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All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Ionic Liquid-Enhanced Interfaces to Boost Reactive C O2 Capture

The addition of ionic liquids (ILs) to a mixture containing a molecular solvent and other ionic species can induce the heterogeneous redistribution of cations and anions at the gas–liquid interface. This nonuniform redistribution of cations and anions driven by the differences in the solvophilicity of ions can improve the thermophysical and interfacial properties of such mixtures, creating a local chemical environment that is conducive to some reactions. In this work, ILs are added to a mixture of potassium hydroxide (KOH) and ethylene glycol (EG), used as a reactive absorbent and electrolyte in the migration-assisted moisture-gradient (MAMG) process for CO 2 capture. Molecular dynamics (MD) simulations are employed to probe into the effects of complex ion–ion and ion–solvent interactions and to examine the chemical composition at the gas–liquid interface. A total of 12 systems are investigated using molecular simulations to identify trends in the performance of IL additives based on the choice of cation, anion, and IL concentration. The cation effects are studied using IL additives based on 1-ethyl-3-methylimidazolium ([EMIM] + ) and 1-butyl-3-methylimidazolium ([BMIM] + ), while the impact of anions is examined using additives based on dicyanamide [DCA] − , triflate [TfO] − , bistriflimide [NTf 2 ] − , and hexafluorophosphate [PF 6 ] − anions, respectively. The influence of the IL concentration is also evaluated at molar concentrations between 1% and 4%. The simulation results indicate that the use of IL additives can affect the physical CO 2 solubility, surface tension, and the localization of CO 2 around the [OH] − ions at the gas–liquid interface. It is also evident that the choice of cations, anions, and IL concentration determines the extent to which the IL additives impact the local physicochemical properties. Physical dissolution, diffusive transport, and interaction with [OH] − are critical intermediate steps toward reactive CO 2 capture using a liquid absorbent. Hence, the improvement in one or more of these properties, aided by IL additives, is expected to improve the overall CO 2 capture performance. Experiments reaffirmed the impact of IL additives on CO 2 capture performance and the sensitivity to the choice of the cation, anion, and concentration of the IL additive.

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

Warm-season net CO 2 uptake outweighs cold-season emissions over Alaskan North Slope tundra under current and RCP8.5 climate

Abstract Arctic warming has increased vegetation growth and soil respiration during recent decades. The rate of Arctic warming will likely amplify over the 21st century. Previous studies have revealed that the most severe Arctic warming occurred during the cold season (September to May). The cold-season warming has posited significant CO 2 emissions to the atmosphere via respiration, possibly offsetting warm-season (June to August) net CO 2 uptake. However, prevailing Earth system land models poorly represent cold-season CO 2 emissions, making estimates of Arctic tundra annual CO 2 budgets highly uncertain. Here, we demonstrate that an improved version of the energy exascale Earth system model (E3SM) land model (ELMv1-ECA) captures the large amount of cold-season CO 2 emissions over Alaskan Arctic tundra as reported by two independent, observationally-constrained datasets. We found that the recent seven-decades warming trend of cold-season soil temperature is three times that of the warm-season. The climate sensitivity of warm-season net CO 2 uptake, however, is threefold higher than for the cold-season net CO 2 loss, mainly due to stronger plant resilience than microbial resilience to hydroclimatic extremes. Consequently, the modeled warm-season net CO 2 uptake has a larger positive trend (0.74 ± 0.14 gC m −2 yr −1 ) than that of cold-season CO 2 emissions (0.64 ± 0.11 gC m −2 yr −1 ) from 1950 to 2017, supported by enhanced plant nutrient uptake and increased light- and water-use efficiency. With continued warming and elevated CO 2 concentrations under the representative concentration pathway (RCP) 8.5 scenario, the increasing rate of warm-season net CO 2 uptake is more than twice the rate of cold-season emissions (1.33 ± 0.32 gC m −2 yr −1 vs 0.50 ± 0.12 gC m −2 yr −1 ), making the modeled Alaskan Arctic tundra ecosystem a net CO 2 sink by 2100. However, other geomorphological and ecological disturbances (e.g. abrupt permafrost thaw, thermokarst development, landscape-scale hydrological changes, wildfire, and insects) that are not considered here might alter our conclusion.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Development of Carbon Molecular Sieves Hollow Fiber Membranes based on Polybenzimidazole Doped with Polyprotic Acids with Superior H 2 /CO 2 Separation Properties (Final Report)

The goal of this project was to develop a highly efficient membrane-based process to capture CO 2 from coal-derived syngas with 95% CO 2 purity, achieving the cost of electricity (COE) 30% below the baseline capture approaches (i.e., Selexol process) when coupled with the advancement in other areas of the power generation facility. Our core approach is based on high-permeance hollow fiber membranes (HFMs) with superior H 2 /CO 2 separation properties at the syngas process conditions, which can then be further utilized to design membrane reactors for process intensification of H 2 production and purification and CO 2 capture. Three organizations with complementary skills collaborated to achieve the goal, including the University at Buffalo (UB), Los Alamos National Laboratory (LANL), and Trimeric Corporation (Trimeric). We formulated logical steps to bring the membrane technology from Technology Readiness Level (TRL) 3 (Experimental proof of concept) to TRL 4 (Laboratory scale validation in relevant environment). During the budget period (BP) 1, we screened various polymeric materials and identified polybenzimidazole doped with inorganic polyprotic acids as the desirable platform. The acid doping increases the H 2 /CO 2 selectivity, and the sequential carbonization increases H 2 permeability while retaining the high selectivity. By manipulating the acid type and doping level and the carbonization temperature, we demonstrated advanced carbon molecular sieving (CMS) materials with H 2 permeability of above 200 Barrer (1 Barrer = 10 -10 cm 3 (STP) cm cm -2 s -2 cmHg -1 ) and H 2 /CO 2 selectivity of above 40 at 200-300°C with simulated syngas containing CO and water vapor. For example, the PBI-(H 3 PO 4 ) 0.11 carbonized at 700 °C exhibits H 2 permeability of 200 Barrer and H 2 /CO 2 selectivity of 60 at 200 °C, and H 2 permeability of 240 Barrer and H 2 /CO 2 selectivity of 54 at 225 °C, which meets the targeted properties and surpasses Robeson’s upper bound. During the BP2, we focused on the conversion of the advanced CMS materials to stable HFMs. Membranes with H 2 permeance of 1,090 GPU (1 GPU = 10 -6 cm 3 (STP) cm -2 s -2 cmHg -1 ) and H 2 /CO 2 selectivity of 57 at 300 °C were successfully fabricated. The effects of temperature, gas compositions, pressure, and time on the separation properties were systematically investigated. Pencil modules were continuously evaluated for 219 h (dry pure gas) and 669 h (dry simulated syngas) and showed initial decline in permeance and increased H 2 /CO 2 selectivity over time, ultimately achieving a steady state stable value, indicating that the ageing phenomena in the nanoporous structures of the membranes during the test. Membrane reactors were fabricated based on the CMS membranes and evaluated for water-gas shift (WGS) reaction. The use of membranes slightly improves the conversion of the CO. However, parametric tests of the membrane reactors at various temperatures and flow rates need to be conducted, as well as the membranes with improved separation performance. We performed a sensitivity analysis on the impact of H 2 /CO 2 selectivity on the COE based on a hybrid process of a membrane unit and cryogenic unit developed by Membrane Technology and Research, Inc. (MTR). Three H 2 /CO 2 selectivity (40, 60, and 15) cases were developed and compared with the baseline capture process (Case B5B) provided by the DOE report. Increasing the membrane H 2 /CO 2 selectivity reduces COE, but the rate of the decrease of COE also diminishes. The COE values for H 2 /CO 2 selectivities of 40 and 60 were nearly the same. As the H 2 /CO 2 selectivity increases, the inert recycling decreases, leading to smaller equipment, less auxiliary power requirements, and less heating, cooling, and refrigeration duty. The refrigeration system used to liquefy the CO 2 is the most expensive piece of equipment and consumes the most electricity within the CO 2 capture process. Increasing the CO 2 concentration in the recycle stream would improve the economics of the process by reducing the refrigeration duty requirement of the unit and also allow for higher liquefaction temperatures. The high H 2 -selective membrane developed by our team may be applicable in other separation processes where lower pressure H 2 retains value. Typically, hydrogen retains its pressure when it is separated from syngas components. Residual components may be used as low-quality fuel and then vented to the atmosphere. Applications might include control of H 2 /CO ratios or mitigation of the water gas shift reaction by CO 2 recycling to the feed of a gasifier or steam methane reformer. To summarize, we have developed industrial HFMs with the best H 2 /CO 2 separation performance reported in the literature. The membranes demonstrate stability with simulated syngas and show great potential for membrane reactors for WGS reactions, lowering the cost of blue H 2 production.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2024

Techno-Economic Analysis and Market Potential of Geological Thermal Energy Storage (GeoTES) Charged With Solar Thermal and Heat Pumps

In this project, we developed a techno-economic analysis (TEA) model that can be used to evaluate the viability of a proposed Geological Thermal Energy Storage (GeoTES) design. This MATLAB-based model integrates distinct subsystem models for the reservoir, wells, power cycle, and solar field to capture their distinct characteristics. It applies this approach in simulating GeoTES storage and dispatch operations for durations ranging from hourly to seasonal. Using cases studies based on GeoTES designs provided by industry partners - Premier Resource Management (PRM) and EarthBridge Energy - we validated the TEA model estimations of system performance and costs (such as thermal and electrical power/energy inflow and outflow, capital costs, and levelized costs of energy and storage) for both concentrating solar thermal (CST) and Carnot Battery (CB) pairings with GeoTES (CST-GeoTES and CB-GeoTES). For the CST-GeoTES case, the model was validated against the proposed system designed by PRM. It showed good agreement with PRM's estimations when well and pump costs derived from PRM's estimations were used. When GETEM-based costs were used, there was a slight overprediction due to GETEM's project/site agnostic assumption of these costs. From a sensitivity analysis perspective, the levelized cost of electricity (LCOE) of the CST-GeoTES case was most sensitive to well flow rate and the charging temperature. An optimal design scenario resulted in an LCOE of 0.11 $\$$/kWhe. CST-GeoTES can also provide a source of heat to meet seasonal demands. With 12-hour and 24-hour levelized cost of heat (LCOH) of 0.018 $\$$/kWhth and 0.022 $\$$/kWhth, respectively, CST-GeoTES could be competitive in the California market with an average industrial price of natural gas in California between 0.041-0.047 $\$$/kWhth. The levelized cost of storage (LCOS) for CST-GeoTES depends on the energy storage duration. Although the LCOS is relatively higher for shorter durations (e.g., ~0.50 $\$$/kWhe for 1 hour of storage), it is an order of magnitude lower (0.06 $\$$/kWhe) for longer storage durations and competitive with lithium-ion batteries (beyond 12 hours of storage) and molten-salt thermal energy storage (beyond 32 hours). Energy. Three options were explored and applied to the EarthBridge case study: (1) A Carnot Battery design using R125 working fluid with both hot and cold storage; (2) A Carnot Battery design using R125 working fluid with only hot storage; (3) A Carnot Battery using a commercially available heat pump with carbon dioxide (CO2) working fluid and hot storage only. The CB-GeoTES with cold storage only had a slight (round-trip) efficiency advantage over the system without (43.4% vs. 42.8%). This is because the cold storage is limited by the freezing point of water, so the cold storage is not much colder than the environment. The system using commercially available technologies was the least efficient - partly because different cycles were used in the heat pump (CO2) and heat engine (binary cycle) which leads to some inefficiencies. Using the commercially available design, the levelized cost of energy (LCOS) from the model (0.10 $\$$/kWhe) was higher than that estimated by EarthBridge (0.068 $\$$/kWhe). This is because of the low round-trip (38.7%) efficiency of the commercially available design. Sensitivity analysis reveals that the model is most sensitive to electricity price. Including electricity price in the TEA for CB-GeoTES leads to an increase in LCOS from the base value to 0.25 $\$$/kWhe. To determine storage sites suitable for GeoTES, we gathered and analyzed geological, petrophysical, and geophysical data of oil and gas reservoir and aquifers in California and Texas. We down-selected possible sites based on cut-off values for site characteristics (e.g., reservoir temperature, formation thickness, permeability, porosity, depth, and brine salinity) and preliminary costs. Using this approach, the Carrizo-Wilcox, Yegua-Jackson, and Dockum brackish aquifers in Texas were identified as having the highest suitability. Similarly, in the central California region, the White Wolf, Belridge South Tulare, and Belridge South Reef Ridge were the most suitable. Going further, we assessed the storage potential in the selected sites. To do this we developed distributions of reservoir characteristic data and applied a Monte Carlo-based analysis to account for intrinsic uncertainty in the acquired data. The analysis revealed that the Carrizo-Wilcox aquifer had the highest storage potential with a mean capacity of 554 TWhth (i.e., 63 TWhe). The estimated capacity serves as an upper limit of storage potential given that not all fields in the basin will be developed. We participated in multiple outreach activities including conference presentations, panel session discussions, and the facilitation of a GeoTES workshop at the NREL Golden campus.

15 GEOTHERMAL ENERGY↗
NASA NTRS2015

Opportunities and Strategies for Testing and Infusion of ISRU in the Evolvable Mars Campaign

HE Evolvable Mars Campaign (EMC) is developing the plans and systems needed for a robust, evolutionary strategy to explore cis-lunar space, the Mars sphere of influence (including the moons of Mars), and the surface of Mars. Recently, the emphasis of NASA's plans has changed to focus on the prolonged pioneering of space, rather than focusing on a single crewed mission as the ultimate goal. A sustainable, pioneering vision of space would include in-situ resource utilization (ISRU) in multiple forms and at multiple destinations: atmospheric capture of Mars CO2 and/or volatiles for consumables and propellants, regolith for bulk and refined materials, and in-situ manufacturing at the Moon, Mars, and other bodies. These resources would enable a reduction in the logistical needs from Earth for future missions, thus preparing the way for a sustained presence on Mars. Although the EMC initially relies only on propellant production for the Mars ascent vehicle via ISRU, one of its primary objectives is to prospect at every EMC destination to understand the potential for ISRU; this will permit true pioneering to be enabled after the first crew arrives at Mars. Recent and ongoing analysis has considered the possible prospecting measurements that can be performed at the asteroid returned to cis-lunar space by the Asteroid Robotic Redirect Mission (ARRM), at the lunar surface, at Phobos and Deimos, and on the surface of Mars to identify available resources for future use. These opportunities will be available on missions currently in the Evolvable Mars Campaign construct, and will also facilitate the testing and demonstration of resource acquisition, processing, storage, and useage technologies that can play a role in later missions. This analysis has also led to the identification of several objectives that should be targeted during the missions building up to and including the initial crewed missions. These objectives are mapped to strategies for incorporating ISRU to support resource cycle closure and reduce mass requirements from Earth. This analysis has yielded engineering constraints, based on ISRU, that impact the evaluation of landing sites for missions to the surface of Mars. The terrain of a particular site must be sufficiently flat to permit ISRU systems, as well as ancillary systems such as power and propellant storage tanks, to be landed, moved into position, set up, and operated. Water must be accessible in a form that can be acquired via ISRU, in quantities that align with demands. The chosen method of acquiring and processing water should align with the available resources at a particular site, and that site must have sufficient quantities to meet the requirements (based on crew consumables and propellant demands). Lower altitude landing sites are preferred, as the increase in density can facilitate carbon dioxide acquisition from the atmosphere. Another preference is for sites with a greater ability to move regolith for civil engineering purposes; for example, this would be conducive to both bulk regolith uses (such as the manufacture of berms), and processed regolith uses (such as microwave sintering).

Evolvable Mars Campaign↗
DOE OSTI2024

Assessment of the impacts of renewable energy variability in long-term decarbonization strategies

To meet the nationally determined contributions proposed by the countries that signed the Paris Agreement, investments must be made in renewable generation technologies such as solar and wind. However, due to their high variability, these technologies pose challenges in terms of meeting demand or generating excess electricity. For this reason, energy system models are designed to capture this variability by considering flexibility technologies. Nevertheless, it is important to note that some energy system models lack integration with other sectors. Therefore, integrated assessment models have been employed to evaluate mitigation strategies, as they endogenously consider the linkages between energy and non-energy sectors. In addition, due to their complexity, these models do not account for the variability of renewable resources. Hence, this research aims to address this issue. Here, this work represents the first attempt to evaluate how the introduction of hourly resolution affects the outcomes of integrated assessment models, specifically focusing on the Global Change Analysis Model (GCAM). We employ a soft-linking approach between the GCAM and the Highway to Renewable Energy Systems model (H2RES, an hourly level energy system model) to accomplish this. The proposed approach is tested using Chile’s Nationally Determined Contributions under different hydrological profiles in the power sector. The results show that it is possible to use the capacity obtained from the Global Change Analysis Model and implement it on an hourly scale. However, the feasibility of implementation depends on high levels of flexibility technologies, such as battery energy storage. When given the choice of investments in renewable sources and flexible technologies, the optimal dispatch of the H2RES model show small differences than those obtained by GCAM-Chile. H2RES differs from GCAM-Chile in approximately 5% for wind and 3% for solar electricity generation in the year 2050. However, feasible integration of significant renewable sources is obtained with relatively high Critical Excess Electricity Production levels, reaching 20% in 2050. This excess electricity is attributed to the necessity for flexible technologies to manage the intermittency of renewables sources when hourly profiles of such sources are considered.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2024

SUBTASK 1.6 – BASIN ELECTRIC CARBON STORAGE RESEARCH PROJECT: NOVEL MONITORING TECHNIQUES

The Energy & Environmental Research Center (EERC) conducted baseline activities associated with an applied research project at Basin Electric Power Cooperative’s (Basin’s) carbon capture and storage (CCS) site in Beulah, North Dakota, to establish novel carbon storage-monitoring techniques as commercial methods under Cooperative Agreement No. DE-FE0024233, Subtask 1.6. The following report summarizes the baseline activities performed and briefly describes the subsequent (operational monitoring) activities that have been proposed to the U.S. Department of Energy (DOE) as part of the overall project to develop and demonstrate novel monitoring techniques at North America’s largest permitted CCS operation. Dakota Gasification Company (DGC), a wholly owned subsidiary of Basin, owns and operates the Great Plains Synfuels Plant (GPSP) approximately 5 miles northwest of the town of Beulah, North Dakota (Figure 1). In 2023, DGC received approval from the North Dakota Industrial Commission (NDIC) to develop a storage facility on-site for injecting a stream of carbon dioxide (CO2) captured from GPSP. DGC will transport the captured CO2 stream with approximately 6.8 miles of transmission lines that extend north of GPSP and inject >1 million tonnes (MMt) of CO2 annually (>1 MMt/yr) over a 12-year period with up to six underground injection control (UIC) Class VI-compliant injection wells completed in the Broom Creek Formation, a predominantly sandstone reservoir and saline aquifer underlying GPSP. The Broom Creek Formation lies approximately 5900 feet (ft) below ground surface (bgs) at GPSP. The commercial scale (i.e., >1 MMt/yr) of DGC’s permitted carbon storage project is ideal for developing and testing the novel monitoring techniques included within Subtask 1.6. The goals of this project are to demonstrate 1) the cost-effectiveness of novel monitoring technologies included as part of this research, 2) technology capability for tracking the CO2 plume and/or associated pressure response in the subsurface and monitoring out-of-zone migration, and 3) compliance with UIC Class VI program requirements. The research activities proposed for the overall project include 1) design of an automated, integrated, modular (AIM) monitoring station; 2) time-lapse electromagnetic (EM) field surveys; 3) drone-based surveillance studies; 4) time-lapse monitoring with seismic methods; 5) advanced wellbore-monitoring methods; 6) deployment of an AIM monitoring network; 7) EM monitoring of CO2 with real-time data processing; 8) continued seasonal drone-based surveillance studies; 9) seismic monitoring with passive and active surveys; and 10) wellbore monitoring with nuclear magnetic resonance (NMR) for near-surface characterization. Completion of Activities 1.0–5.0 (baseline activities) are described in this report. Upon authorization of funding by DOE, the EERC will initiate Activities 6.0– 10.0 (operational monitoring activities). Current state-of-the-art (SOA) carbon storage-monitoring techniques require countless labor hours dedicated to the acquisition of data. Once data are gathered, these SOA techniques often rely on commercial facilities to process raw data from the field. However, it is anticipated that next-generation monitoring techniques, such as those being demonstrated, will lower acquisition footprints, be less operationally intensive, and improve data acquisition efficiencies. These new techniques are more conducive to the application of machine learning, artificial intelligence, and automation, thus providing a pathway for integration into active control systems, informing site operability, and improving the integration of data for future CCS projects across the United States. Additionally, reclaimed and active mining lands are present within the project site, creating a unique opportunity to demonstrate the effectiveness of remote sensing and surface-based geophysics monitoring techniques at similar project sites that may include disturbed, unconsolidated, or actively excavated near-surface environments. The efforts included in the overall project will produce necessary designs, learnings, and data acquired during the baseline and operational monitoring periods that are necessary for time-lapse demonstration and validation of the described monitoring techniques. In addition, it is anticipated that the monitoring technologies included in this study will be compliant with UIC Class VI requirements to enable the potential for implementation at other CCS sites across the United States.

42 ENGINEERING↗
DOE OSTI2021

Experimental study and demonstration of pilot-scale, dry feed, oxy-coal combustion under pressure

In this paper, we discuss how pressurized oxy-combustion is a promising technology for low-carbon, fossil fuel utilization. It has the potential of improved efficiency and economics compared with conventional atmospheric pressure oxy-combustion. Washington University in St. Louis has proposed a new pressurized oxy-combustion process, namely Staged Pressurized Oxy-Combustion, which has the potential to improve further the plant efficiency, operational flexibility, and economics. This process burns pulverized coal in a pressurized, oxy-combustion environment, which has not been demonstrated in a pilot-scale system before. To address this gap, a 100 kWth pressurized oxy-combustion facility was designed and constructed. This facility has a unique burner and furnace design featuring a co-axial, low-mixing flow field, which is drastically different from conventional coal-fired boiler designs where strong mixing is sought by introducing swirl or recirculating flows. This work aims to present the first pilot-scale experimental results of a dry-feed, pressurized oxy-combustion system. The tests focused on exploring flame stability and shape, char burnout, and fine particulate matter formation. Testing results suggest that the burner has excellent flame stability. The flame shape is consistent with the design philosophy and agrees with large eddy simulations. Importantly, complete char combustion can be achieved with an oxygen mole fraction in the flue gas of only 0.8%, as opposed to a required value of ~3% for conventional atmospheric pressure air-fired or oxyfuel combustion, which reduces the costs of both oxygen generation upstream and oxygen removal downstream. The testing results show promise for dry-feed, pressurized oxy-combustion, and the new burner and furnace design.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2020

2D Retrieval Frameworks for Hot Jupiter Phase Curves

Spectroscopic phase curves provide unique access to the three-dimensional properties of transiting exoplanet atmospheres. However, a modeling framework must be developed to deliver accurate inferences of atmospheric properties for these complex data sets. Here, we develop an approach to retrieve temperature structures and molecular abundances from phase curve spectra at any orbital phase. In the context of a representative hot Jupiter with a large day–night temperature contrast, we examine the biases in typical one-dimensional (1D) retrievals as a function of orbital phase/geometry, compared to two-dimensional (2D) models that appropriately capture the disk-integrated phase geometry. We guide our intuition by applying our new framework on a simulated Hubble Space Telescope (HST)+Spitzer phase curve data set in which the “truth” is known, followed by an application to the spectroscopic phase curve of the canonical hot Jupiter, WASP-43b. We also demonstrate the retrieval framework on simulated James Webb Space Telescope (JWST) phase curve observations. We apply our new geometric framework to a joint fit of all spectroscopic phases, assuming longitudinal molecular abundance homogeneity, resulting in an a factor of 2 improvement in abundances precision when compared to individual phase constraints. With a 1D retrieval model on simulated HST+Spitzer data, we find strongly biased molecular abundances for CH{sub 4} and CO{sub 2} at most orbital phases. With 2D, the day and night profiles retrieved from WASP-43b remain consistent throughout the orbit. JWST retrievals show that a 2D model is strongly favored at all orbital phases. Based on our new 2D retrieval implementation, we provide recommendations on when 1D models are appropriate and when more complex phase geometries involving multiple TP profiles are required to obtain an unbiased view of tidally locked planetary atmospheres.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2016

Characterization of Carbon Dioxide Washout Measurement Techniques in the Mark-III Space Suit

Providing adequate carbon dioxide (CO2) washout is essential to the reduction of risk in performing suited operations. Long term CO2 exposure can lead to symptoms such as headache, lethargy, dizziness, and in severe cases can lead to unconsciousness and death. Thus maintaining adequate CO2 washout in both ground testing and during in flight EVAs is a requirement of current and future suit designs. It is necessary to understand the inspired CO2 of suit wearers such that future requirements for space suits appropriately address the risk of inadequate washout. Testing conducted by the EVA Physiology Laboratory at the NASA Johnson Space Center aimed to characterize a method for noninvasively measuring inspired oronasal CO2 under pressurized suited conditions in order to better inform requirements definition and verification techniques for future CO2 washout limits in space suits. Prior work conducted by the EPL examined several different wearable, respirator style, masks that could be used to sample air from the vicinity surround the nose and mouth of a suited test subject. Previously published studies utilized these masks, some being commercial products and some novel designs, to monitor CO2 under various exercise and flow conditions with mixed results for repeatability and/or consistency between subjects. Based on a meta-analysis of those studies it was decided to test a nasal cannula as it is a commercially available device that is placed directly in the flow path of the user as they breathe. A nasal cannula was used to sample air inhaled by the test subjects during both rest and exercise conditions. Eight subjects were tasked with walking on a treadmill or operating an arm ergometer to reach target metabolic rates of 1000, 2000, and 3000 BTU/hr. Suit pressure was maintained at 4.3 psid for all tests, with supply flow rates of 6, 4, and 2 actual cubic feet per minute depending on the test condition. Each test configuration was conducted twice with subjects breathing either through their nose only, or however they felt comfortable. By restricting breathing through a single orifice, we are able to more accurately define exactly what flow stream the sampled CO2 is taken from. Oronasal CO2 was monitored using real time infrared gas analyzers fed via sample tubes connected to the nasal cannula within the suit. Two additional sampling tubes were placed at the head and chin of the test subject, in an effort to capture CO2 concentrations across the entire flow stream of the Mark-III vent system (flow path is head to neck). Metabolic rate was calculated via the exhaust CO2 concentration and used to adjust subject workload on either the treadmill or arm ergometer until the target was reached. Forward work will aim to characterize the historically accepted minimum ppCO2 in suit during EVA by repeating this study in the Extravehicular Mobility Unit (EMU) space suit. This will help to define washout requirements for future suits, be they NASA (e.g. Z-2) or Commercial Crew designed. Additionally it is important to determine the functional consequences of CO2 exposure during EVA. Severe CO2 symptoms are a result of very high concentration, acute exposures. While long term, low concentration exposures have been shown to result in slight cognitive decline, symptoms resolve upon quickly returning to nominal concentrations and it remains unknown the impact that minor deficits in cognitive performance can have on EVA performance.

Norcross, J.↗
NASA NTRS2012

Real-Time X-ray Radiography Diagnostics of Components in Solid Rocket Motors

Solid rocket motors (SRMs) typically use nozzle materials which are required to maintain their shape as well as insulate the underlying support structure during the motor operation. In addition, SRMs need internal insulation materials to protect the motor case from the harsh environment resulting from the combustion of solid propellant. In the nozzle, typical materials consist of high density graphite, carbon-carbon composites and carbon phenolic composites. Internal insulation of the motor cases is typically a composite material with carbon, asbestos, Kevlar, or silica fibers in an ablative matrix such as EPDM or NBR. For both nozzle and internal insulation materials, the charring process occurs when the hot combustion products heat the material intensely. The pyrolysis of the matrix material takes away a portion of the thermal energy near the wall surface and leaves behind a char layer. The fiber reinforcement retains the porous char layer which provides continued thermal protection from the hot combustion products. It is of great interest to characterize both the total erosion rates of the material and the char layer thickness. By better understanding of the erosion process for a particular ablative material in a specific flow environment, the required insulation material thickness can be properly selected. The recession rates of internal insulation and nozzle materials of SRMs are typically determined by testing in some sort of simulated environment; either arc-jet testing, flame torch testing, or subscale SRMs of different size. Material recession rates are deduced by comparison of pre- and post-test measurements and then averaging over the duration of the test. However, these averaging techniques cannot be used to determine the instantaneous recession rates of the material. Knowledge of the variation in recession rates in response to the instantaneous flow conditions during the motor operation is of great importance. For example, in many SRM configurations the recession of the solid propellant grain can drastically alter the flow-field and effect the recession of internal insulation and nozzle materials. Simultaneous measurement of the overall erosion rate, the development of the char layer, and the recession of the char-virgin interface during the motor operation can be rather difficult. While invasive techniques have been used with limited success, they have serious drawbacks. Break wires or make wire sensors can be installed into a sufficient number of locations in the charring material from which a time history of the charring surface can be deduced. These sensors fundamentally alter the local structure of the material in which they are imbedded. Also, the location of these sensors within the material is not known precisely without the use of an X-ray. To determine instantaneous recession rates, real-time X-ray radiography (X-ray RTR) has been utilized in several SRM experiments at PSU. The X-ray RTR system discussed in this paper consists of an X-ray source, X-ray image intensifier, and CCD camera connected to a capture computer. The system has been used to examine the ablation process of internal insulation as well as nozzle material erosion in a subscale SRM. The X-ray source is rated to 320 kV at 10 mA and has both a large (5.5 mm) and small (3.0 mm) focal spot. The lead-lined cesium iodide X-ray image intensifier produces an image which is captured by a CCD camera with a 1,000 x 1,000 pixel resolution. To produce accurate imagery of the object of interest, the alignment of the X-ray source to the X-ray image intensifier is crucial. The image sequences captured during the operation of an SRM are then processed to enhance the quality of the images. This procedure allows for computer software to extract data on the total erosion rate and the char layer thickness. Figure 1 Error! Reference source not found.shows a sequence of images captured during the operation the subscale SRM with the X-ray RTR system. The X-rayTR system, alignment procedure, uncertainty determination, and image analysis process will be discussed in detail in the full manuscript.

Cortopassi, A. C.↗
DOE OSTI2024

Achieving Unprecedented CO 2 Utilization InCO 2 Concrete™: System Design, Product Development and Process Demonstration

Anthropogenic sources of carbon dioxide are generated from a number of sources, but the key among these are ordinary Portland cement (OPC) production and combustion of fossil fuels. Cement production is the largest global CO 2 source from the mineral decomposition of carbonates. This is due to the clinkering process whereby limestone (mainly consisting of CaCO 3 ) is decomposed into CaO and CO 2 , and combined with silica rich clays at high temperatures to form clinkers (i.e. the four key minerals that comprise cement). The high temperature range of 1400 – 1550°C required for this process accounts for up to 60% of the generated CO 2 from cement production. Combination of the limestone decomposition and thermal requirements of the clinkering process causes cement production to contribute 8-9% of annual global CO 2 emissions. Combustion of fossil fuels (coal, oil and gas) was shown to contribute a much larger portion of global CO 2 emissions. As of 2018, combustion of fossil fuels accounted for 65% of global CO 2 , where 41% was derived from stationary sources for electricity and heat generation and the other 24% was related to transport. To reduce these contributions, key steps forward in CO 2 utilization technologies are required. Therefore, a CO 2 mineralization technology (CO 2 mineralization concrete) to reduce the OPC content in concrete, while utilizing flue gas emissions from fossil fuel combustion has been developed to address both areas simultaneously. This Reversa™ technology utilizes low-carbon cementation agents produced by in situ CO 2 mineralization (“mineral carbonation reactions”) to offer a promising alternative to OPC. CO 2 mineralization relies upon the reaction of dissolved CO 2 with inorganic alkaline reactants to precipitate mineral carbonates (e.g., CaCO 3 ), which bind proximate particles and achieve cementation. Herein, a concrete green body, which is composed of a mixture of binder, water, and mineral aggregates, is exposed to CO 2 borne in industrial flue gas streams. This manner of CO 2 mineralization allows the production of construction components that feature equivalent engineering attributes as their OPC-based counterparts while featuring a much smaller embodied carbon intensity (eCI). The purpose of this project is to demonstrate the feasibility of the Reversa process evolving from a TRL-3 technology at the bench-scale up to TRL-6 technology at the pilot-scale. The reliability of the Reversa technology was tested to prove the effective production of three standard industrial concrete products selected during the course of the project. The results detailed herein will demonstrate the evolution of this technology to the industrial scale. The culmination of this work resulted in 9 production runs completed at the National Carbon Capture Center (NCCC), Wilsonville, AL, using natural gas (NG) flue gas as the CO 2 source. Over the course of the production runs at NCCC, the CO 2 utilization as a function of time, 24-h CO 2 uptake, electricity usage, and 28-d net area compressive strength recorded for each run. Collection of this data will be used to determine the success of the demonstration goals: (1) achieving in excess of 0.2gCO 2 /g reactant , (2) achieving greater than 50% reduction in global warming potential compared to standard produced units, and (3) ensuring compliance of carbonated concrete with industry standard specifications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Microstructure Experiments-Enabled MARMOT Simulations of SiC/SiC-based Accident Tolerant Nuclear Fuel System

We have undertaken an experimental-computational project that addresses a few key technology gaps associated with the use of SiC/SiC composites for light water reactor fuel cladding. Two principal endeavors in this project are to assess the irradiation-induced microstructural changes and swelling in SiC/SiC composites, and to characterize and model the porous oxide surface layer (when exposed to steam) along SiC recession that is detrimental to the clad integrity under accident conditions. The project tasks are: (i) ion irradiation and characterization (University of Tennessee, Knoxville), (ii) mechanical tests and analysis (University of South Carolina), (iii) steam exposure tests (Oak Ridge National Laboratory), (iv) electron microscopy and spectroscopic characterization (NC State University), (v) x-ray microscopy and reconstruction (University of South Carolina and NC State University), (vi) phase field modeling and simulations (NC State University and Idaho National Laboratory). The effects of 10 MeV Au ion irradiation at 350°C on the microstructure evolution in SiC/SiC composites are investigated at doses up to 400 displacements per atom (dpa) at the University of Tennessee, Knoxville. Atomic force microscopy and optical profilometry reveal irradiation induced axial and radial shrinkage of the fibers for doses greater than 10 dpa. Based on detailed electron microscopy characterization, the primary cause of the fiber shrinkage is attributed to irradiation-induced loss of carbon packets. Additionally, the multilayer PyC interface is observed to portray high resistance to irradiation damage. The mechanical response and failure mechanisms of un-irradiated samples is also assessed through loading tests and X-ray imaging at the University of South Carolina. Steam exposure tests are performed at the Oak Ridge National Laboratory in a facility that represents a reactor pressure vessel under a loss-of-coolant-accident scenario. The samples that are analyzed methodically in this report are tested for 32/31 hours at 1200°C with a velocity of 0.25 cm/s for the pressures: 0.1 MPa, 0.45 MPa, 0.92 MPa and 1.38 MPa. Scanning/transmission electron microscopy analysis conducted at the NC State University (NCSU) shows that the oxide layer thickness increases with the steam pressure. While the oxide layer is crystalline (α- cristobalite) for the pressures 0.45 MPa, 0.92 MPa and 1.38 MPa, the layer is amorphous at 0.1 MPa. Results from Raman spectroscopy have also confirmed the formation of α-cristobalite phase of SiO₂. The abrupt increase in the integrated Raman intensity ratio between steam pressures 0.1 and 0.45 MPa suggests the onset of accelerated crystallization. Non-destructive three dimensional X-ray microscopy/tomography (XCT) and computational image processing techniques are employed by the University of South Carolina to probe the porous oxidation features on SiC samples at varying pressures. Interestingly, most pores are observed to be located away from the surface as well as the oxide-SiC interface. The average oxide layer thickness assessed from the XCT analysis is seen to be in excellent agreement with the values determined through scanning electron microscopy analysis for the highest pressures where the oxide layer is relatively more uniform. A phase-field model developed by the NC State University and Idaho National Laboratory for simulating oxidation of SiC by steam captures the paralinear kinetics of SiC oxidation with a high degree of fidelity. Results from quasi-one-dimensional and two dimensional simulations show that the pores with oxidizing species lead to a higher volatilization rate. These simulations indicate that the enhanced apparent volatilization rates at higher pressures observed in experiments can be rationalized by the increased volatilization from the pores. The project team has also successfully developed the capability to import images from experiments for realistic evolution of the oxidizing microstructure.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1994

Carbon, nitrogen, magnesium, silicon, and titanium isotopic compositions of single interstellar silicon carbide grains from the Murchison carbonaceous chondrite

Seven hundred and twenty SiC grains from the Murchison CM2 chondrite, ranging in size from 1 to 10 micrometers, were analyzed by ion microprobe mass spectrometry for their C-isotopic compositions. Subsets of the grains were also analyzed for N (450 grains), Si (183 grains), Mg (179 grains), and Ti (28 grains) isotopes. These results are compared with previous measurements on 41 larger SiC grains (up to 15 x 26 micrometers) from a different sample of Murchison analyzed by Virag et al. (1992) and Ireland, Zinner, & Amari (1991a). All grains of the present study are isotopically anomalous with C-12/C-13 ratios ranging from 0.022 to 28.4 x solar, N-14/N-15 ratios from 0.046 to 30 x solar, Si-29/Si-28 from 0.54 to 1.20 x solar, Si-30/Si-28 from 0.42 to 1.14 x solar, Ti-49/Ti-48 from 0.96 to 1.95 x solar, and Ti-50/Ti-48 from 0.94 to 1.39 x solar. Many grains have large Mg-26 excesses from the decay of Al-26 with inferred Al-26/Al-27 ratios ranging up to 0.61, or 12,200 x the ratio of 5 x 10(exp -5) inferred for the early solar system. Several groups can be distinguished among the SiC grains. Most of the grains have C-13 and N-14 excesses, and their Si isotopic compositions (mostly excesses in Si-29 and Si-30) plot close to a slope 1.34 line on a Delta Si-29/Si-28 versus Delta Si-30/Si-28 three-isotope plot. Grains with small C-12/C-13 ratios (less than 10) tend to have smaller or no N-14 excesses and high Al-26/Al-27 ratios (up to 0.01). Grains with C-12/C-13 greater than 150 fall into two groups: grains X have N-15 excesses and Si-29 and Si-30 deficits and the highest (0.1 to 0.6) Al-26/Al-27 ratios; grains Y have N-14 excesses and plot on a slope 0.35 line on a Si three-isotope plot. In addition, large SiC grains of the Virag et al. (1992) study fall into three-distinct clusters according to their C-, Si-, and Ti-isotopic compositions. The isotopic diversity of the grains and the clustering of their isotopic compositions imply distinct and multiple stellar sources. The C- and N-isotopic compositions of most grains are consistent with H-burning in the CNO cycle. These and s-process Kr, Xe, Ba, and Nd suggest asymptotic giant branch (AGB) or Wolf-Rayet stars as likely sources for the grains, but existing models of nucleosynthesis in these stellar sites fail to account in detail for all the observed isotopic compositions. Special problems are posed by grains with C-12/C-13 less than 10 and almost normal and heavy N-isotopic compositions. Also the Si- and Ti-isotopic compositions, with excesses in Si-29 and Si-30 relative to Si-28 and excesses in all Ti isotopes relative to Ti-48, do not precisely conform with the compositions predicted for slow neutron capture. Additional theoretical efforts are needed to achieve an understanding of the isotopic composition of the SiC grains and their stellar sources.

Hoppe, Peter↗
NASA NTRS2003

Mechanical Testing of PMCs under Simulated Rapid Heat-Up Propulsion Environments: In-Plane Compressive Behavior - II

Carbon fiber thermoset polymer matrix composites (PMC) with high temperature polyimide based in-situ polymerized monomer reactant (PMR) resin has been used for some time in applications which can see temperatures up to 550 F. Currently, graphite fiber PMR based composites are used in several aircraft engine components including the outer bypass duct for the GE F-404, exit flaps for the P&W F-100-229, and the core cowl for the GE/Snecma CF6-80A3. Newer formulations, including PMR-II-50 are being investigated as potential weight reduction replacements of various metallic components in next generation high performance propulsion rocket engines that can see temperatures which exceed 550 F. Extensive FEM thermal modeling indicates that these components are exposed to rapid heat-up rates (up to -200 F/sec) and to a maximum temperature of around 600 F. Even though the predicted maximum part temperatures were within the capability of PW-II-50, the rapid heat-up causes significant through-thickness thermal gradients in the composite part and even more unstable states when combined with moisture. Designing composite parts for such extreme service environments will require accurate measurement of intrinsic and transient mechanical properties and the hygrothermal performance of these materials under more realistic use conditions. The mechanical properties of polymers degrade when exposed to elevated temperatures even in the absence of gaseous oxygen. Accurate mechanical characterization of the material is necessary in order to reduce system weight while providing sufficient factors of safety. Historically, the testing of PMCs at elevated temperatures has been plagued by the antagonism between two factors. First, moisture has been shown to profoundly affect the mechanical response of these materials at temperatures above their glass transition temperature while concurrently lowering the material's Tg. Moisture phenomena is due to one or a combination of three effects, i.e., plastization of polymeric material by water, the internal pressure generated by the volatilization of water at elevated temperatures, and hydrolytic chemical decomposition. However, moisture is lost from the material at increasing rates as temperature increases. Second, because PMCs are good thermal insulators, when they are externally heated at even mild rates large thermal gradients can develop within the material. At temperatures where a material property changes rapidly with temperature the presence of a large thermal gradient is unacceptable for intrinsic property characterization purposes. Therefore, long hold times are required to establish isothermal conditions. However, in the service environments high-heating-rates, high temperatures, high-loading rates are simultaneous present along with residual moisture. In order to capture the effects of moisture on the material, holding at- temperature until isothermal conditions are reached is unacceptable particularly in materials with small physical dimensions. Thus, the effects due to moisture on the composite's mechanical characteristics, ie., their so-called analog response, may be instructive. One approach employed in this program was rapid heat-up (approx. 200 F/sec.) and loading of both dry and wet in-plane compressive specimens to examine the effects of moisture on this resin dominated mechanical property of the material.

Stokes, Eric H.↗
DOE OSTI2023

Energy-Community-Geo-Database

Fundamental to understanding evolving infrastructure and technology is understanding the drivers for energy communities that affect where and how infrastructure is placed and used. An Energy Community Geo Database aligned to carbon storage systems will aid stakeholders in decision making around key future infrastructure (e.g., CCS injection locations) placement while helping contextualize these analyses against past and present-day social and environmental attributes. Much of the data required to support analyses are available from authoritative, largely governmental sources, but at present are disparate and require time-consuming acquisition, integration, and upkeep for currency. The CCS-EC-GB v2.0 integrates datasets from various federal agencies and authoritative sources to aid stakeholders and decision makers of the social and environmental factors that might impact the viability of CCS and energy related project implementation. There are 5 categories in the CCS-EC-GB v2 database. Most of the layers within each category have been updated in this version. As compared to the old database, there is 1 new category in the CCS-EC-GB v2 database: infrastructure. This is an evolving project and application will be updated periodically with new datasets and information. Notes for consideration: This database/web map will be updated with additional as new data and information becomes available and has been processed, reviewed, and approved for release. Additional state and federal entity data are planned to be integrated and included in future revisions. Summary layers provided in this application are derived from proprietary layers and do not always contain key features (age, status, or TVD) and therefore might not be shown when data are queried for those features.

CCS,Carbon capture and storage,Carbon storage,U.S.↗
DOE OSTI2022

Impact of Variable Gas Mixtures on Bubble Size Distribution and Mass Transfer in Gas Fermentation Reactors

Gas fermentation has emerged as a promising new technology for the generation of fuels and chemicals from mixtures of greenhouse and energy rich gas streams (CO2/CH4/H2/CO) via microbial bioreaction. Example pathways include biomethanation (CO2/H2 to CH4), biogas upgrading, CO fermentation and wet-waste conversion. Effective Gas-liquid mass-transfer is an important physical phenomenon that determines the design and scale-up of these systems. There is currently a knowledge-gap regarding bubble-size distributions when using a mixture of gases with vastly different properties, which can have a significant impact on overall mass-transfer. For example, hydrogen bubbles are more buoyant compared to other relatively heavier gases (CO2/CH4/CO), resulting in a large distribution of residence times and bubble sizes. This work therefore develops a deeper understanding of bubble dynamics and interphase mass transfer in such heterogenous gas mixtures through well-resolved computational models. We use a detailed multiphase computational-fluid-dynamics (CFD) model to study the impact of gas-mixtures on overall mass-transfer in bubble column and air-lift reactors. The CFD tool previously developed by the authors (1) for simulating aerobic fermentation reactors at scale is used in this study. The Reynolds-averaged mass, momentum, energy, and species transport equations are solved for interpenetrating gas and liquid phase in this model. We use a population balance-based bubble-size-distribution model that is validated against small-scale experiments in our solver. Results pertaining to multiple simulations of gas-fermentation reactors are presented where gas mixtures with varying compositions of CO2/CH4/CO/H2 are imposed at the sparger boundaries. The spatio-temporal variations in bubble-size distribution and mass transfer coefficient is analyzed for varying superficial velocities and gas-compositions for varying sizes of bubble-column and airlift reactors.

BIOMASS FUELS,MATHEMATICS AND COMPUTING↗
DOE OSTI2025

Optimizing Alabama’s CO 2 Storage in Shelby County (Project OASIS) - Deliverable Task 7: Risk Assessment

The “Optimizing Alabama’s CO 2 Storage in Shelby County: Project OASIS” CarbonSAFE Phase II Project seeks to build on regional data sets that demonstrate that the subsurface within Shelby County, Alabama has the potential to store commercial volumes of CO 2 safely, permanently, and economically. The primary target CO 2 Storage Complex is the deep Ketona Dolomite located within a 140 square mile area of the Valley and Ridge Region of Alabama. This deep saline reservoir is beneath a confining system encompassing at least 6,500 ft of shales and other low permeability sediments. Project OASIS drilled a deep stratigraphic test well to confirm the geological properties of the confining system and storage reservoir(s) within the Storage Complex. The geological data was incorporated into numerical models to establish the areal extent of the CO 2 plume and help design the storage site and its monitoring system. The project is managed by the Southern States Energy Board (SSEB), an interstate compact organization consisting of governors and state legislative leaders from sixteen southern states, Puerto Rico, and the U.S. Virgin Islands, as well as an appointee by the President of the United States. The organizational compact provides it with access to state government organizations and legislatures. The Board also maintains an Associate Members program comprised of energy resource companies, utilities, trade groups, academic R&D science and technology experts and energy consultants. Further, the SSEB staff is experienced in managing and coordinating complex energy and environmental programs, from research programs to full-scale design and demonstrations of new and innovative technologies. Project OASIS is a public-private partnership of six entities with multiple principal investigators (PIs). SSEB’s Lead PI and Co-PI are responsible for all aspects of project performance in accordance with the DOE-NETL Cooperative Agreement. SSEB has issued subgrants to Advanced Resources International, Inc., Alabama A&M University, Auburn University, Crescent Resource Innovation, and Oklahoma State University. Advanced Resources International, Inc., issued subgrants to Baker Hughes and Loudon Technical Services for field services

20 FOSSIL-FUELED POWER PLANTS↗