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At least 109 records · Page 6

Photoassisted carbon dioxide reduction and formation of twoand three-carbon compounds

The photoassisted reduction of aqueous carbon dioxide in the presence of naturally occurring minerals is investigated as a possible abiotic precursor of photosynthesis. Aqueous carbon dioxide saturated suspensions or surfaces of the minerals nontronite, bentonite, anatase, wolframite, molybdenite, minium, cinnabar and hematite were irradiated with high-pressure mercury lamps or sunlight. Chemical analyses reveal the production of formic acid, formaldehyde, methanol and methane, and the two and three-carbon compounds glyoxal (CHOCHO) and malonaldehyde (CH2(CHO)2). It is suggested that such photosynthetic reactions with visible light in the presence of semiconducting minerals may provide models for prebiological carbon and nitrogen fixation in both oxidized and reduced atmospheres.

Halmann, M.↗

Water content of carbon dioxide at hydrate forming conditions

There is an interest to ensure sub-saturated water content in lines containing carbon dioxide in applications such as enhanced oil recovery and carbon sequestration, to reduce risks of hydrate blockage and corrosion. The water content of carbon dioxide at various temperatures and pressures has been measured in the past, but there is no consistent set of measurements that could be used for carbon dioxide storage and transportation design work. The solubility of water in a carbon dioxide rich gas phase at hydrate forming conditions was measured in this work. Pressures ranged from 12.06 to 29.30 bar along two isotherms, 1 °C and -7 °C, all within the gaseous carbon dioxide and hydrate stability zone. For the first time in these types of measurements, the solid phase was also characterized and confirmed to be carbon dioxide hydrate via X-ray computed tomography, simultaneous with water content measurements of the gas phase. Once carbon dioxide hydrate conversion had reached a maximum value (65% estimated by X-ray computed tomography), the equilibrium water content was measured. Prior to reaching this maximum carbon dioxide hydrate conversion, the water content in carbon dioxide was observed to decrease as liquid water converted to carbon dioxide hydrate. Furthermore, this slow conversion to hydrate, metastability of the hydrate phase, or unexpected phases may be responsible for the large discrepancy between prior data sets for similar carbon dioxide water content measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Progress of Four Bed Carbon Dioxide Scrubber

The Four Bed Carbon Dioxide Scrubber flight demonstration is presently operating onboard the International Space Station. After being launched in August of 2021 and installed in October, the system has been removing metabolic CO2 from the cabin as a supplement and replacement for other CO2 systems, specifically the two Carbon Dioxide Removal Assemblies. This work describes the conclusion of the ground integration and testing campaign and the start of on orbit operations. Additionally, performance, reliability, and forward works will be summarized. Interactions of the software with off-nominal events will be discussed and how the system will be reconfigured to sustain operations.

4BCO2↗

KCMP Minnesota Tall Tower Carbon Dioxide Data 2007-2019

This data set contains carbon dioxide concentration values and supporting metadata information measured at a tall tower (KCMP radio station, 244 meters) site near St. Paul, Minnesota, USA. The data package includes a text file containing hourly continuous carbon dioxide concentration measurements from 2007 to 2019, including raw, de-spiked, and gap filled data. Carbon dioxide concentrations were measured at approximately 100 meters using tunable diode laser spectroscopy. The instrumentation was maintained at the base of the tall tower in a temperature-controlled building. This data was collected to track and improve the understanding of carbon dioxide levels over a twelve year period for the region.

54 ENVIRONMENTAL SCIENCES↗

Separation of Carbon Monoxide and Carbon Dioxide for Mars ISRU-Concepts

Solid oxide electrolyzers, such as electrolysis cells utilizing yttria-stabilized zirconia, can produce oxygen from Mars atmospheric carbon dioxide and reject carbon monoxide and unreacted carbon dioxide in a separate stream. The oxygen-production process has been shown to be far more efficient if the high-pressure, unreacted carbon dioxide can be separated and recycled back into the feed stream. Additionally, the mass of the adsorption compressor can be reduced. Also, the carbon monoxide by-product is a valuable fuel for space exploration and habitation, with applications from fuel cells to production of hydrocarbons and plastics. In our research, we will design, construct, and test an innovative, robust, low mass, low power separation device that can recover carbon dioxide and carbon monoxide for Mars ISRU. Such fundamental process technology, involving gas-solid phase separation in a reduced gravitational environment, will help to enable Human Exploration and Development of Space. The separation device will be scaled to operate with a CO2 sorption compressor and a zirconia electrolysis device built at the NASA Ames Research Center and the University of Arizona, respectively. In our research, we will design, construct, and test an innovative, robust, low mass, low power separation device that can recover carbon dioxide and carbon monoxide for Mars ISRU, Such fundamental process technology, involving gas-solid phase separation in a reduced gravitational environment, will help to enable Human Exploration and Development of Space. The separation device will be scaled to operate with a CO2 sorption compressor and a zirconia electrolysis device built at the NASA Ames Research Center and the University of Arizona, The separation device will be scaled to operate with a CO2 sorption compressor and a zirconia electrolysis device built at the NASA Ames Research Center and the University of Arizona, Research needs for the design shown are as follows: (1) The best adsorbent for the process must be determined. (2) Adsorption isotherms must be measured, both for pure components and mixtures. (3) Mathematical modeling must be performed to provide a solid framework for design. (4) The separation system must be constructed and tested. (5) System integration must be studied.

LeVan, M. Douglas↗

A Comprehensive Greenhouse Gas Assessment of Biomass-Based Carbon Dioxide Removal and Storage

Biomass with Carbon Removal and Sequestration (BiCRS) is a suite of technological pathways that provide a relatively affordable and high-potential way to remove carbon dioxide from the atmosphere and simultaneously re-purpose residual biomass. BiCRS technologies are individually optimized to different biomass feedstocks, temperatures and oxygen, with the goal of capturing a high percentage of biomass-derived carbon dioxide and storing it in permanent below-ground storage (i.e. geologic storage). The current standard for BiCRS life cycle assessments does not account for carbon dioxide, methane and nitrous oxide (CO 2 , CH 4 , and N 2 O) fluxes from surface soil amendment of BiCRS byproducts (e.g. char, ash) and their alternate fates. This is partly due to a paucity of empirical data due to the novelty of BiCRS conversion technologies, the range in feedstocks, and the heterogeneity of soils to which they might be amended. To fill this gap in in the life-cycle assessment (LCA) and provide a realistic range of parameters for a soil amendment component of the BiCRS LCA, we conducted an incubation experiment to measure soil carbon changes, microbial respiration, methane fluxes, and nitrous oxide fluxes from two different soils amended with char- and ash- byproducts from biomass after gasification to hydrogen, fast pyrolysis to bio-oil, and torrefaction.

54 ENVIRONMENTAL SCIENCES↗

Unique nanotechnology converts carbon dioxide to valuable products

Carbon capture and management are increasing challenges associated with global warming. Current commercial-scale carbon dioxide (CO 2 ) capture technologies are associated with a heavy economic penalty – they require at least one-third of the plant’s steam and power to operate. The objective of this project was to develop and test an innovative nanotechnology that can utilize CO 2 , from coal-based power systems or other industrial sources, as the primary feedstock to produce commercially valuable products to potentially offset the cost of CO 2 capture. The scope of this project includes conversion of CO 2 to nanomaterials using two unique amino acids in synthetic flue gases and the completion of a process design and techno-economic and lifecycle analyses to demonstrate the economic feasibility and environmental impact of the developed technology. The International Energy Agency predicts that fossil fuels will continue to play a significant role in meeting global energy demand. The goal of the research is to lead to an affordable and transformational CO 2 capture and reuse technology that will reduce the release of CO 2 thereby reducing global climate variability and its enormous impact on our daily lives.

01 COAL, LIGNITE, AND PEAT↗

Assessing the Effect of Explicit Polarizability on Models of Carbon Dioxide Solvation in Ionic Liquids

Ionic liquids are an important possible carbon capture material because of their anomalously high sorption selectivity for carbon dioxide over other gases common in air. Many research groups have investigated the molecular origins of this property and provided important insights, including using 1D and 2D-IR spectroscopy. Molecular dynamics simulations have been indispensable to the interpretation of these experiments. In prior molecular dynamics simulation work, charge-scaled force fields have typically been used to provide a mean-field treatment of effects vital to ionic liquid systems such as charge transfer and polarization. Here, we compare models of carbon dioxide solvated in ionic liquids with explicit polarization to models of the same with implicit polarizability through charge-scaling. We calculate structural, dynamical, and spectroscopic properties, and make comparisons to the same items measured in experiment. In this study, we focus on two ionic liquids: 1-butyl-3- methylimidazolium (BMIM + ) paired with bis(trifluoromethane sulfonyl imide) (Tf 2 N − ) and 1-butyl-3-methylimidazolium (BMIM+) paired with hexafluorophosphate (PF 6 − ). We find that many structural, dynamical, and spectroscopic properties are changed when polarization is modeled explicitly. We also find that explicit polarizability softens local ion cages around the carbon dioxide and that the long-time diffusion of the carbon dioxide is gated by the reorganization of the ionic liquid molecules. Comparisons to experiment show modest improvement of many observables compared with experiment for the explicitly polarizable model over the charge-scaled model. Overall, our results show that charge-scaled force fields are likely sufficient to compute spectroscopic properties of carbon dioxide in ionic liquids and suggest some interpretive rules for understanding their structural and dynamical properties. Those using charge-scaled force fields should generally assume that the ion cages around solutes such as carbon dioxide are too stiff and cation-rich in their models and adjust their interpretations and predictions accordingly.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrochemical Conversion of Carbon Dioxide to Alcohols

The vast quantities of fossil fuels used by our society have led to unprecedented atmospheric carbon dioxide levels with widespread climate impacts. Electrochemical conversion of carbon dioxide to valuable fuels and chemicals is a promising technology to utilize carbon dioxide emitted from coal-fired power plants. In this project, the team developed an integrated electrolyzer system that takes the flue gas from the power plant and produce C2/C3 alcohols (i.e., ethanol and n-propanol) through a two-stage electrolysis process. The pretreated carbon dioxide from the flue gas is converted into carbon monoxide by the first stage carbon dioxide electrolysis, followed by the second stage where the produced carbon monoxide is further converted into liquid C2/C3 alcohols with a high selectivity and energy efficiency. Impact and anticipated fate of flue gas contaminants, such as sulfur dioxide and nitrogen oxides, on the proposed technology was also evaluated. Furthermore, a full analysis of economics and life-cycle of the carbon dioxide electrolysis technology for carbon dioxide emissions mitigation from coal-fired power plants was conducted to evaluate the economic feasibility and carbon dioxide mitigation potential of the proposed technology.

20 FOSSIL-FUELED POWER PLANTS↗

Development of a prototype regeneration carbon dioxide absorber

A prototype regenerable carbon dioxide absorber was developed to maintain the environmental quality of the portable life support system. The absorber works on the alkali metal carbonate-bicarbonate solid-gas reaction to remove carbon dioxide from the atmosphere. The prototype sorber module was designed, fabricated, and tested at simulated extravehicular activity conditions to arrive at optimum design. The unit maintains sorber outlet concentration below 5 mm Hg. An optimization study was made with respect to heat transfer, temperature control, sorbent utilization, sorber life and regenerability, and final size of the module. Important parameters influencing the capacity of the final absorber unit were identified and recommendations for improvement were made.

Patel, P. S.↗

Evaluation of 2-μm Pulsed Integrated Path Differential Absorption Lidar for Carbon Dioxide Measurement—Technology Developments, Measurements, and Path to Space

The societal benefits of understanding climate change through the identification of global carbon dioxide sources and sinks led to the recommendation for NASA's Active Sensing of Carbon Dioxide Emissions over Nights, Days, and Seasons space-based mission for global carbon dioxide measurements. For more than 15 years, the NASA Langley Research Center has developed several carbon dioxide active remote sensors using the differential absorption lidar technique operating at 2-μm wavelength. Recently, an airborne double-pulsed integrated path differential absorption lidar was developed, tested, and validated for atmospheric carbon dioxide measurement. Results indicated 1.02% column carbon dioxide measurement uncertainty and 0.28% bias over the ocean. Currently, this technology is progressing toward triple-pulse operation targeting both atmospheric carbon dioxide and water vapor-the dominant interfering molecule on carbon dioxide remote sensing. Measurements from the double-pulse lidar and the advancement of the triple-pulse lidar development are presented. In addition, measurement simulations with a space-based IPDA lidar, incorporating new technologies, are also presented to assess feasibility of carbon dioxide measurements from space.

Singh, Upendra N.↗

Carbon Dioxide Absorption Heat Pump

A carbon dioxide absorption heat pump cycle is disclosed using a high pressure stage and a super-critical cooling stage to provide a non-toxic system. Using carbon dioxide gas as the working fluid in the system, the present invention desorbs the CO2 from an absorbent and cools the gas in the super-critical state to deliver heat thereby. The cooled CO2 gas is then expanded thereby providing cooling and is returned to an absorber for further cycling. Strategic use of heat exchangers can increase the efficiency and performance of the system.

Jones, Jack A.↗

Performance Characterization and Simulation of Amine-Based Vacuum Swing Sorption Units for Spacesuit Carbon Dioxide and Humidity Control

Controlling carbon dioxide (CO2) and water (H2O) vapor concentrations in a space suit is critical to ensuring an astronauts safety, comfort, and capability to perform extra-vehicular activity (EVA) tasks. Historically, this has been accomplished using lithium hydroxide (LiOH) and metal oxide (MetOx) canisters. Lithium hydroxide is a consumable material that requires priming with water before it becomes effective at removing carbon dioxide. MetOx is regenerable through a power-intensive thermal cycle but is significantly heavier on a volume basis than LiOH. As an alternative, amine-based vacuum swing beds are under aggressive development for EVA applications. The vacuum swing units control atmospheric concentrations of both CO2 and H2O through fully-regenerative process. The current concept, referred to as the rapid cycle amine (RCA), has resulted in numerous laboratory prototypes. Performance of these prototypes have been assessed experimentally and documented in previous reports. To support developmental e orts, a first principles model has also been established for the vacuum swing sorption technology. For the first time in several decades, a major re-design of Portable Life Support System (PLSS) for the extra-vehicular mobility unit (EMU) is underway. NASA at Johnson Space Center built and tested an integrated PLSS test bed of all subsystems under a variety of simulated EVA conditions of which the RCA prototype played a significant role. The efforts documented herein summarize RCA test performance and simulation results for single and variable metabolic rate experiments in an integrated context. In addition, a variety of off-nominal tests were performed to assess the capability of the RCA to function under challenging circumstances. Tests included high water production experiments, degraded vacuum regeneration, and deliberate valve/power failure and recovery.

Swickrath, Michael J.↗