Solution and Active Site Speciation Drive Selectivity for Electrocatalytic Reactive Carbon Capture in Diethanolamine over Ni-N-C Catalysts (Lightning Talk)
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Chemistry↗
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Solution and Active Site Speciation Drive Selectivity for Electrocatalytic Reactive Carbon Capture in Diethanolamine over Ni-N-C Catalysts
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Chemistry↗
A COMPACT model reduction methodology for articulated, multi-flexible bodies structures
To simulate the dynamical motion of articulated, multiflexible body structures, one can use multibody simulation packages such as DISCOS. To this end, one need appropriate reduced-order models for all the flexible components involved. The component modes projection and assembly model reduction methodology is one way to construct these reduced-order component models. However, the generated reduced-order system models typically contain high frequency extraneous modes. The presence of high frequency extraneous modes in a reduced-order system model forces us to use a small stepsize in the numerical integration of that model, resulting in an increase in the elapsed time of the integration process. To eliminate these high-frequency modes, we first identify and discard the component modes that 'contributed' to the generations of these modes. A sensitivity analysis is then used to determine how the remaining component modes should be perturbed in order to still closely capture the selected system modes. The effectiveness of the proposed methodology has been successfully verified using a finite-element model of the Galileo spacecraft.
Lee, Allan Y.↗
The HIAD Orbital Flight Demonstration Instrumentation Suite
NASA's Hypersonic Inflatable Aerodynamic Decelerator (HIAD) technology has been selected for a Technology Demonstration Mission under the Science and Technology Mission Directorate. HIADs are an enabling technology that can facilitate atmospheric entry of heavy payloads to planets such as Earth and Mars using a deployable aeroshell. The deployable nature of the HIAD technology allows it to overcome the size constraints imposed on current rigid aeroshell entry systems. This permits use of larger aeroshells resulting in increased entry system performance (e.g. higher payload mass and/or volume, higher landing altitude at Mars). The Low Earth Orbit Flight Test of an Inflatable Decelerator (LOFTID) is currently scheduled for mid-2021. LOFTID will be launched out of Vandenberg Air Force Base as a secondary payload on an expendable launch vehicle. The flight test will employ a 6m diameter, 70 degree sphere-cone aeroshell and will provide invaluable high-energy orbital re-entry flight data. This data will be essential in supporting the HIAD team to mature the technology to diameters of 10m and greater. Aeroshells of this scale will address near-term commercial applications and potential future NASA missions. LOFTID will incorporate an extensive instrumentation suite totaling over 150 science measurements. This will include thermocouples, heat flux sensors, IR cameras, and a radiometer to characterize the aeroheating environment and aeroshell thermal response. An inertial measurement unit (IMU), GPS, and flush air data system will be included in order to reconstruct the flown trajectory and aerodynamic characteristics. Loadcells will be used to measure the HIAD structural loading, and HD cameras will be mounted on the aft segment looking at the aeroshell to monitor structural response. In addition to the primary instrumentation suite, a new fiber optic sensing system will be used to measure nose temperatures as a technology demonstration. The LOFTID instrumentation suites leverages Agency-wide expertise, with hardware development occurring at Ames Research Center, Langley Research Center, Marshall Space Flight Center and Armstrong Flight Research Center. This presentation will discuss the measurement objectives for the LOFTID mission, and the extensive instrumentation suite that has been selected to capture the HIAD's performance during the high-energy orbital re-entry flight test.
Swanson, G. T.↗
The HIAD Orbital Flight Demonstration Instrumentation Suite
NASA's Hypersonic Inflatable Aerodynamic Decelerator (HIAD) technology has been selected for a Technology Demonstration Mission under the Science and Technology Mission Directorate. HIADs are an enabling technology that can facilitate atmospheric entry of heavy payloads to planets such as Earth and Mars using a deployable aeroshell. The deployable nature of the HIAD technology allows it to overcome the size constraints imposed on current rigid aeroshell entry systems. This permits use of larger aeroshells resulting in increased entry system performance (e.g. higher payload mass and/or volume, higher landing altitude at Mars). The Low Earth Orbit Flight Test of an Inflatable Decelerator (LOFTID) is currently scheduled for mid-2021. LOFTID will be launched out of Vandenberg Air Force Base as a secondary payload on an expendable launch vehicle. The flight test will employ a 6m diameter, 70-deg sphere-cone aeroshell and will provide invaluable high-energy orbital re-entry flight data. This data will be essential in supporting the HIAD team to mature the technology to diameters of 10m and greater. Aeroshells of this scale will address near-term commercial applications and potential future NASA missions.LOFTID will incorporate an extensive instrumentation suite totaling over 150 science measurements. This will include thermocouples, heat flux sensors, IR cameras, and a radiometer to characterize the aeroheating environment and aeroshell thermal response. An inertial measurement unit (IMU), GPS, and flush air data system will be included in order to reconstruct the flown trajectory and aerodynamic characteristics. Loadcells will be used to measure the HIAD structural loading, and HD cameras will be mounted on the aft segment looking at the aeroshell to monitor structural response. In addition to the primary instrumentation suite, a new fiber optic sensing system will be used to measure nose temperatures as a technology demonstration. The LOFTID instrumentation suites leverages Agency-wide expertise, with hardware development occurring at Ames Research Center, Langley Research Center, Marshall Space Flight Center and Armstrong Flight Research Center.This presentation will discuss the measurement objectives for the LOFTID mission, and the extensive instrumentation suite that has been selected to capture the HIAD's performance during the high-energy orbital re-entry flight test.
Swanson, Greg↗
Contingent Attentional Capture
Four experiments address the degree of top-down selectivity in attention capture by feature singletons through manipulations of the spatial relationship and featural similarity of target and distractor singletons in a modified spatial cuing paradigm. Contrary to previous studies, all four experiments show that when searching for a singleton target, an irrelevant featural singleton captures attention only when defined by the same feature value as the target. Experiments 2, 3, and 4 provide a potential explanation for this empirical discrepancy by showing that irrelevant singletons can produce distraction effects that are independent of shifts of spatial attention. The results further support the notion that attentional capture is contingent on top-down attention control settings but indicates that such settings can be instantiated at the level of feature values.
Remington, Roger↗
Bicarbonate-Carbonate Selectivity through Nanofiltration for Direct Air Capture of Carbon Dioxide
Direct air capture (DAC) of carbon dioxide is one approach among many proposed that is capable of offsetting hard-to-avoid emissions. In previous work, we developed the alkalinity concentration swing (ACS) method, which is driven through concentrating an alkaline solution that has been loaded with atmospheric CO 2 by desalination technologies, such as reverse osmosis or capacitive deionization. Though the ACS is promising in terms of energy usage and implementation, its absorption rate and water requirements are infeasible for a large-scale DAC process. Here, we propose an improvement on the ACS, the bicarbonate-enriched alkalinity concentration swing (BE-ACS), which selects bicarbonate ions from a stream of aqueous alkaline solution that has absorbed atmospheric CO 2 . The bicarbonate-rich stream is then concentrated, which greatly increases its CO 2 partial pressure, and then CO 2 is extracted from solution. We experimentally investigate the use of pressure-driven nanofiltration (NF) membrane-based separation to select bicarbonate ions over carbonate ions. We screen commercial membranes and select one high-performance membrane for detailed studies, quantifying its bicarbonate-carbonate selectivity factor and bicarbonate-passage factor. Feed pH, the combined concentration of aqueous CO 2 , bicarbonate, and carbonate species (or dissolved inorganic carbon), alkalinity, and permeation flux are systematically varied to study NF separation properties. We find that the selectivity factor, which exceeds 30 times in certain regimes, increases with higher feed pH and higher alkalinity. Lastly, the performance metrics of the selected NF membrane are input into a theoretical BE-ACS cycle analysis, and the required energy input and cycle capacity output are evaluated. Ideal cycle energy is found to be as low as around 250 kJ/mol, with opportunities identified for further decreases through process engineering and forward osmosis energy recovery.
animal feed↗
Two-stage membrane-based process utilizing highly CO 2 -selective membranes for cost and energy efficient carbon capture from coal flue gas: A process simulation study
Membrane technology for CO 2 capture has become an attractive strategy due to its cost and energy efficiency and low materials costs. In the past decade, membrane-based process designs for post-combustion power plant CO 2 capture have been developed, utilizing existing highly CO 2 -permeable membranes with relatively low CO 2 /N 2 selectivity (<50), and have obtained reasonably economic carbon capture. However, few membrane-based process designs were proposed for moderate to highly CO 2 -selective membranes (CO 2 /N 2 selectivity of 50–300, and >300, respectively), which have vastly emerged in recent years, such as various facilitated transport membranes (FTMs). Herein, we proposed a two-stage membrane-base process design targeting economic carbon capture from coal-fired flue gas. This process design features the utilization of highly CO 2 -selective membranes for one-stage CO 2 enrichment to 95% dry-base purity in the first stage and recycle of the remaining CO 2 by a highly CO 2 -permeable membrane in the second stage, in order to achieve economic CO 2 capture with 90% capture rate and >95% CO 2 product purity. Through an integration-iteration membrane model and the Aspen Plus process simulation, a sensitivity study of operating pressures (feed and permeate pressures) and membrane properties (CO 2 permeance and CO 2 /N 2 selectivity) was conducted. Critical CO 2 /N 2 selectivity of 300–400 was found for the highly CO 2 -selctive membranes to meet the demand for cost and energy efficient results. The lowest possible membrane area of 4.8 × 10 5 m 2 and fractional energy of 19.3% were obtained, which is comparable to or even more attractive than reported membrane-based process designs. Here, this work provides a new membrane process design option for highly CO 2 -selective membranes and gives insights on the influence of membrane performance and operation condition.
42 ENGINEERING↗
Probing Electrolyte Influence on CO 2 Reduction in Aprotic Solvents
Selective CO 2 capture and electrochemical conversion are important tools in the fight against climate change. Industrially, CO 2 is captured using a variety of aprotic solvents due to their high CO 2 solubility. However, most research efforts on electrochemical CO 2 conversion use aqueous media and are plagued by competing hydrogen evolution reaction (HER) from water breakdown. Fortunately, aprotic solvents can circumvent HER, making it important to develop strategies that enable integrated CO 2 capture and conversion. However, the influence of ion solvation and solvent selection within nonaqueous electrolytes for efficient and selective CO 2 reduction is unclear. In this work, we show that the bulk solvation behavior within the nonaqueous electrolyte can control the CO2 reduction reaction and product distribution occurring at the catalyst-electrolyte interface. We study different tetrabutylammonium (TBA) salts in two electrolyte systems with glyme ethers (e.g., 1,2 dimethoxyethane or DME) and dimethyl sulfoxide (DMSO) as a low and high dielectric constant medium, respectively. Using spectroscopic tools, we quantify the fraction of ion pairs that forms within the electrolyte. Also, we show how ion pair formation is prevalent in DME and is dependent on the anion type. More importantly, we show that as ion pair formation decreases within the electrolyte, CO 2 current densities increase, and a higher CO Faradaic efficiency is observed at low overpotentials. Meanwhile, in an electrolyte medium where the ion pair fraction does not change with the anion type (such as in DMSO), a smaller influence of solvation is observed on CO 2 current densities and product distribution. By directly coupling bulk solvation to interfacial reactions and product distribution, we showcase the importance and utility of controlling the reaction microenvironment in tuning the electrocatalytic reaction pathways. Insights gained from this work will enable novel electrolyte designs for efficient and selective CO 2 conversion to desired fuels and chemicals.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Highly selective hollow fiber membranes for carbon capture via in-situ layer-by-layer surface functionalization
Not Available
Mishra, Naveen K. (ORCID:0000000235428408)↗
A New High Flux with High Selectivity Membrane for Low Cost CO2 Capture
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01 COAL, LIGNITE, AND PEAT↗
Challenges in Product Selectivity for Electrocatalytic Reduction of Amine-Captured CO 2 : Implications for Reactive Carbon Capture
CO 2 is a potential feedstock for carbon-based fuels or materials, but is only available in dilute streams. Integrated processes for CO 2 capture and conversion directly valorize the CO 2 captured by sorbent materials, skipping the energetically expensive sorbent regeneration step. Amines are the most heavily studied liquid-phase sorbent materials for CO 2 capture from dilute streams. Amines react with CO 2 in a 2:1 ratio to form the corresponding ammonium carbamate. Ammonium carbamate [NH 4 ][H 2 NCO 2 ] was tested as the substrate using the highly selective and robust CO 2 -to-formate reduction electrocatalyst [( tBu POCOP)Ir(H)(NCCH 3 ) 2 ], where ( tBu POCOP) is the tridentate pincer ligand 2,6-bis(di tert -butyl-phosphonito). When ammonium carbamate was used as the substrate instead of CO 2 , only hydrogen was produced. An equivalent electrolysis with ammonium hexafluorophosphate with CO 2 also resulted in primarily hydrogen. Methyl carbamate and urea were also tested as substrates as proxies for carbamate that do not contain an equivalent of ammonium, and there was also negligible reduction to carbon-based products. These results indicate that the loss of selectivity observed for aminecaptured CO 2 , or ammonium carbamate, is likely due to the generation of the acidic ammonium equivalent as well as the greater challenge of reducing carbamate compared to CO 2 . This study illustrates that catalysts with high selectivity for concentrated CO 2 can favor hydrogen evolution and loss of carbon-based products when amine-captured CO 2 is used instead.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Bituminous Coal and Natural Gas to Electricity: >90% Capture Cases Technical Note
This technical note provides cost and performance estimates for post combustion carbon capture (PCCC) systems designed for greater than 90 percent capture on conventional PC- and NG-fueled power plants. The cost and performance estimates provided here were developed using the National Energy Technology Laboratory’s (NETL’s) well-documented methodology for conducting technoeconomic analysis of fossil energy conversion systems and leveraging published performance and cost projections for higher capture rate systems. Included in this technical note is a brief description of the method used to adjust select 90 percent capture cases from NETL’s Cost and Performance Baselines for Fossil Energy Systems Volume 1: Bituminous Coal and Natural Gas to Electricity, hereafter referred to as the Baseline Study. This technical note is intended to serve as an interim update to NETL’s Baseline Study cases by providing cost and performance estimates for high capture PCCC technology that can be deployed in the near-term at fossil-fueled electricity generating units.
20 FOSSIL-FUELED POWER PLANTS↗
Experimental Investigation of the Distribution of Shock Effects in Regolith Impact Ejecta Using an Ejecta Recovery Chamber
Because the mass-flux of solar system meteoroids is concentrated in the approx. 200 microns size range, small-scale impacts play a key role in driving the space weathering of regoliths on airless bodies. Quantifying this role requires improved data linking the mass, density and velocity of the incoming impactors to the nature of the shock effects produced, with particular emphasis on effects, such as production of impact melt and vapor, that drive the optical changes seen in space weathered regoliths. Of particular importance with regard to space weathering is understanding not only the composition of the shock melt created in small-scale impacts, but also how it is partitioned volumetrically between the local impact site and more widely distributed ejecta. To improve the ability of hypervelocity impact experiments to obtain this type of information, we have developed an enclosed sample target chamber with multiple-geometry interior capture cells for in-situ retention of ejecta from granular targets. A key design objective was to select and test capture cell materials that could meet three requirements: 1) Capture ejecta fragments traveling at various trajectories and velocities away from the impact point, while inducing minimal additional damage relative to the primary shock effects; 2) facilitate follow-up characterization of the ejecta either on or in the cell material by analytical SEM, or ex-situ by microprobe, TEM and other methods; and 3) enable the trajectories of the captured and characterized ejecta to be reconstructed relative to the target.
Christoffersen, R.↗
Lithium cuprate, a multifunctional material for NO selective catalytic reduction by CO with subsequent carbon oxide capture at moderate temperatures
Li 2 CuO 2 was evaluated as a possible catalyst for the NO selective catalytic reduction (NO SCR) by CO. The initial idea was supported by ab initio thermodynamic analysis. This analysis showed that NO SCR was favored by using Li 2 CuO 2 as a catalyst, based on the calculated heat of reaction and Gibbs free energy. The NO SCR reaction was evaluated under dynamic, isothermal and cyclic conditions using different NO : CO ratios (2 : 1, 1 : 1 and 1 : 2). The dynamic and isothermal experiments showed that Li 2 CuO 2 does reduce NO in the presence of CO to reach higher conversions (>90%) between 400 and 450 °C. However, it must be mentioned that the catalytic process was reduced once some of the produced CO 2 was captured on the ceramic. At that point, Li 2 CuO 2 acts as a bifunctional material, catalyzing the NO SCR reaction and capturing some of the produced CO 2 . Moreover, cyclic experiments evidenced high NO reduction. Finally, a different set of experiments showed that this catalytic reduction performed differently if NO and CO were previously fed. Finally, when lithium cuprate is previously carbonated (initial CO feed), the catalytic reaction does not complete. In contrast, when there was a previous nitrate formation (initial NO feed), the reaction reached 100% efficiency.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Exploitation of Pore Structure for Increased CO 2 Selectivity in Type 3 Porous Liquids
CO 2 capture requires materials with high adsorption selectivity and an industrial ease of implementation. To address these needs, a new class of porous materials was recently developed that combines the fluidity of solvents with the porosity of solids. Type 3 porous liquids (PLs) composed of solvents and metal–organic frameworks (MOFs) offer a promising alternative to current liquid carbon capture methods due to the inherent tunability of the nanoporous MOFs. However, the effects of MOF structural features and solvent properties on CO 2 –MOF interactions within PLs are not well understood. Herein experimental and computational data of CO 2 gas adsorption isotherms were used to elucidate both solvent and pore structure influences on ZIF-based PLs. The roles of the pore structure including solvent size exclusion, structural environment, and MOF porosity on PL CO 2 uptake were examined. A comparison of the pore structure and pore aperture was performed using ZIF-8, ZIF-L, and amorphous-ZIF-8. Adsorption experiments here have verified our previously proposed solvent size design principle for ZIF-based PLs (1.8× ZIF pore aperture). Furthermore, the CO 2 adsorption isotherms of the ZIF-based PLs indicated that judicious selection of the pore environment allows for an increase in CO 2 selectivity greater than expected from the individual PL components or their combination. This nonlinear increase in the CO 2 selectivity is an emergent behavior resulting from the complex mixture of components specific to the ZIF-L + 2'-hydroxyacetophenone-based PL.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Design of CO 2 Selective Type 3 Porous Liquids Through Porous Host Morphology
Direct air capture (DAC) of CO 2 is a negative emission technology under development to limit the impacts of climate change. The dilute concentration of CO 2 in the atmosphere (~400 ppm) requires new materials for carbon capture with increased CO 2 selectivity that is not met with current carbon capture materials. Porous liquids (PLs) are an emerging candidate for carbon capture and consists of a combination of solvents and porous hosts that creates a liquid with permanent porosity. The fundamental mechanisms of carbon capture in a PL are relatively unknown. To uncover these mechanisms, PLs were synthesized consisting of three different zeolitic-imidazolate framework (ZIF-8, ZIF-67, or ZIF-69) porous host in a water/glycol/2-methylimidazole solvent. The most stable composition was based on ZIF-8 and exhibited carbon capture following exposure to CO 2 . Density functional theory identified a three-step carbon capture mechanism based on (i) reaction of OH- with ethylene glycol in the solution followed by (ii) formation of 2-hydroxyethyl carbonate, which (iii) further react with OH- to form a carbonate species. This mechanism was validated with experimental nuclear magnetic resonance spectroscopy (NMR) to identify the dissolved carbonate phases and the decrease in the pH during CO 2 exposure. Deuterated samples of the ZIF-8 PLs were synthesized and analyzed via neutron diffraction at the Spallation Neutron Sources at Oak Ridge National Laboratory. Results identified differences in diffraction for PLs pre- and post-CO 2 exposure that will be combined with ab initio molecular dynamics data of the same PL composition to identify how the presence of a solvent-porous host interfaces results in carbon capture.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Capture and real-time display of selected Space Shuttle reentry data
Because the flight planning for the orbital flight test (OFT) flights of the NASA Space Shuttle required several months, there was very little time to analyze data from one flight before it was necessary to start final planning for the next flight. Real-time and selected immediate postflight data display of the reentry data minimized the postflight computer analysis time required so that the rigid time restraints imposed by the program could be met. This paper describes the methods used to decommutate and provide real-time and immediate postflight data display of selected Space Shuttle reentry data.
Chiles, H. R.↗