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At least 1,657 records · Page 92
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Transport and Co-Transport of Carboxylate Ions and Ethanol in Anion Exchange Membranes

Understanding multi-component transport behavior through hydrated dense membranes is of interest for numerous applications. For the particular case of photoelectrochemical CO 2 reduction cells, it is important to understand the multi-component transport behavior of CO 2 electrochemical reduction products including mobile formate, acetate and ethanol in the ion exchange membranes as one role of the membrane in these devices is to minimize the permeation of these products. Anion exchange membranes (AEM) have been employed in these and other electrochemical devices as they act to facilitate the transport of common electrolytes (i.e., bicarbonates). However, as they act to facilitate the transport of carboxylates as well, thereby reducing the overall performance, the design of new AEMs is necessary to improve device performance through the selective transport of the desired ion(s) or electrolyte(s). Here, we investigate the transport behavior of formate and acetate and their co-transport with ethanol in two types of AEMs: (1) a crosslinked AEM prepared by free-radical copolymerization of a monomer with a quaternary ammonium (QA) group and a crosslinker, and (2) Selemion® AMVN. We observe a decrease in diffusivities to carboxylates in co-diffusion. We attribute this behavior to charge screening by the co-diffusing alcohol, which reduces the electrostatic attraction between QAs and carboxylates.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Fischer-Tropsch Synthesis: The Characterization and Testing of Pt-Co/SiO 2 Catalysts Prepared with Alternative Cobalt Precursors

Different low-cost cobalt precursors (acetate, chloride) and thermal treatments (air calcination/H 2 reduction versus direct H 2 -activation) were investigated to alter the interaction between cobalt and silica. H 2 -activated catalysts prepared from cobalt chloride had large Co 0 particles (XRD, chemisorption) formed by weak interactions between cobalt chloride and silica (temperature programmed reduction (TPR), TPR with mass spectrometry (TPR-MS), TPR with extended X-ray absorption fine structure (EXAFS) and X-ray absorption near edge spectroscopy (XANES) techniques) and retained Cl-blocked active sites, resulting in poor activity. In contrast, unpromoted Co/SiO 2 catalysts derived from cobalt acetate had strong interactions between Co species and silica (TPR/TPR-MS, TPR-EXAFS/XANES); adding Pt increased the extent of the Co reduction. For these Pt-promoted catalysts, the reduction of uncalcined catalysts was faster, resulting in larger Co 0 clusters (19.5 nm) in comparison with the air-calcined/H 2 -activated catalyst (7.8 nm). Both catalysts had CO conversions 25% higher than that of the Pt-promoted catalyst prepared in the traditional manner (air calcination/H 2 reduction using cobalt nitrate) and three times higher than that of the traditional unpromoted Co/silica catalyst. The retention of residual cobalt carbide (observed in XANES) from cobalt acetate decomposition impacted performance, resulting in a higher C 1 –C 4 selectivity (32.2% for air-calcined and 38.7% for uncalcined) than that of traditional catalysts (17.5–18.6%). The residual carbide also lowered the α-value and olefin/paraffin ratio. Future work will focus on improving selectivity through oxidation–reduction cycles.

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

Evaluating Class 6 Delivery Truck Fuel Economy and Emissions Using Vehicle System Simulations for Conventional and Hybrid Powertrains and Co-Optima Fuel Blends

The US Department of Energy’s Co-Optimization of Engine and Fuels Initiative (Co-Optima) investigated how unique properties of bio-blendstocks considered within Co-Optima help address emissions challenges with mixing controlled compression ignition (i.e., conventional diesel combustion) and enable advanced compression ignition modes suitable for implementation in a diesel engine. Additionally, the potential synergies of these Co-Optima technologies in hybrid vehicle applications in the medium- and heavy-duty sector was also investigated. In this work, vehicles system were simulated using the Autonomie software tool for quantifying the benefits of Co-Optima engine technologies for medium-duty trucks. A Class 6 delivery truck with a 6.7 L diesel engine was used for simulations over representative real-world and certification drive cycles with four different powertrains to investigate fuel economy, criteria emissions, and performance. Comparisons were made between ultralow-sulfur diesel and a blend of 25% hexyl hexanoate with diesel. Model validation data were informed by 2019 model year Cummins ISB 6.7 L diesel engine maps and transient validation data in a pre-production hybrid configuration and a direct dyno coupled configuration with diesel fuel and a blend of 25% hexyl hexanoate with diesel.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2020

Leveraging the signature of heterotrophic respiration on atmospheric CO 2 for model benchmarking

Spatial and temporal variations in atmospheric carbon dioxide (CO 2 ) reflect large-scale net carbon exchange between the atmosphere and terrestrial ecosystems. Soil heterotrophic respiration (HR) is one of the component fluxes that drive this net exchange, but, given observational limitations, it is difficult to quantify this flux or to evaluate global-scale model simulations thereof. Here, we show that atmospheric CO 2 can provide a useful constraint on large-scale patterns of soil heterotrophic respiration. We analyze three soil model configurations (CASA-CNP, MIMICS, and CORPSE) that simulate HR fluxes within a biogeochemical test bed that provides each model with identical net primary productivity (NPP) and climate forcings. We subsequently quantify the effects of variation in simulated terrestrial carbon fluxes (NPP and HR from the three soil test-bed models) on atmospheric CO 2 distributions using a three-dimensional atmospheric tracer transport model. Our results show that atmospheric CO 2 observations can be used to identify deficiencies in model simulations of the seasonal cycle and interannual variability in HR relative to NPP. In particular, the two models that explicitly simulated microbial processes (MIMICS and CORPSE) were more variable than observations at interannual timescales and showed a stronger-than-observed temperature sensitivity. Our results prompt future research directions to use atmospheric CO 2 , in combination with additional constraints on terrestrial productivity or soil carbon stocks, for evaluating HR fluxes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

The ABCflux database: Arctic–boreal CO 2 flux observations and ancillary information aggregated to monthly time steps across terrestrial ecosystems

Past efforts to synthesize and quantify the magnitude and change in carbon dioxide (CO 2 ) fluxes in terrestrial ecosystems across the rapidly warming Arctic–boreal zone (ABZ) have provided valuable information but were limited in their geographical and temporal coverage. Furthermore, these efforts have been based on data aggregated over varying time periods, often with only minimal site ancillary data, thus limiting their potential to be used in large-scale carbon budget assessments. To bridge these gaps, we developed a standardized monthly database of Arctic–boreal CO 2 fluxes (ABCflux) that aggregates in situ measurements of terrestrial net ecosystem CO 2 exchange and its derived partitioned component fluxes: gross primary productivity and ecosystem respiration. The data span from 1989 to 2020 with over 70 supporting variables that describe key site conditions (e.g., vegetation and disturbance type), micrometeorological and environmental measurements (e.g., air and soil temperatures), and flux measurement techniques. Here, we describe these variables, the spatial and temporal distribution of observations, the main strengths and limitations of the database, and the potential research opportunities it enables. In total, ABCflux includes 244 sites and 6309 monthly observations; 136 sites and 2217 monthly observations represent tundra, and 108 sites and 4092 observations represent the boreal biome. The database includes fluxes estimated with chamber (19 % of the monthly observations), snow diffusion (3 %) and eddy covariance (78 %) techniques. The largest number of observations were collected during the climatological summer (June–August; 32 %), and fewer observations were available for autumn (September–October; 25 %), winter (December–February; 18 %), and spring (March–May; 25 %). ABCflux can be used in a wide array of empirical, remote sensing and modeling studies to improve understanding of the regional and temporal variability in CO 2 fluxes and to better estimate the terrestrial ABZ CO 2 budget.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS1972

Preferential orientation of CO adsorption on Ni as determined by extended Hueckel calculations.

The adsorption of CO on the nickel surface has been calculated using a modified extended Hueckel technique for a number of different orientations of the CO with respect to the nickel surface. The calculations show that double site adsorption with the CO molecule normal to the surface and the carbon atom closest to the metal gives the most stable configuration (2.57 eV). The single site absorbs with an energy of 2.39 eV. However, other configurations also give fairly large bonding energies. The CO normal to the surface with oxygen closest to the metal gives a heat of adsorption of 0.37 eV. Two-center adsorption with the CO axis parallel to the surface and the molecule symmetrically placed between the nearest neighbors gives a chemisorption energy of 1.34 eV. These values compare with an experimental value of 1.98 eV.

Robertson, J. C.↗
NASA NTRS1972

Lifetime and quenching of CO /a super 3 pi/ produced by recombination of CO2 ions in a helium afterglow.

Demonstration that rapid dissociative recombination of CO2(+) in a flowing, helium afterglow is an efficient source of CO in the a super 3 pi metastable state. Ions produced by mixing CO2 with He(2 super 3 S) recombine to produce a CO metastable afterglow with a number density as great as 10 to the 9th per sq cm. Monitoring of the (a super 3 pi-X super 1 sigma) Cameron transition in CO was used to study the lifetime and quenching of CO (a super 3 pi) by CO2, N2, NO, and He. Recombination of CO2(+) also produces CO in the d super 3 delta and a' super 3 sigma states.

Wauchop, T. S.↗
NASA NTRS1973

The adsorption and decomposition of CO on Pt/111/.

A cylindrical mirror electron energy analyzer has been used to study the adsorption and decomposition of CO on an initially clean Pt(111) surface. The observed rate of adsorption and fractional surface coverage as a function of CO exposure are identical to those observed previously in this laboratory by a flash filament adsorption technique. This result provides an absolute calibration of the Auger spectrometry system for carbon and oxygen. Beam-induced decomposition of CO was observed at high incident fluxes. The surface oxygen coverage decreased exponentially to zero during electron bombardment, while surface carbon decreased and then levelled off at a finite value. CO adsorption studies on this carbon contaminated surface showed decreasing CO adsorption rate and decreasing saturation coverage with increasing carbon contamination.

Martinez, J. M.↗
NASA NTRS1976

Interactions of CH4 and CO in the earth's atmosphere

Global distributions, sources, and sinks of methane and carbon monoxide in upper and lower levels of the earth's atmosphere, and the global budgets of methane and carbon monoxide, are studied, with emphasis on cumulative pollution. Stratospheric contents, vertical profiles of concentrations, simulation of vertical transport through the atmosphere, and latitudinal distributions are examined. Diffuse and localized (urban) concentrations of CO as pollutant are studied, and anthropogenic sources and sinks for CH4 and CO are considered. Perturbation of the CH4-CO-CO2 cycle, crucial to self-cleansing mechanisms of the troposphere, by anthropogenic CO emissions, and the effect of CO long life as global pollutant, are investigated.

Wofsy, S. C.↗
NASA NTRS1979

The implications of CO production in electrical discharges

The high temperature chemistry of the N-O-H-C system has been studied to determine the production of NO and CO by atmospheric lightning. The yield of NO is found to be equivalent to results obtained for a pure N2/O2 atmosphere. The CO yield is highly dependent upon the detailed cooling processes within the discharge and thus an experiment designed to measure the CO source in discharges could yield useful insights into the discharge itself. An upper limit of 3.5 x 10 to the 11th g CO per yr is estimated for the global CO source from lightning.

Chameides, W. L.↗
NASA NTRS1979

Expansion cooled CO nuclear pumped laser

The paper describes a series of experiments designed to investigate the performance of a fission fragment excited CO laser with gasdynamic cooling. The experiments use a wall source of fission fragments to provide excitation of CO or CO gas mixtures. A separate investigation examines the effects on vibrational excitation distribution of CO or CO gas mixtures with the addition of UF6.

Davis, J. F.↗
NASA NTRS1980

Brightness profiles of CO/+/ in the ionosphere of Comet West /1976 VI/

The observed sunward and tailward brightness profiles of the (2-0) band of the (A2Pi-X2Sigma) system of CO(+) (4260 A) in Comet West (1976 VI) are established over a range of heliocentric distance from 0.440 to 0.842 AU. From these data the variation with heliocentric distance of the CO(+) production rate is investigated along with the size of the contact surface (the diameter of the onset of the tail). A photoionization model is proposed for the production of CO(+) in Comet West in which CO photoionization is considered to be the principle source of CO(+); the model is consistent with the observational data and the MHD theories.

Combi, M. R.↗
NASA NTRS1980

Observations of CO in the stratosphere of Venus via its J = 0 - 1 rotational transition

Carbon monoxide has been observed in the stratosphere of Venus at phase angles of 180 and 120 deg via the J = 0 - 1 rotational transition at 115.2712 GHz. The mixing ratio profile of CO has been obtained by fitting the theoretical spectrum produced by a small number of layers with constant CO mixing ratio to the line profile, and the results suggest that the CO mixing ratio below the 1-mb level increased by at least a factor of 10 between 180 and 120 deg phase angles. The depletion of CO on the nightside of the planet was not anticipated and may require either a new loss mechanism for CO which can operate without sunlight or an increase in the amount of vertical mixing on the nightside.

Schloerb, F. P.↗
NASA NTRS1981

Far-infrared observations of shocked CO in Orion

The J = 27-26 and J = 30-29 transitions of CO have been detected in the Orion molecular cloud. These detections, together with an improved measurement of the J = 21-20 transition, allow estimation of the temperature and density of the shocked material and the fractional abundance of CO. By solving the equations of detailed balance for J less than or equal to 50 and fitting the data to a two-component model consistent with earlier 2-micron and 12-micron H2 observations, it is shown that the hot (2000 K) component has a density of approximately 1.0 x 10 to the 6th/cu cm, while the cooler component lies in the range of 400-1000 K and is 2-5 times more dense. Approximately 25% of the carbon is in the form of CO. The spatial extent of the hot CO has also been examined by observing the J = 21-20 transition at a number of positions, and it is found to be distributed similarly to the H2 lines. In addition, a search for J = 21-20 and J = 22-21 CO emission from six other sources has resulted in 3-standard-deviation upper limits of a factor of 10 below the intensity of the Orion lines.

Storey, J. W. V.↗
NASA NTRS1981

A measurement of the hyperfine structure of CO-17

It is pointed out that the isotope of carbon monoxide, CO-17, has appreciable hyperfine structure caused by the electric quadrupole and the magnetic dipole interactions of the O-17 nucleus which has a spin of 5/3. During a radioastronomical study of the structure and dynamics of cold interstellar clouds, it was found that the Bok globule B335 had an extremely small velocity dispersion such that the hyperfine components are clearly resolved. A graph is provided which shows the antenna temperature (a measure of intensity) of the CO-17 emission as a function of frequency. The hyperfine constants and line frequencies were redetermined for the CO-17 J=1 yields 0 rational transition. The observation of CO-17 was carried out with a 7 meter Cassegrain antenna during 1979 and 1980. The CO-17 molecular line parameters are listed in a table.

Frerking, M. A.↗
NASA NTRS1982

On Kaplun's optimal co-ordinates

Optimal co-ordinates were introduced by Kaplun (1954) as a result of his study on the role of co-ordinate systems in boundary-layer theory. In this paper the basic ideas of optimal co-ordinates are examined and many restrictions of Kaplun's optimal co-ordinates are removed. His rule for constructing optimal co-ordinates is found to apply unaltered to axisymmetric flows, to flows with oncoming streams containing vorticity, to free boundary layers such as jets, to free-convection flows and to compressible flows. It is also extended to unsteady boundary layers, and to three-dimensional boundary layers using a pair of stream functions.

Legner, H. H.↗
NASA NTRS1982

Chemisorption of CO on particulate deposits of platinum

Morphology and CO chemisorption properties are studied as a function of particle size for the case of particulate Pt films, vapor-deposited onto ultrahigh vacuum-cleaved and heat-treated mica surfaces at a 200 C substrate temperature. The particles were found to be mostly irregular in shape and randomly-oriented, with two desorption peaks after CO absorption at 60 C: (1) an alpha peak, at 120 C, attributed to smooth particle surfaces, and (2) a beta peak, at about 175 C, attributed to particle edges and steps. Transmission electron microscopy showed that major changes occur in particle morphology during absorption-desorption cycling, so that the decrease in CO desorption flux may be interpreted as due to particle restructuring, rather than contamination by CO decomposition as in the cases of Ni or Pd on mica. Auger electron spectroscopy corroborates the lack of CO decomposition, even for the case of very small Pt particles.

Doering, D. L.↗
NASA NTRS1982

Microwave spectra of terrestrial mesospheric CO

Mesospheric CO was observed in absorption against the moon in early December 1979 at a wavelength of 1.3 mm and in early December 1980 at 2.6 mm with the 10.4-m millimeter wavelength telescope at the Owens Valley Radio Observatory. No significant change in the column density of CO above about 65 km is found between the 1979 and 1980 observations. Comparison with other published spectra of mesospheric CO suggests a large seasonal variation (about a factor of 2-3) in the column density of CO above 65 km, with a maximum in winter and a minimum in summer. It is concluded that the understanding of CO in the mesosphere can be improved with earth-based microwave measurements, but data with high signal-to-noise ratios must be obtained.

Clancy, R. T.↗