 nm. The nano-engineered catalyst showed CH 4 conversion >95%, H 2 /CO ratio in the range of 0.7-1.0, and CH 4 reforming rate as high as 2,500 L/h/gNi at 850 ºC and pressure of 15-25 psia. The Ni-based ALD catalyst also showed good stability in DMR reaction during a 200-h continuous operation at 850 °C. This is due to strong bonding between the nanoparticles and substrates since the Ni nanoparticles were chemically bonded to the substrate during the ALD process. The high thermal stability maintains the high dispersion of Ni nanoparticles, which can inhibit coke formation because their step edges are small enough to limit carbon nucleation and growth. Technoeconomic analysis (TEA) indicates the levelized cost of syngas (LCOS) is $172/ton with our technology, which is lower than the equivalent (molar) cost of hydrogen produced by steam methane reforming (SMR) or autothermal reforming (ATR). The major operating cost is natural gas feed and fuel, and the levelized cost is highly sensitive to the price of natural gas and relatively insensitive to the CAPEX. Revenues from syngas could have a significant impact on the net cost of electricity (COE), depending on the cost of natural gas and the selling price of syngas, estimated at $36 per MWh if the syngas were sold at $195 per ton. Following DOE NETL’s guidance, a lifecycle analysis (LCA) was conducted to compare with SMR. The functional unit for the basis of comparison was defined as 1kg carbon monoxide in the product stream. The global warming potential (GWP) of our process was found to be 40% lower than the state-of-the-art SMR process. The sensitivity analysis confirms the emissions are most sensitive to the natural gas fuel requirements to deliver heat to the process.

01 COAL, LIGNITE, AND PEAT↗

Permeability evolution of reservoir rocks interacting with CO2/brine under CO2 sequestration conditions

The Mount Simon formation in the Midwest region of the U.S. is considered as a potential candidate host reservoir for carbon storage. Obtaining knowledge of possible geochemically induced changes to the permeability and porosity of host CO2 storage sandstone will enable us to gain a deeper insight of the long-term reservoir behavior under the CO2 storage conditions. An experimental study of the interaction of CO2/brine/rock on saline formations in a static system under CO2 storage conditions was conducted.

Soong, Yee↗

Reduced CO 2 uptake and growing nutrient sequestration from slowing overturning circulation

Current Earth system models (ESMs) project dramatic slowing (28–42% by 2100) of Atlantic Meridional Overturning Circulation and Southern Meridional Overturning Circulation (SMOC) across a range of climate scenarios, with a complete shutdown of SMOC possible by year 2300. Slowing meridional overturning circulation (MOC) differentially impacts the ocean biological and solubility carbon pumps, leaving the net impact on ocean carbon uptake uncertain. Here using a suite of ESMs, we show that slowing MOC reduces anthropogenic carbon uptake by the solubility pump but increases deep-ocean storage of carbon and nutrients by the biological pump. The net effect reduces ocean uptake of anthropogenic CO 2 . The deep-ocean nutrient sequestration will increasingly depress global-scale, marine net primary production over time. As a result, MOC slowdown represents a positive feedback that could extend or intensify peak-warmth climate conditions on multi-century timescales.

58 GEOSCIENCES↗

Robust In-Situ Strain Measurements to Monitor CO 2 Storage

The goal of this project was to develop and demonstrate robust instrumentation to monitor the in-situ strain tensor in order to improve the reliability and security of CO 2 storage in geologic formations. We met the original goals of the project and the major overarching accomplishment is the advancement of strain tensor monitoring from an intriguing concept to a commercially available technology with a solid foundation of novel instruments supported by theoretical analyses and validation experiments. The main accomplishments of the project are summarized below. We designed, built and evaluated nine new optical fiber strainmeters and tiltmeters using Michelson interferometers to measure deformation with ultra-high resolution at both shallow and deep point locations in the subsurface. These are the robust strainmeters that motivated the title of the project. We designed, built and evaluated a novel method of measuring distributed strain in optical fibers with nanostrain resolution, and cm-scale location, and sampling into the seismic band. The new method is called Coherence-length-gated Microwave Photonics Interfereometry (CMPI). CMPI technology has advantages over existing commercial DAS and DSS methods. We developed and demonstrated capabilities to deploy instruments in the field and used them to measure strain caused by ambient signals like barometric pressure and tides, as well as induced signals like surface loading and pore pressure changes from pumping tests. We deployed a working strainmeter at 1,700 ft depth, slightly above an active reservoir. This is to our knowledge the greatest depth a strainmeter has been deployed and the techniques we used can readily be extended to greater depths. Optical fiber borehole tensor strainmeter techology was advanced from a TRL 4 at the start, to a TRL of 7 at the conclusion of the project. The project included advances in simulations and theoretical analyses. We developed and demonstrated a computational workflow that uses machine learning to reduce the computational requirements and make it practical to use Bayesian inversion to solve large numerical poroelastic analyses needed to interpret strain tensor field data. We evaluated the strain tensor fields and time series that would be caused by leaks of CO 2 or other fluids from reservoirs. These simulations demonstrated that signals from leaks could be measured with instruments developed for the project, opening a potentially new method for ensuring storage security. We showed that strains in caprock can be used to estimate pressure in a reservoir. This avoids the need to drill monitoring wells into the reservoir, and it expands the capabilities of monitoring in the caprock. The project includes a derivation and application of a novel analytical solution to the strains in the vicinity of a pressurized poroelastic inclusion. This solution explains field data measured during injeciton tests at the North Avant Field, and it will simplify future interpretation of strain tensor data. The project included a broad range of experiments, and of the most significant is the characterization of the strain tensor at an array three strainmeters during six injection tests at the North Avant Field, Oklahoma. This demonstrated repeatability of the strain signal measured by the new instruments developed for the project, and it showed similarities between the strain signal at shallow depths and pressure in the underlying reservoir. We also demonstrated that useful strain data can be measured at reservoir depths. This confirms that strain tensor data can be measured throughout the caprock over a reservoir. The project demonstrated the feasibility of using the strain tensor and distributed strain measured in caprock during a variety of different well tests where the pumping rate was constant, sinusoidal and positive, or a periodic square wave with zero net rate. This further strengthens the validity of using strain data to characterize reservoirs and aquifers. We also demonstrated that strain caused be fluctuations of air pressure and water pressure in the vadose zone can be measured and interpreted, suggesting that high resolution distributed strain measurements hold promise for monitoring the vadose zone. The project partially supported nine graduate students in the Environmental Engineering, Hydrogeology, Electrical Engineering programs at Clemson University. The research was described in nine journal papers, 23 talks and conference abstracts. Additional journal papers are in preparation. A new company called Tensora was started to provide strainmeter technology for commercial applications.

01 COAL, LIGNITE, AND PEAT↗

Multi-Scale 3D Imaging for Machine Learning Property Upscaling: Mt. Simon Sandstone Case Study

Petrographic properties of principal target reservoirs for carbon sequestration, such as the Mt. Simon Sandstone, are relevant to broad interest groups. The Mt. Simon Sandstone is a deep, saline, regionally extensive Cambrian sandstone, overlain by low permeability sealing formations, making it one of the viable geologic carbon storage reservoirs in the Midwestern US. Its thickness (exceeding 2400 ft in some localities), depth, and lateral extent, combined with high porosity and permeability make it a high-priority target of multiple ongoing geologic carbon sequestration efforts in the United States of America. The National Energy Technology Laboratory in Morgantown, West Virginia, has been engaged in characterization efforts of the Mt. Simon for over a decade, with a strong focus on Computed Tomographic data acquisition. Data generated during this period has been hitherto not accessible to the public. This archival effort focused on preservation of historical CT data and associated metadata, and facilitating their accessibility, culminating with the publication of the entire dataset on NETL’s Energy Data eXchange (EDX) and the associated Gill et. al (2024) paper.

Gill, Magdalena K.↗

Plant litter traits control microbial decomposition and drive soil carbon stabilization

Efforts to manage soils for carbon (C) sequestration remain limited by our understanding of how differences in plant traits and microbial traits mechanistically drive soil organic C (SOC) storage. Addressing this uncertainty is particularly critical in bioenergy agriculture, due to its potential to enhance soil C and provide a C neutral fuel. As such, we examined differences between two contrasting feedstocks, Zea mays (corn) and Miscanthus x giganteus (miscanthus), in the ability of their litter to form new chemically resistant particulate SOC vs. physically protected mineral associated SOC and used this data to improve the parameterization of a microbial SOC model. We tested a hypothesized conceptual model whereby easy to decompose corn litters drive greater microbial carbon use efficiency (CUE) and the formation of more mineral associated SOC over particulate SOC than more complex miscanthus litters. To do this, we performed a soil microcosm experiment where we added 13 C enriched aboveground and belowground litters to soils and traced the fate of the 13 C into microbial respiration and SOC pools. We found that corn litters promoted higher microbial CUE (0.37) than miscanthus litters (0.24). In turn, corn litter formed approximately 50% more mineral associated SOC than miscanthus litters. Similarly, structurally complex root litters promoted a lower CUE and formed less mineral associated SOC than leaf and shoot litters for both crops. When we used our data to parameterize the SOC model, we found that modelling microbial trait differences uniquely allowed the model to capture the fate of litter C in SOC. Collectively, we found a robust link between litter quality, microbial efficiency, and the formation of SOC. This link bridges the empirical uncertainty in how different crops can form new soil C and provides an empirical basis for modelling SOC transformations.

59 BASIC BIOLOGICAL SCIENCES↗

BrzostekEcologyLab/CORPSE-soil-jars

Efforts to manage soils for carbon (C) sequestration remain limited by our understanding of how differences in plant traits and microbial traits mechanistically drive soil organic C (SOC) storage. Addressing this uncertainty is particularly critical in bioenergy agriculture, due to its potential to enhance soil C and provide a C neutral fuel. As such, we examined differences between two contrasting feedstocks, Zea mays (corn) and Miscanthus x giganteus (miscanthus), in the ability of their litter to form new chemically resistant particulate SOC vs. physically protected mineral associated SOC and used this data to improve the parameterization of a microbial SOC model. We tested a hypothesized conceptual model whereby easy to decompose corn litters drive greater microbial carbon use efficiency (CUE) and the formation of more mineral associated SOC over particulate SOC than more complex miscanthus litters. To do this, we performed a soil microcosm experiment where we added 13C enriched aboveground and belowground litters to soils and traced the fate of the 13C into microbial respiration and SOC pools. We found that corn litters promoted higher microbial CUE (0.37) than miscanthus litters (0.24). In turn, corn litter formed approximately 50% more mineral associated SOC than miscanthus litters. Similarly, structurally complex root litters promoted a lower CUE and formed less mineral associated SOC than leaf and shoot litters for both crops. When we used our data to parameterize the SOC model, we found that modeling microbial trait differences uniquely allowed the model to capture the fate of litter C in SOC. Collectively, we found a robust link between litter quality, microbial efficiency, and the formation of SOC. This link bridges the empirical uncertainty in how different crops can form new soil C and provides an empirical basis for modeling SOC transformations.

Ridgeway, Joanna↗