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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Deep Learning Potential For Investigation of Chemical Conversion of CO2 at Air-Reactive Deep Eutectic Solvent Interface

Capturing CO2 from air is urgent to battle against the climate change. Traditional CO2 capture by alkaline solution or aqueous amine has high regeneration cost, equipment corrosion, and amine leakage. Deep eutectic solvents (DESs) are promising alternatives with low corrosion, non-toxicity, and biodegradable nature. Functionalized DESs can capture and convert CO2 at low partial pressures. Developing reactive DESs for efficient CO2 capture needs a foundational understanding of the reaction-transport coupling of CO2 at the air-DES interface. In this study, we develop a deep learning potential (DLP) to investigate the absorption and reaction of CO2 at the air-DES interface (DES: 1-ethyl-3-methylimidazolium 2-cyanopyrrolide ([Emim][2-CNpyr]) and ethylene glycol (EG)). The DLP model allows us to simulate chemical reactions at a lower computational cost with ab initio accuracy. By analyzing reaction free energy surfaces, molecular interactions among CO2, DES components and reaction products, and transport of CO2 through the interface, we identify three main reaction pathways of CO2 at the interface: forming carboxylate with [Emim], carbamate with [2-CNpyr], and carbonate with EG. The mechanistic understanding of CO2 chemisorption at the interface will facilitate the development of novel direct air capture technology using DESs.

Nguyen, Manh Tien↗
NASA NTRS2014

Dual Fan Separator within the Universal Waste Management System

Since NASA's new spacecraft in development for both LEO and Deep Space capability have considerable crew volume reduction in comparison to the Space Shuttle, the need became apparent for a smaller commode. In response the Universal Waste Management System (UWMS) was designed, resulting in an 80% volume reduction from the last US commode, while enhancing performance. The ISS WMS and previous shuttle commodes have a fan supplying air flow to capture feces and a separator to capture urine and separate air from the captured air/urine mixture. The UWMS combined both rotating equipment components into a single unit, referred to at the Dual Fan Separator (DFS). The combination of these components resulted in considerable packaging efficiency and weight reduction, removing inter-component plumbing, individual mounting configurations and required only a single motor and motor controller, in some of the intended UWMS platform applications the urine is pumped to the ISS Urine Processor Assembly (UPA) system. It requires the DFS to include less than 2.00% air inclusion, by volume, in the delivered urine. The rotational speed needs to be kept as low as possible in centrifugal urine separators to reduce air inclusion in the pumped fluid, while fans depend on rotational speed to develop delivered head. To satisfy these conflicting requirements, a gear reducer was included, allowing the fans to rotate at a much higher speed than the separator. This paper outlines the studies and analysis performed to develop the DFS configuration. The studies included a configuration trade study, dynamic stability analysis of the rotating bodies and a performance analysis of included labyrinth seals. NASA is considering a program to fly the UWMS aboard the ISS as a flight experiment. The goal of this activity is to advance the Technical Readiness Level (TRL) of the DFS and determine if the concept is ready to be included as part of the flight experiment deliverable.

Stapleton, Tom↗
DOE OSTI2020

Porosity and hydrophilicity modulated quaternary ammonium-based sorbents for CO 2 capture

Quaternary ammonium (QA)-based polymeric sorbents are known to be effective for CO 2 capture, especially from ultradilute streams like air. In this work, we address two major challenges in QA sorbent design for application in moisture-swing processes, porosity control and hydrophilicity modulation. Facilely substituting porous CO 2 -active components for non-porous ones can enhance the sorption kinetics by 4-fold compared to the state-of-art, and micro–mesoporous structures are identified as optimal porous structures. A method to modulate the hydrophilicity of QA-based sorbents is developed using controlled radical polymerization, incorporating fluorine-containing monomers. The CO 2 sorption capacity and the tolerance towards moisture are simultaneously enhanced via adjustment of the structure and the content of fluorine-containing blocks. Finally, we postulate that porosity and hydrophilicity optimization can make QA-based sorbents adaptive to deployment of scalable moisture-swing processes in varied and complex atmospheric circumstances.

42 ENGINEERING↗
DOE OSTI2024

Impact of cement composition, brine concentration, diffusion rate, reaction rate and boundary condition on self-sealing predictions for cement-CO 2 systems

Geological CO 2 storage (GCS) plays an important role in curbing CO 2 emissions by reducing the carbon footprint of difficult to decarbonize operations and achieve negative CO 2 emissions through activities like Bioenergy with Carbon Capture and Storage (BECCS) and Direct Air Carbon Capture and Storage (DACCS). Leakage of CO 2 through wells is an important concern when it comes to deployment of large-scale GCS. Existing wells in sites that are otherwise suitable for GCS can act as conduits for stored CO 2 to escape the reservoir. There is broad consensus that the main risk of leakage through wellbores is via fractures/damaged pathways. The results from several studies evaluating the permeability evolution of cement fractures in wells upon leakage of CO 2 agree that smaller fracture apertures, slower brine velocities and higher brine residence times promote self-sealing of fractures by mineral precipitation. Quantitatively, however, the differences in sealing conditions are significant and are typically attributed to differences in experimental conditions or model assumptions. Here we examine the sensitivity of our model, describing CO 2 leakage through wellbores, to cement composition, brine concentration, diffusion rates, and reaction rates. We also evaluate the impact of the boundary condition to allow comparisons between observations from experiments performed at constant flow rate and model predictions made at constant pressure conditions. Our results show that diffusion and reactions rates have the most impact on the self-sealing criteria for cement-CO 2 systems. In addition, conditions associated with self-sealing of fractures at constant flow rate require longer fractures, smaller fracture apertures, and slower velocities than under constant pressure.

58 GEOSCIENCES↗
DOE OSTI2023

Big Data Analysis and Technical Review of Regeneration for Carbon Capture Processes

Carbon capture remains an integral technology to mitigate pollution from one of the most prevalent greenhouse gases. CO 2 desorption/absorbent regeneration for both solid- and liquid-based systems is widely recognized as an energy-intensive and costly process operation. Consequently, tremendous work was devoted towards developing new absorbents and regeneration processes to promote their economic feasibility for extensive implementation. In this review, we broadly and deeply review more than 10,000 papers and extract the hidden trends of carbon capture and absorbents regeneration in the past few decades, using a novel data-mining analysis technique. We comprehensively analyzed an array of recent absorbent regeneration methods utilized in post-combustion, pre-combustion, carbon capture from industrial point sources, and direct air carbon capture, with an emphasis on sorbent and solvent-based techniques. In conclusion, advanced regeneration methods in these techniques were illustrated and discussed, followed by recommendations for further research efforts.

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

Isotherm Model for Moisture-Controlled CO 2 Sorption

Moisture-controlled sorption of CO 2 , the basis for moisture-swing CO 2 capture from air, is a novel phenomenon observed in strong-base anion exchange materials. Prior research has shown that Langmuir isotherms provide an approximate fit to moisture-controlled CO 2 sorption isotherm data. However, this fit still lacks a governing equation derived from an analytic model. As such, in this paper we derive an analytic form for an isotherm equation from a bottom-up approach, starting with a fundamental theory for an alkali liquid. In the range of interest relevant to CO 2 capture from air, an isotherm equation for an alkali liquid reduces to a simple analytic form with a single parameter, $K_{\text{eq}}$. In the limit $K_{\text{eq}} \gg 1$, a 2nd order approximation simplifies to a Langmuir isotherm that, however, deviates from experimental data. The isotherm theory for an alkali liquid has been generalized to a strong-base anion exchange material. In a strong-base anion exchange material, water concentration inside a sorbent, [H 2 O], is not large enough to be regarded as constant, which allows us to extend $K_{\text{eq}}$ to $K_{\text{eq(AEM)eff}} = K_{\text{eq(AEM)}} \times$ [H 2 O]$^{–n}$ according to the law of mass action. The final isotherm formula has been validated by experimental data from the literature. For a moisture-controlled CO 2 sorbent, $K_{\text{eq(AEM)eff}}$ varies significantly with moisture content of the sorbent. Depending on moisture level, the observed $K_{\text{eq(AEM)eff}}$ in a specific sorbent ranges from a few times to a few thousand times the value of $K_{\text{eq}}$ of a 2 mol L –1 alkali liquid.

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

Performance of a Natural Gas Solid Oxide Fuel Cell System With and Without Carbon Capture

The fuel cell program at the United States Department of Energy (DOE) National Energy Technology Laboratory (NETL) is focused on the development of low-cost, highly efficient, and reliable fossil-fuel-based solid oxide fuel cell (SOFC) power systems that can generate environmentally-friendly electric power with at least 90 percent carbon capture. NETL’s SOFC technology development roadmap is aligned with near-term market opportunities in the distributed generation sector to validate and advance the technology while paving the way for utility-scale natural gas (NG)- and coal-derived synthesis gas-fueled applications via progressively larger system demonstrations. The present study represents a part of a series of system evaluations being carried out at NETL to aid in prioritizing technological advances along research pathways to the realization of utility-scale SOFC systems, a transformational goal of the fuel cell program. In particular, the system performance of utility-scale NG fuel cell (NGFC) systems with and without carbon dioxide (CO2) capture is presented. The NGFC system analyzed features an external auto-thermal reformer (ATR) feeding the fuel to the SOFC system consisting of planar anode-supported SOFC with separated anode and cathode off-gas streams. In systems with CO2 capture, an air separation unit (ASU) is used to provide the oxygen for the ATR and for the combustion of unutilized fuel in the SOFC anode exhaust along with a CO2 purification unit to provide a nearly pure CO2 stream suitable for transport for usage in enhanced oil recovery operations or for storage in underground saline formations. Remaining thermal energy in the exhaust gases is recovered in a bottoming steam Rankine cycle while supplying any process heat requirements. A reduced order model (ROM) developed at the Pacific Northwest National Laboratory (PNNL) is used to predict the SOFC performance. The ROM, while being computationally effective for system studies, provides other detailed information about the state of the stack, such as the internal temperature gradient, generally not available from simple performance models often used to represent the SOFC. Such additional information can be important in system optimization studies to preclude operation under off-design conditions that can adversely impact overall system reliability. The NGFC system performance was analyzed by varying salient system parameters, including the percent of internal (to the SOFC module) NG reformation—ranging from 0 to 100 percent—fuel utilization, and current density. The impact of advances in underlying SOFC technology on electrical performance was also explored.

solid oxide fuel cell (SOFC), natural gas fuel cel↗
DOE OSTI2023

High-Performance, Hybrid Polymer Membrane for Carbon Dioxide Separation from Ambient Air

The Department of Energy (DOE) seeks to develop carbon capture materials specifically tailored for Direct Air Capture (DAC) processes. Related to this, they require recipients to develop novel DAC materials such as: solvents, membranes, or sorbents that demonstrate high affinities or capacities for carbon dioxide (CO2) at concentrations typically available in air and at near ambient conditions. Toward this, InnoSense LLC (ISL) is developing High-Performance, Hybrid Polymer Membranes (HypoMemTM) for Carbon Dioxide Separation from Ambient Air. HypoMem consists of two major layers. The first layer is the active layer which contains the active ingredients that help to separate CO2 from ambient air. The second is the support layer that provides good mechanical support to have a free-standing membrane without interfering with the properties of the active layer.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2024

Carbon Capture: The Road Ahead

Presentation to the Pittsburgh Regional Carbon Capture Conference at Washington Jefferson College describing the need for carbon capture and its methods.

carbon capture↗
NASA NTRS2005

Remote Sensing Characterization of the Urban Landscape for Improvement of Air Quality Modeling

The urban landscape is inherently complex and this complexity is not adequately captured in air quality models, particularly the Community Multiscale Air Quality (CMAQ) model that is used to assess whether urban areas are in attainment of EPA air quality standards, primarily for ground level ozone. This inadequacy of the CMAQ model to sufficiently respond to the heterogeneous nature of the urban landscape can impact how well the model predicts ozone pollutant levels over metropolitan areas and ultimately, whether cities exceed EPA ozone air quality standards. We are exploring the utility of high-resolution remote sensing data and urban growth projections as improved inputs to the meteorology component of the CMAQ model focusing on the Atlanta, Georgia metropolitan area as a case study. These growth projections include "business as usual" and "smart growth" scenarios out to 2030. The growth projections illustrate the effects of employing urban heat island mitigation strategies, such as increasing tree canopy and albedo across the Atlanta metro area, in moderating ground-level ozone and air temperature, compared to "business as usual" simulations in which heat island mitigation strategies are not applied. The National Land Cover Dataset at 30m resolution is being used as the land use/land cover input and aggregated to the 4km scale for the MM5 mesoscale meteorological model and the (CMAQ) modeling schemes. Use of these data has been found to better characterize low densityhburban development as compared with USGS 1 km land use/land cover data that have traditionally been used in modeling. Air quality prediction for fiture scenarios to 2030 is being facilitated by land use projections using a spatial growth model. Land use projections were developed using the 2030 Regional Transportation Plan developed by the Atlanta Regional Commission, the regional planning agency for the area. This allows the state Environmental Protection agency to evaluate how these transportation plans will affect fbture air quality.

Quattrochi, Dale A.↗
NASA NTRS2005

Urban Landscape Characterization Using Remote Sensing Data For Input into Air Quality Modeling

The urban landscape is inherently complex and this complexity is not adequately captured in air quality models that are used to assess whether urban areas are in attainment of EPA air quality standards, particularly for ground level ozone. This inadequacy of air quality models to sufficiently respond to the heterogeneous nature of the urban landscape can impact how well these models predict ozone pollutant levels over metropolitan areas and ultimately, whether cities exceed EPA ozone air quality standards. We are exploring the utility of high-resolution remote sensing data and urban growth projections as improved inputs to meteorological and air quality models focusing on the Atlanta, Georgia metropolitan area as a case study. The National Land Cover Dataset at 30m resolution is being used as the land use/land cover input and aggregated to the 4km scale for the MM5 mesoscale meteorological model and the Community Multiscale Air Quality (CMAQ) modeling schemes. Use of these data have been found to better characterize low density/suburban development as compared with USGS 1 km land use/land cover data that have traditionally been used in modeling. Air quality prediction for future scenarios to 2030 is being facilitated by land use projections using a spatial growth model. Land use projections were developed using the 2030 Regional Transportation Plan developed by the Atlanta Regional Commission. This allows the State Environmental Protection agency to evaluate how these transportation plans will affect future air quality.

Quattrochi, Dale A.↗
NASA NTRS2006

Remote Sensing and Spatial Growth Modeling Coupled with Air Quality Modeling to Assess the Impact of Atlanta, Georgia on the Local and Regional Environment

The growth of cities, both in population and areal extent, appears as an inexorable process. Urbanization continues at a rapid rate, and it is estimated that by the year 2025, 80 percent of the world s population will live in cities. Directly aligned with the expansion of cities is urban sprawl. Urban expansion has profound impacts on a host of biophysical, environmental, and atmospheric processes. A reduction in air quality over cities is a major result of these impacts. Strategies that can be directly or indirectly implemented to help remediate air quality problems in cities and that can be accepted by political decision makers and the general public are now being explored to help bring down air pollutants and improve air quality. The urban landscape is inherently complex and this complexity is not adequately captured in air quality models, particularly the Community Multiscale Air Quality (CMAQ) model that is used to assess whether urban areas are in attainment of EPA air quality standards, primarily for ground level ozone. This inadequacy of the CMAQ model to sufficiently respond to the heterogeneous nature of the urban landscape can impact how well the model predicts ozone pollutant levels over metropolitan areas and ultimately, whether cities exceed EPA ozone air quality standards. We are exploring the utility of high-resolution remote sensing data and urban spatial growth modeling (SGM) projections as improved inputs to the meteorology component of the CMAQ model focusing on the Atlanta, Georgia metropolitan area as a case study. These growth projections include "business as usual" and "smart growth" scenarios out to 2030. The growth projections illustrate the effects of employing urban heat island mitigation strategies, such as increasing tree canopy and albedo across the Atlanta metro area, which in turn, are used to model how ozone and air temperature can potentially be moderated as impacts on elevating ground-level ozone, as opposed to not utilizing heat island mitigation strategies. The National Land Cover Dataset at 30m resolution is being used as the land use/land cover input and aggregated to the 4km scale for the MM5 mesoscale meteorological model and the (CMAQ) modeling schemes. Use of these data have been found to better characterize low density/suburban development as compared with USGS 1km land use/land cover data that have traditionally been used in modeling. Air quality prediction for future scenarios to 2030 is being facilitated by land use projections using a spatial growth model. Land use projections were developed using the 2030 Regional Transportation Plan developed by the Atlanta Regional Commission, the regional planning agency for the area. This allows the State Environmental Protection agency to evaluate how these transportation plans will affect future air quality. The coupled SGM and air quality modeling approach provides insight on what the impacts of Atlanta s growth will be on the local and regional environment and exists as a mechanism that can be used by policy makers to make rationale decisions on urban growth and sustainability for the metropolitan area in the future.

Quattrochi, Dale A.↗
NASA NTRS2014

Dual Fan Separator within the Universal Waste Management System

Since NASA's new spacecraft in development for both LEO and Deep Space capability have considerable crew volume reduction in comparison to the Space Shuttle, it is clear that NASA requires a smaller and less expensive commode. The UTAS Universal Waste Management System (UWMS) was designed to address these new constraints, resulting in an 80% volume reduction in the cabin while enhancing performance. Whereas all of the current space commodes use air flow to capture both urine and feces and separate air from the captured air/urine mixture, the UWMS commode and urine fans and the urine separator were combined into a single unit. This unit enables use of a single motor and motor controller, which provides considerable packaging and weight efficiency. In some of the intended platform applications for the UWMS, the urine is pumped to a water reclamation system. The ISS Urine Processor Assembly (UPA) system requires delivered urine to include less than 0.25% air inclusion. Air inclusion in centrifugal urine separators is greatly dependent on its rotational speed. To satisfy this requirement, a gear reducer was included, allowing the fans to rotate at a much higher speed than the separator. This new design, the Dual Fan Separator (DFS) has been designed, prototyped and tested. This paper will outline the studies and analysis performed to develop the design configuration for testing. The studies included a configuration trade study, dynamic stability analysis of the rotating bodies and a performance analysis of included labyrinth seals. NASA is considereing a program to fly the UWMS aboard the ISS as a flight experiment. The goal of the design activity is to elevate the Technical Readiness Level (TRL) of the Dual Fan Separator and determine if the concept is ready to be included in flight experiment deliverable.

Stapleton, Tom↗
NASA NTRS2021

Comparison of chemical lateral boundary conditions for air quality predictions over the contiguous United States during pollutant intrusion events

The National Air Quality Forecast Capability (NAQFC) operated in U.S.’s National Oceanic and Atmospheric Administration (NOAA) provides the operational forecast guidance for ozone and fine particulate matters with aerodynamic diameters less than 2.5μm (PM2.5) over the contiguous 48 U.S. states (CONUS) using the Community Multi-scale Air Quality (CMAQ) model. The existing NAQFC uses climatological chemical lateral boundary conditions ( CLBCs), which cannot capture pollutant intrusion events originating outside of the model domain. In this study, we developed a model framework to use dynamic CLBCs from the Goddard Earth Observing System Model, version 5 (GEOS) to drive NAQFC. A mapping of the GEOS chemical species to the CMAQ’s Carbon Bond 5 (CB05)-Aero6 species was developed. The utilization of the GEOS dynamic CLBCs in NAQFC showed the best overall performance in simulating the surface observations during the Saharan dust intrusion and Canadian wildfire events in summer 2015.The simulated PM2.5 was improved from 0.18 to 0.37 and the mean bias was reduced from -6.74 μg/m3 to -2.96 μg/m3 over CONUS. Although the effect of CLBCs on the PM2.5 correlation was mainly near the inflow boundary, its impact on the background concentrations reached further inside the domain. The CLBCs could affect background ozone concentrations through the inflows of ozone itself and its precursors, such as CO. It was further found that the aerosol optical thickness (AOT) from satellite retrievals correlated well with the column CO and elemental carbon from GEOS. The satellite-derived AOT CLBCs generally improved the model performance for the wildfire intrusion events during a summer 2018 case study, and demonstrated how satellite observations of atmospheric composition could be used as an alternative method to capture the air quality effects of intrusions when the global model CLBCs, such as GEOS CLBCs, are not available.

Community Multi-scale Air Quality (CMAQ) model↗
DOE OSTI2022

Thermodynamic Model and Initial Experimental Investigation of Air Dehumidification through Electrically Charged Vapor Capturing Electrostatic Droplets

The removal of water vapor from the air to reduce relative humidity is a well known indoor environmental comfort requirement. Common dehumidification approaches require a substantial amount of energy and usually involve the cooling of atmospheric humid air below its dew point or the use of absorbent/adsorbent materials to extract water vapor out of the air. More recently, researchers investigated the effect of electrostatic forces for enhancing water vapor condensation with the goal to reduce the energy consumption associated with dehumidification. However, the studies are limited, and there is a lack of correlations that can predict the dehumidification rate. In this thesis, a broad theoretical investigation to study the electrostatically enhanced condensation processes was carried out. These processes consist of the use of highly charged particles, preferably highly charged water droplets to attract polar water vapor molecules to their surfaces and promote condensation, a phenomenon known as dielectrophoresis. The electrical charge promotes the reduction of the vapor pressure on the droplets' surface with respect to the saturated pressure predicted by the Kelvin equation on curved surfaces and, consequently, the equilibrium between evaporation and condensation is shifted towards condensation. This investigation resulted in the development of a thermodynamics model, which was able to predict an effective size range of the charged droplets for optimal dehumidification, under ideal conditions. The range resulted in about 2 to 4 m in diameter, while the electrical charge was kept to the maximum limit predicted by the Rayleigh model. A sensitivity analysis on the variation of the size and the charge of the charged droplets was also performed. In terms of dehumidification rates, when six electrospray heads, i.e. the maximum number of heads tested in the experimental campaign, were considered, the model predicted very limited rates, way lower than the target of this research, i.e. a dehumidification rate in terms of relative humidity of 5 % with an air flow rate of 5 cfm. While ways to increase this rate existed, their implementation proved difficult for this initial investigation. According to the requirements predicted by the model, the use of electrosprays appeared the most suitable solution for the production of small but highly charged droplets. The electrospray features and operational modes were studied in detail and an electrospray assembly was designed to be tested in this initial experimental investigation. For this initial investigation, an experimental system was designed and built to validate the thermodynamics model and with the goal to achieve a dehumidification rate of 5 % in terms of relative humidity with an air flow rate of 5 cfm. The experimental system consisted of a wind tunnel test apparatus, dew point sensors, thermocouples for temperature measurements, pressure sensors and other devices. The experimental system was equipped with a computerized data acquisition and storage system. The system was suitable to evaluate the air water content differential before and after the test section where the electrospray heads were installed. The air water content differential was evaluated in terms of the ∆ω/ω_1 ratio, to eliminate the dependence on the dry bulb temperature along the test apparatus. This work presented initial experimental data for electrostatically enhanced dehumidification processes. Working parameters, such as air and water flow rates, high voltage potentials and polarity, deionized water types with different electrical conductivity, were varied to find the best combination for an improved dehumidification. With the set up used and the conditions considered, it was never possible to achieve a 5 % dehumidification rate with 5 cfm. In general, the dehumidification rate was always limited and lower than 1 % for all the air flow rates considered and mainly within the uncertainty of the dew point sensors. These results confirmed the already limited predictions of the thermodynamics model, for ideal conditions and the interesting and promising results obtained in some experimental investigations available in the open literature were not achievable in this thesis. The more probable reasons were the higher air flow rates considered and the complete absence of the use of cooling power, which was mainly implemented to facilitate the vapor condensation.

Morcelli, Stefano↗