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At least 469 records · Page 26

Ultrahigh Areal Capacity Holey Graphene Air Cathodes for Li-O2 and Li-CO2 Batteries

Advanced lithium (Li) batteries using gaseous cathode reactants such as oxygen (O2) and carbon dioxide (CO2)are attractive energy storage platforms because the gases are obtained externally and thus not accounted for in the total battery weight when fully charged.The discharge products at the cathode, typically Li2O2 for Li-O2 batteries and Li2CO3 for Li-CO2 batteries, are insoluble in the electrolyte.Therefore, in order for such batteries to function properly, an “air cathode”,which is a conductive scaffold within the battery cell,is required as a physical location for cathode electrochemical reactions to occur. Prior research has identified many carbon nanomaterials such as carbon nanotubes and graphene as viable choices for air cathode scaffold, while various metallic and metal-free catalytic systems integrated onto carbon-based air cathodes have been developed to improve the sluggish discharge and charge reactions. For future practical applications, the air cathode must exhibit a usable capacity per unit electrode area, or areal capacity, a critical parameter that has been largely overlooked so far in this field. In order to achieve high areal capacity, the air cathode must exhibit a sufficient amount of accessible void volume per unit electrode area while maintaining the conductive scaffold integrity during the entire electrochemical process. Here we present an ultrathick,holey graphene-based air cathode platform fabricated from a facile dry compression process that exhibits remarkable areal capacity values. Holey graphene is a carbon nanomaterial derived from graphene, but with nanometer sized holes through the nanosheet thickness.The presence of these holes enhances mass transport through electrode thickness and also enables the unique dry-press fabrication process that is not achievable using other carbon scaffold materials.The dry-pressed holey graphene air cathode platform is not only compatible with catalyst incorporation to improve battery reaction kinetics, but also allows for novel engineering of electrode architectures that is not achievable using conventional electrode fabrication approaches.The applications of such highly versatile, ultrahigh areal capacity air cathode platforms to both Li-O2 and Li-CO2 battery chemistries will be discussed.

Li-O2 batteries, Li-CO2 batteries, holey graphene,↗

Dynamical and Trace Gas Responses of the Quasi-Biennial Oscillation to Increased CO2

Long-term projections of the Quasi-Biennial Oscillation (QBO) remain uncertain. Using the high-top \Middle Atmosphere" (MA) version of the NASA Goddard Institute for Space Studies (GISS) ModelE (E2.2-AP), we show that increased CO2 reduces the QBO period and weakens its amplitude, consistent with results from recent multimodel studies. The amplitude response is asymmetric, with the easterly phase weakening more than the westerly phase. Results from both coupled atmosphere{ocean and climatologically fixed sea surface temperature simulations link the period response to changes in parameterized convective gravity wave fluxes, whereas the amplitude changes are more closely tied to changes in tropical upwelling. Comparisons of simulations with and without ozone-dynamical feedbacks reveal that ozone feedbacks increase the QBO amplitude and period in pre-industrial control simulations, and reduce the response of the amplitude to increased CO2. The response of stratospheric tracers to projected changes in the QBO is also investigated. Similarity between results using fully interactive (trace gas and aerosol) versus linearized ozone chemical mechanisms suggests that the QBO response to CO2 does not depend on additional chemical feedbacks beyond those associated with ozone, which implies that projected QBO changes may be credibly represented using simpli fied stratospheric ozone schemes.

GISS Model E2.2-AP↗

Spatial Heterogeneity in CO2, CH4, and Energy Fluxes: Insights from Airborne Eddy Covariance Measurements Over the Mid-Atlantic Region

The exchange of carbon between the Earth’s atmosphere and biosphere influences the atmospheric abundances of carbon dioxide (CO2) and methane (CH4). Airborne eddy covariance can quantify surface-atmosphere exchange from landscape-to-regional scales, offering a unique perspective on carbon cycle dynamics. We use extensive airborne measurements to quantify fluxes of sensible heat, latent heat, CO2, and CH4across multiple ecosystems in the Mid-Atlantic region during September 2016 and May 2017. In conjunction with footprint analysis and land cover information, we use the airborne dataset to explore the effects of landscape heterogeneity on measured fluxes. Our results demonstrate large variability in CO2 uptake over mixed agricultural and forested sites, with fluxes ranging from -3.4 ± 0.7 to -11.5 ± 1.6μmol m-2s-1 for croplands and -9.1 ± 1.5 to -22.7 ± 3.2μmol m-2s-1for forests. We also report substantial CH4emissions of 32.3 ± 17.0to 76.1 ± 29.4nmol m-2s-1 from a brackish herbaceous wetland and 58.4± 12.0 to 181.2 ± 36.8nmol m-2s-1 from a freshwater forested wetland. Comparison of ecosystem-specific aircraft observations with measurements from eddy covariance flux towers along the flight path demonstrate that towers capture ~30–75% of the regional variability in ecosystem fluxes. Diel patterns measured at the tower sites suggest that peak, midday flux measurements from aircraft accurately predicts net daily CO2exchange. We discuss next steps in applying airborne observations to evaluate bottom-up flux models and improve understanding of the biophysical processes that drive carbon exchange from landscape-to-regional scales.

airborne measurements to quantify fluxes of sensib↗

Analysis of Volatile Compounds from CO2 Removal Systems

One of the primary concerns when designing CO2 scrubber systems that will be integrated with a Sabatier reactor to produce water and methane is the amount of water released from the scrubber. Because the gas stream entering a Sabatier reactor must be compressed, water entering the reactor can condense and compromise the integrity of the system, thus rendering its valuable conversion capability useless. When the Johnson Space Center Environmental Chemistry Laboratory was tasked to develop an assay to quantify the water concentration in air samples from CO2 scrubbers, additional testing was also performed to see if any other compounds were being concentrated on the scrubbers. It was thought that the efficiency of the scrubber systems could be quantified by comparing the differences in samples from the ambient air on the International Space Station (ISS) to the exit gas of the scrubber. As this analysis was carried out, it became evident that the concentrations of certain volatile compounds were higher in the samples from the scrubbers than they were in nominal environmental samples. This meant these compounds were being retained and concentrated on the scrubber beds. Based on this finding, concerns were raised about their potential for these compounds to poison the Sabatier reactor. Further investigation was required to identify these compounds due to their high concentrations and unique matrix of the CO2 scrubber exhaust. This paper describes these events as well as the process that was developed to identify the volatile compounds that increased. An examination of how much the certain compounds can be concentrated by the scrubber systems is also included.

Volatiles↗

Analysis of Volatile Compounds From CO2 Removal Systems

One of the primary concerns when designing CO2 scrubber systems that will be integrated with a Sabatier reactor to produce water and methane is the amount of water released from the scrubber. Because the gas stream entering a Sabatier reactor must be compressed, water entering the reactor can condense and compromise the integrity of the system, thus rendering its valuable conversion capability useless. When the Johnson Space Center Environmental Chemistry Laboratory was tasked to develop an assay to quantify the water concentration in air samples from CO2 scrubbers, additional testing was also performed to see if any other compounds were being concentrated on the scrubbers. It was thought that the efficiency of the scrubber systems could be quantified by comparing the differences in samples from the ambient air on the International Space Station (ISS) to the exit gas of the scrubber. As this analysis was carried out, it became evident that the concentrations of certain volatile compounds were higher in the samples from the scrubbers than they were in nominal environmental samples. This meant these compounds were being retained and concentrated on the scrubber beds. Based on this finding, concerns were raised about their potential for these compounds to poison the Sabatier reactor. Further investigation was required to identify these compounds due to their high concentrations and unique matrix of the CO2 scrubber exhaust. This paper describes these events as well as the process that was developed to identify the volatile compounds that increased. An examination of how much the certain compounds can be concentrated by the scrubber systems is also included.

Volatiles↗

Dissociative excitation of vacuum ultraviolet emission features by electron impact on molecular gases. 3: CO2

Vacuum ultraviolet multiplets of C I, C II, and O I were produced by electron impact of CO2. Absolute emission cross sections for these multiplets were measured from threshold to 350 eV. The electrostatically focussed electron gun used in this series of experiments is described in detail. The atomic multiplets which were produced by dissociative excitation of CO2 and the cross sections at 100 eV are given. The dependence of the excitation functions on electron energy shows that these multiplets are produced by electric-dipole-allowed transitions in CO2.

Mumma, M. J.↗

Dissociative excitation of vacuum ultraviolet emission features by electron impact on molecular gases. 3: CO2

Vacuum ultraviolet multiplets of C I, C II, and O I were produced by electron impact on CO2. Absolute emission cross sections for these multiplets were measured from threshold to 350 eV. The electrostatically focused electron gun used is described in detail. The atomic multiplets which were produced by dissociative excitation of CO2 and the cross sections at 100 eV are presented. The dependence of the excitation functions on electron energy shows that these multiplets are produced by electric-dipole-allowed transitions in CO2.

Mumma, M. J.↗

Climatic modification by CO2, H2O, and aerosol

Research is reported on the effects of increasing the CO2, aerosols, and water content of the atmosphere on the surface temperature and climatology. An atmospheric model is described with the incoming solar radiation for a planetary albedo of 33 percent, surface temperature of 288 K, relative humidity of 75 percent, cloud cover of 48 percent, CO2 of 0.3 parts per thousand, and aerosol density of two million per square centimeter. The results show that if the CO2 increases by a factor of 1000 or more, the total pressure of the atmosphere increases, and the earth may become as hot as Venus. It is also shown that as the amount of dust particles in the atmosphere increases, the solar radiation decreases, and the surface temperature lowers.

Rasool, I.↗

Digital simulation and experimental evaluation of the CO2-H(plus) control of pulmonary ventilation

Previous models of the CO2-H(+) control of ventilation have been concerned either with the response to CO2 inhalation, or the response to perfusion of the surface of the medulla with mock cerebrospinal fluid having a high P sub CO2. Simulation of both responses with the same model has not been attempted. The purpose of the present study was two fold; first to develop such a model and, second, to obtain experimental data from human subjects for both developing this model and for evaluating this and future models.

Milhorn, H. T., Jr.↗

Gain and power of CO2 gasdynamic lasers.

This paper presents experimental and theoretical studies of the small signal gain and the radiant power for one configuration of CO2 gasdynamic lasers to define the optimum-gas temperature, pressure and gas compositions for the gain and the laser power. The laser was operated with two gas mixtures (CO2-N2-He and CO2-N2-H2O) at temperatures of 800-2200 deg K, pressures of 2-16 atm, and a wide range of gas compositions. For this laser optimum gas temperatures were roughly 1500-1600 deg K for gain and more than 2200 deg K for power. It was found that the gasdynamic laser would not oscillate for He or H2O concentrations of less than 10% and 1%, respectively. The various kinetic processes for establishing gain and the various laser cavity parameters that determine laser power were examined. The theories were assessed for their ability to predict gain and power. In most cases, the gain theory gave excellent quantitative results whereas the power theory gave only qualitative results. Laser power of nearly 2 kw was obtained.

Lee, G.↗

Gain kinetics of CO2 gasdynamic laser mixtures at high pressure.

Description of a combined analytical and experimental investigation of rapidly expanded CO2 laser mixtures. Study of the vibrational kinetics indicates that population inversions with high vibrational energy density can be produced at high pressures by utilizing low (starved) concentrations of CO2. Scaling laws for predicting the gain of starved systems are developed. A description is given of gain measurements carried out using a CO2 laser to probe the flow in a nozzle at the point where the Mach number is approximately four. Population inversions at static pressures as high as about 1 atm have been observed and found to be in reasonable agreement with predictions.

Christiansen, W. H.↗

Line shape parameters for HCl and HF in a CO2 atmosphere.

Results of high-resolution (0.1 cm/cm) on several CO2-broadened lines in the fundamentals of HCl35 and HCl37. Line intensities, half-widths, and shapes were determined at room temperature. Half-widths in HCl-CO2 collisions were computed for several temperatures, employing Anderson's (1949) theory. The measured shapes of HCl lines broadened by CO2 are described by a semiempirical super-Lorentzian shape. The curve-of-growth for this line shape is derived in terms of a function similar to the Ladenburgh-Reiche function. Absorption between R(0) and P(1) is affected by the appearance of several pressure-induced Q-branch lines, at the pressures from 1 to 10 atm used in the present study.

Varanasi, P.↗

A transient performance method for CO2 removal with regenerable adsorbents

A computer program is described which can be used to predict the transient performance of vacuum-desorbed sorbent beds for CO2 or water removal, and composite beds of two sorbents for simultaneous humidity control and CO2 removal. The program was written primarily for silica gel and molecular sieve inorganic sorbents, but can be used for a variety of adsorbent materials. Part 2 of this report describes a computer program which can be used to predict performance for multiple-bed CO2-removal sorbent systems. This program is an expanded version of the composite sorbent bed program described in Part 1.

Hwang, K. C.↗

CO2 removal by solid amine sorbents. 1: Experimental studies of amine resin IR-45 with regard to spacecraft applications. 2: Computer program for predicting the transient performance of solid amine sorbent systems

The sorbent behavior of solid amine resin IR-45 with regard to potential use in regenerative CO2-removal systems for manned spacecraft is considered. Measurements of equilibrium sorption capacity of IR-45 for water and for CO2 are reported, and the dynamic mass transfer behavior of IR-45 beds is studied under conditions representative of those expected in a manned spacecraft. A digital computer program was written for the transient performance prediction of CO2 removal systems comprised of solid amine beds. Also evaluated are systems employing inorganic molecular-sieve sorbents. Tests show that there is definitely an effect of water loading on the absorption rate.

Wright, R. M.↗

Electron impact excitation and assignment of the low-lying electronic states of CO2

Electron scattering spectra of CO2 are reported in the 7 to 10 eV energy-loss range, at energies of 0.2, 0.35, 0.6, 0.7, and 7.0 eV above threshold, and at a scattering angle of 90 deg. Several new distinct overlapping continua with weak, diffuse bands superimposed are observed to lie in this energy-loss range. The experimental spectra are discussed in the light of recent ab initio configuration-interaction calculations of the vertical transition energies of CO2. The experimental spectra are shown to be consistent with the excitation states of CO2.

Hall, R. I.↗

Condensation in CO2 free jet expansions. II - Growth of small clusters.

An investigation into the kinetics of molecular clustering processes which occur in the highly supersaturated vapor of a CO2 free jet is described. Terminal cluster concentrations in expansions from room temperature and reservoir pressures in the range from 400 to 900 torr were determined for trimeric CO2 for nozzle diameters of .0076 cm, .015 cm, and .023 cm and in the case of CO2 tetramer and pentamer for .015 cm nozzle diameter. The measurements were made mass spectrometrically in a supersonic molecular beam apparatus. A kinetic analysis was developed from an extension of the critical nucleus concept of nucleation theory and rate equations based on intermolecular collisions. The observed cluster populations could be accounted for by the theory by adopting sticking probabilities of approximately .03 for monomer impinging on dimer, trimer, and tetramer.

Dorfeld, W. G.↗

Excitation of the CO fourth positive system by the dissociative recombination of CO2/+/ ions.

The fourth positive system of CO has been excited in a static afterglow experiment by the dissociative recombination of CO2(+) ions. From combined absolute optical and microwave measurements the specific recombination coefficient for exciting the CO system was found to be (2 plus 1 or minus 0.5) x 10 to the minus 8th cu cm/sec. This value represents approximately 5% of the total recombination coefficient (4.0 plus or minus 0.5) x 10 to the minus 7th cu cm/sec measured in this experiment, implying that CO2(+) dissociative recombination will contribute significantly to the excitation of the CO fourth positive system in the Martian airglow. Corroborative electron heating experiments showed that the magnitude of the specific recombination coefficient decreased as the electron temperature was increased. Evidence was also found for the presence of vibrationally excited ions in the CO2(+) plasma, a result which indicates that analogous laboratory studies on the dissociative recombination of O2(+), N2(+), and NO(+) ions may have also involved vibrationally hot plasmas.

Gutcheck, R. A.↗

CO2 laser design procedure.

A simple but powerful formalism is presented that allows one to physically design a sealed CO2 laser of any specified fundamental transverse-mode output power. The design material presented, graphically whenever possible, also allows one to determine the effect on the others of varying one design parameter. Although the formalism presented is based on some empirical and some theoretical parametric interrelationships pertinent to the CO2 laser, the treatment is general and with appropriate adjustments can be applied to other laser systems as well. The design of a 5-W sealed CO2 laser is presented to illustrate the use of the formalism developed.

Fahlen, T. S.↗