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All sourcesNASA NTRSDOE OSTI
NASA NTRS1979

Water vapor-nitrogen absorption at CO2 laser frequencies

The paper reports the results of a series of pressure-broadened water vapor absorption measurements at 27 CO2 laser frequencies between 935 and 1082 kaysers. Both multiple traversal cell and optoacoustic (spectrophone) techniques were utilized together with an electronically stabilized CW CO2 laser. Comparison of the results obtained by these two methods shows remarkable agreement, indicating a precision which has not been previously achieved in pressure-broadened studies of water vapor. The data of 10.59 microns substantiate the existence of the large (greater than 200) self-broadening coefficients determined in an earlier study by McCoy. In this work, the case of water vapor in N2 at a total pressure of 1 atm has been treated.

Peterson, J. C.↗
NASA NTRS1997

Roto-Translational Collision-Induced Absorption of CO2 for the Atmosphere of Venus at Frequencies from 0 to 250 cm(exp -1), at Temperatures from 200 to 800 K

The collision-induced absorption (CIA)of gaseous CO2 is the primary source of far-infrared opacity of the atmosphere of Venus. At the temperatures and densities of the venusian atmosphere, the absorption is due mainly to binary collisions of CO2 molecules. Using a realistic anisotropic intermolecular potential and assuming the absorbing dipole to be due to the electrostatic induction and a quantum overlap, a series of molecular dynamics simulations were performed for the temperature range 200 to 800 K, and the roto-translational (RT) collision-induced absorption spectra at frequencies from 0 to 250 cm(exp -1) were derived. The absorption coefficient in the submillimeter region, used in constituency retrieval studies, decreases more than 10 times in the temperature range 200 to 800 K. On the other hand, the absorption coefficient at 800 K and at the frequency range above 150 cm(exp -1) was found to be almost 10 times higher than at 200 K. Earlier works relied on experimental RT CIA data at a fixed temperature of 300 K. The new, temperature-dependent absorption bands may, when included in the analysis of the atmospheric radiative transfer of the planet, help explain the observed high far-infrared opacity of the lower layers of the atmosphere. To make the results of the simulations readily available for atmospheric abundance and radiative transfer analysis, an analytic model of the roto-translational collision-induced absorption spectral profile, applicable from 200 to 800 K, is being proposed here. The FORTRAN computer code of this newly developed model is available from the authors on request.

Gruszka, Marcin↗
NASA NTRS1994

Spectral Moments of Collision-Induced Absorption of CO2 Pairs: The Role of the Intermolecular Potential

In this paper we examine the role of the anisotropy of the intermolecular potential in the rototranslational collision-induced absorption of the CO2 pairs. Using newly developed formulas that include the effects of anisotropy of the potential to all orders, we calculate the two lowest spectral moments gamma(prime), and alpha(prime), for four different classes of C02 pair potentials and compare the results with the experimental values. We assumed only multipolar induction in the process of forming the induced dipole, with the second-order contributions included. Using a site-site LJ and a site-site semi-ab initio intermolecular potentials we were able to reproduce the experimental values of gamma(prime), and alpha(prime) moments over entire temperature range from 230 to 330 K. Also, the role of an electrostatic interaction between two C02 molecules and its impact on the spectral moments is thoroughly investigated. An isotropic core with a point quadrupole centered at each molecule is shown to be an inadequate representation of the C02-CO2 potential. Additionally, we show the results obtained with the first- and second-order perturbation theory to be more than twice too small.

Gruszka, Marcin↗
NASA NTRS2013

Airborne Measurements of CO2 Column Concentration and Range Using a Pulsed Direct-Detection IPDA Lidar

We have previously demonstrated a pulsed direct detection IPDA lidar to measure range and the column concentration of atmospheric CO2. The lidar measures the atmospheric backscatter profiles and samples the shape of the 1,572.33 nm CO2 absorption line. We participated in the ASCENDS science flights on the NASA DC-8 aircraft during August 2011 and report here lidar measurements made on four flights over a variety of surface and cloud conditions near the US. These included over a stratus cloud deck over the Pacific Ocean, to a dry lake bed surrounded by mountains in Nevada, to a desert area with a coal-fired power plant, and from the Rocky Mountains to Iowa, with segments with both cumulus and cirrus clouds. Most flights were to altitudes >12 km and had 5-6 altitude steps. Analyses show the retrievals of lidar range, CO2 column absorption, and CO2 mixing ratio worked well when measuring over topography with rapidly changing height and reflectivity, through thin clouds, between cumulus clouds, and to stratus cloud tops. The retrievals shows the decrease in column CO2 due to growing vegetation when flying over Iowa cropland as well as a sudden increase in CO2 concentration near a coal-fired power plant. For regions where the CO2 concentration was relatively constant, the measured CO2 absorption lineshape (averaged for 50 s) matched the predicted shapes to better than 1% RMS error. For 10 s averaging, the scatter in the retrievals was typically 2-3 ppm and was limited by the received signal photon count. Retrievals were made using atmospheric parameters from both an atmospheric model and from in situ temperature and pressure from the aircraft. The retrievals had no free parameters and did not use empirical adjustments, and >70% of the measurements passed screening and were used in analysis. The differences between the lidar-measured retrievals and in situ measured average CO2 column concentrations were <1.4 ppm for flight measurement altitudes >6 km.

Lidar↗
DOE OSTI2020

Solvent-Based Absorption

Solvent-based CO2 absorption processes are the oldest and most mature technology, having been deployed at what would be considered full-scale for post-combustion CO2 capture. There are many commercial 1st and 2nd generation technologies such as Econamine FG+, CANSOLV, Oase Blue, KS-1, with dozens if not hundreds of 3rd generation solvents that are been studied at varying stages of testing. While there are many solvents that are under development, nearly all solvents function on the same physical and chemical principles and it is not surprising that they all have similar configurations with somewhat comparable levels of performance. The enhancements in energy efficiency for solvents have come primarily from the engineering advancements over many decades of refinement, though surprisingly little has changed with respect to the molecular structure of solvents over the same period of time. In this chapter, we explain the tenets of solvent-based processes and provide a chronological timeline of solvents throughout their nearly 90-year history with discussions of why and how advancements in solvent efficiency have been achieved and we conclude with an outlook for the future of solvents and their place in CCUS.

Heldebrant, David J.↗
NASA NTRS2014

Advanced Sine Wave Modulation of Continuous Wave Laser System for Atmospheric CO2 Differential Absorption Measurements

NASA Langley Research Center in collaboration with ITT Exelis have been experimenting with Continuous Wave (CW) laser absorption spectrometer (LAS) as a means of performing atmospheric CO2 column measurements from space to support the Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) mission.Because range resolving Intensity Modulated (IM) CW lidar techniques presented here rely on matched filter correlations, autocorrelation properties without side lobes or other artifacts are highly desirable since the autocorrelation function is critical for the measurements of lidar return powers, laser path lengths, and CO2 column amounts. In this paper modulation techniques are investigated that improve autocorrelation properties. The modulation techniques investigated in this paper include sine waves modulated by maximum length (ML) sequences in various hardware configurations. A CW lidar system using sine waves modulated by ML pseudo random noise codes is described, which uses a time shifting approach to separate channels and make multiple, simultaneous online/offline differential absorption measurements. Unlike the pure ML sequence, this technique is useful in hardware that is band pass filtered as the IM sine wave carrier shifts the main power band. Both amplitude and Phase Shift Keying (PSK) modulated IM carriers are investigated that exibit perfect autocorrelation properties down to one cycle per code bit. In addition, a method is presented to bandwidth limit the ML sequence based on a Gaussian filter implemented in terms of Jacobi theta functions that does not seriously degrade the resolution or introduce side lobes as a means of reducing aliasing and IM carrier bandwidth.

Campbell, Joel F.↗
DOE OSTI2024

Nonconvex Robust Optimization for the Design and Operation of Advanced Energy Systems Using PyROS

This work discusses recent advances of the two-stage robust optimization (RO) solver PyROS and applications to advanced energy systems optimization. To demonstrate the computational performance and reliability of PyROS, a study on a monoethanolamine (MEA)-based CO2 absorption flowsheet is presented. (Near-)robust feasible designs for CO2 absorption flowsheet at high carbon capture are obtained with the PyROS solver. The results demonstrate that the PyROS solver, including recent extensions to multi-stage RO settings, provides a reliable avenue to optimize the design and operation of advanced energy systems subject to various sources of parametric uncertainty.

Sherman, Jason↗
NASA NTRS1975

Comments on "Venus' spectroscopic phase variation: Implications of the Mariner 10 photographs

From a misinterpretation of Mariner 10 pictures, Chamberlain (1974) constructed a model in which he used horizontal variations in the Venus atmosphere to explain the phase-variation of CO2 absorption at small phase angles. Published observations of spatial variations in CO2 absorption on Venus show that they are too small to explain the phase effect. The question of uniqueness that is, if more than one model can explain the phase-effect observations is discussed. Before this question can be answered, a realistic model that does account for the data must be constructed. No such calculations exist.

Young, A. T.↗
NASA NTRS2010

NASA's Advancements in Space-Based Spectrometry Lead to Improvements in Weather Prediction and Understanding of Climate Processes

AIRS (Atmospheric Infra-Red Sounder), was launched, in conjunction with AMSU-A (Advanced Microwave Sounding Unit-A) on the NASA polar orbiting research satellite EOS (Earth Observing System) Aqua satellite in May 2002 as a next generation atmospheric sounding system. Atmospheric sounders provide information primarily about the vertical distribution of atmospheric temperature and water vapor distribution. This is achieved by measuring outgoing radiation in discrete channels (spectral intervals) which are sensitive primarily to variations of these geophysical parameters. The primary objectives of AIRS/AMSU were to utilize such information in order to improve the skill of numerical weather prediction as well as to measure climate variability and trends. AIRS is a multi-detector array grating spectrometer with 2378 channels covering the spectral range 650/cm (15 microns) to 2660/cm (3.6 microns) with a resolving power (i/a i) of roughly 1200 where a i is the spectral channel bandpass. Atmospheric temperature profile can be determined from channel observations taken within the 15 micron (the long-wave CO2 absorption band) and within the 4.2 micron (the short-wave CO2 absorption band). Radiances in these (and all other) spectral intervals in the infrared are also sensitive to the presence of clouds in the instrument?s field of view (FOV), which are present about 95% of the time. AIRS was designed so as to allow for the ability to produce accurate Quality Controlled atmospheric soundings under most cloud conditions. This was achieved by having 1) extremely low channel noise values in the shortwave portion of the spectrum and 2) a very flat spatial response function within a channel?s FOV. IASI, the high spectral resolution IR interferometer flying on the European METOP satellite, does not contain either of these important characteristics. The AIRS instrument was also designed to be extremely stabile with regard to its spectral radiometric characteristics, which is critical with regard to the ability to measure accurate long term trends.

Susskind, Joel↗
DOE OSTI2021

Modeling, Design, and Testing of a Novel Biphasic Solvent-Enabled Absorption System for Post-Combustion Carbon Capture

A novel absorption process enabled by a new class of biphasic solvents for post-combustion carbon capture (BiCAP) is presently being developed at the University of Illinois at Urbana-Champaign. The new biphasic solvents are water-lean solvent blends that develop dual liquid phases with the absorbed CO2 highly enriched in one of the phases. These solvents are superior in CO2 capacity and have high thermal and oxidative stability compared to MEA. The BiCAP technology features a unique process configuration of multi-stage CO2 absorption and liquid–liquid phase separation during CO2 absorption, allowing continual separation and removal of the CO2-enriched liquid phase for maintaining low solvent viscosity and a fast absorption rate. A 40 kWe-scale skid has recently been constructed at the Abbott Power Plant in Champaign, IL, to test the BiCAP solvent in continuous operation with a slipstream of real post-combustion flue gas. Along with improvements in the stripping configuration including cold feed bypass, the process is expected to achieve a minimum reboiler duty of 2,210 kJ/kg CO2 captured at a stripper operating pressure of 6 bar.

20 FOSSIL-FUELED POWER PLANTS↗
NASA NTRS1985

The use of superoxide mixtures as air-revitalization chemicals in hyperbaric, self-contained, closed-circuit breathing apparatus

In portable breathing apparatus applications at 1 atm, potassium superoxide (KO2) has exhibited low-utilization efficiency of the available oxygen (O2) and diminished carbon dioxide-(CO2) scrubbing capacity caused by the formation of a fused, hydrated-hydroxide/carbonate product coating on the superoxide granules. In earlier work, it was discovered that granules fabricated from an intimate mixture of KO2 and calcium superoxide, Ca(O2)2, did not exhibit formation of a fused product coating and the utilization efficiency with respect to both O2 release and CO2 absorption was superior to KO2 granules when both types of granules were reacted with humidified CO2 under identified conditions. In the work described here, single pellets of KO2, KO2/Ca(O2), mixtures and commercially available KO2 tables and granules were reacted with a flow of humidified CO2 in helium at 1- and 10-atm total pressure and at an initial temperature of 40 C. In the 1-atm flow tests, the reaction rates and utilization efficiency of the KO2/Ca(O2)2 pellets were markedly superior to the KO2 pellets, tablets, and granules when the samples were reacted under identical conditions. However, at 10 atm, the rates of O2 release and CO2 absorption, as well as the utilization efficiencies of all the superoxide samples, were one-third to one-eighth of the values observed at 1 atm. The decrease in reaction performance at 10 atm compared to that at 1 atm has been attributed principally to the lower bulk diffusivity of the CO2 and H2O reactants in helium at the higher pressure and secondarily to the moderation of the reaction temperature caused by the higher heat capacity of the 10-atm helium.

Wood, P. C.↗
NASA NTRS2011

New Broadband LIDAR for Greenhouse Carbon Dioxide Gas Sensing in the Earth's Atmosphere

We present demonstration of a novel broadband lidar technique capable of dealing with the atmospherically induced variations in CO2 absorption using a Fabry-Perot based detector and a broadband laser. The Fabry-Perot solid etalon in the receiver part is tuned to match the wavelength of several CO2 absorption lines simultaneously. The broadband technique tremendously reduces the requirement for source wavelength stability, instead putting this responsibility on the Fabry- Perot based receiver. The instrument technology we are developing has a clear pathway to space and realistic potential to become a robust, low risk space measurement system.

Georgieva, Elena↗
NASA NTRS1982

A flow-system comparison of the reactivities of calcium superoxide and potassium superoxide with carbon dioxide and water vapor

A single pass flow system was used to test the reactivity of calcium superoxide with respiratory gases and the performance was compared to that of potassium superoxide. The KO2 system is used by coal miners as a self-contained unit in rescue operations. Particular attention was given to the reactivity with carbon dioxide and water vapor at different temperatures and partial pressures of oxygen, carbon dioxide, and water vapor. The calcium superoxide beds were found to absorb CO2 and H2O vapor, releasing O2. The KO2 bed, however, released O2 at twice the rate of CO2 absorption at 37 C. It is concluded that the calcium superoxide material is not a suitable replacement for the KO2 bed, although Ca(O2)2 may be added to the KO2 bed to enhance the CO2 absorption.

Wood, P. C.↗
NASA NTRS2010

A Broad Bank Lidar for Precise Atmospheric CO2 Column Absorption Measurement from Space

Accurate global measurement of carbon dioxide column with the aim of discovering and quantifying unknown sources and sinks has been a high priority for the last decade. In order to uncover the "missing sink" that is responsible for the large discrepancies in the budget the critical precision for a measurement from space needs to be on the order of 1 ppm. To better understand the CO2 budget and to evaluate its impact on global warming the National Research Council (NRC) in its recent decadal survey report (NACP) to NASA recommended a laser based total CO2 mapping mission in the near future. That's the goal of Active Sensing of CO2 Emissions over Nights, Days, and Seasons (ASCENDS) mission - to significantly enhance the understanding of the role of CO2 in the global carbon cycle. Our current goal is to develop an ultra precise, inexpensive new lidar system for column measurements of CO2 changes in the lower atmosphere that uses a Fabry-Perot interferometer based system as the detector portion of the instrument and replaces the narrow band laser commonly used in lidars with a high power broadband source. This approach reduces the number of individual lasers used in the system and considerably reduces the risk of failure. It also tremendously reduces the requirement for wavelength stability in the source putting this responsibility instead on the Fabry- Perot subsystem.

Georgieva, E. M.↗
NASA NTRS2010

Lasers and the Dynamic Mesosphere/Thermosphere of Venus

A review of ground based mid-infrared uniquely high spectral. resolution measurements of Venus dynamics, temperature, and chemistry will be presented. The described studies will focus on the use of CO2 absorption features and the discovery- and use of CO2 thermospheric non-thermal emission: lines as probes of Venus' atmosphere, from the cloud tops to approx.120 km in the thermosphere. The first investigations using infrared heterodyne spectroscopy with resolving power lambda/Delta(lambda) approx. 10(exp 6) to measure true emission line profiles and to determine their non-thermal nature and lasing component will be described. The use of the thermospheric non-thermal CO2 emission to directly measure sub-solar to anti-solar winds and zonal circulation near 110 km altitudes on Venus to approx.2 m/s accuracy will also be described. The measured emission lures are also used to obtain global maps of mesospheric/thermospheric kinetic and rotational temperatures as well as to obtain evidence of the natural lasing phenomena. Carbon dioxide absorption features globally probe lower altitudes in the atmosphere and can be used to determine nightside temperatures. Isotopic 13 CO2 absorption lines are used to probe deeper in the atmosphere to measure the sub-solar to anti-solar return flow at altitudes just above the cloud tops. These results provided a model for global circulation in the 65 - 120 km altitude region first proposed by Goldstein (1989, PhD.Thesis, U. Pennsylvania, Philadelphia, USA). Results of similar wind and temperature measurements made in recent years will be compared to earlier results to investigate changes in the circulation and temperatures since approx.1990. The high resolution infrared heterodyne technique was also used to investigate chemical processes above the cloud tops, specifically evidence and constraints on oxygen-based chemistry. Described measurements were made by infrared heterodyne spectroscopy using the Goddard Space Flight Center Infrared Heterodyne Spectrometer (IRHS) the GSFC Heterodyne Instrument for Planetary wind And Composition (HIPWAC) and the University of Cologne Tuneable Heterodyne Infrared Spectrometer (THIS).

Kostiuk, Theodor↗
NASA NTRS1992

Martian atmospheric chemistry during the time of low water abundance

The importance of odd hydrogen (or HO(x)) radicals in the catalytic recombination of carbon monoxide and oxygen in the Martian atmosphere is a well known fact. The inclusion of recent chemical kinetics data, specifically temperature-dependent CO2 absorption cross sections, into our one dimensional photochemical model shows that HO(x) is too efficient in this regard. The absorption cross sections of CO2 are smaller than previously assumed; this leads to a reduction in the photolysis rate of CO2 while the photolysis rate of H2O has increased. As a consequence the predicted mixing ratio of CO in our models is substantially less than the observed value of 6.5(10)(exp -4). Simultaneous measurements of water, ozone, and carbon monoxide were obtained in the Martian atmosphere in early Dec. 1990 (L(sub s) for Mars was 344 deg.).

Nair, Hari↗