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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS1975

Chlorine compounds and stratospheric ozone

A report by Cicerone et al. (1974) concerned with the potential size of the atmospheric perturbation produced by man-made chlorofluoromethanes is considered, giving attention to a number of errors made in the first investigation and their correction. However, the corrections do not significantly change the results reported. It had been found that chlorine oxides which arise from chlorofluoromethane usage will within 10 or 15 years provide a sink for stratospheric ozone which will dominate the natural sinks for ozone.

Cicerone, R. J.↗
NASA NTRS1975

Estimate of late 1974 stratospheric concentration of gaseous chlorine compounds /ClX/

The total concentration (ClX) versus altitude of Cl-containing molecules (principally HCl, Cl, ClO) is estimated. It is shown that the predicted present stratospheric concentrations are due to photolysis near 30 km of man-made CF2Cl2 and CFCl3, and CCl4 from a ground-level source, either man-made or natural. The contribution of CH3Cl to stratospheric ClX is evaluated from preliminary measurements of the compound at ground level. Although ground-level sources of HCl and Cl2 are large, tropospheric processes preclude significant impact on the stratosphere.

Cicerone, R. J.↗
NASA NTRS1976

High temperature reformation of aluminum and chlorine compounds behind the Mach disk of a solid-fuel rocket exhaust

Chemical reactions expected to occur among the constituents of solid-fuel rocket engine effluents in the hot region behind a Mach disk are analyzed theoretically. With the use of a rocket plume model that assumes the flow to be separated in the base region, and a chemical reaction scheme that includes evaporation of alumina and the associated reactions of 17 gas species, the reformation of the effluent is calculated. It is shown that AlClO and AlOH are produced in exchange for a corresponding reduction in the amounts of HCl and Al2O3. For the case of the space shuttle booster engines, up to 2% of the original mass of the rocket fuel can possibly be converted to these two new species and deposited in the atmosphere between the altitudes of 10 and 40 km. No adverse effects on the atmospheric environment are anticipated with the addition of these two new species.

Park, C.↗
NASA NTRS1990

Effects of atmospheric transport on column abundances of nitrogen and chlorine compounds in the arctic stratosphere

In the absence of heterogeneous processes, distributions of NO(y), HNO3, Cl(x) and HCl in the polar winter stratosphere should be determined by transport. A model simulating distributions of these species in the arctic for January and February 1989 is developed using observed fields of potential vorticity and potential temperature. Comparison of model results with column measurements from the DC-8 indicates conversion of NO(x) to HNO3, condensation of HNO3, conversion of HCl to CINO3, and conversion of HCl plus CINO3 to an unmeasured species. Heterogeneous processes strongly affect abundances of NO(y) and Cl(x) species in the winter arctic stratosphere.

Yatteau, John H.↗
NASA NTRS1995

Seasonal variations in the atmospheric distribution of a reactive chlorine compound, tetrachloroethene (CCl2 = CCl2)

Tropospheric mixing ratios of CCl2 = CCl2 were measured at remote surface locations in the Pacific between 71 deg N and 47 deg S during September and December of 1989, and March and June of 1990. The observed gradient of decreasing concentrations from the northern to the southern hemisphere, and very low concentrations in the southern hemisphere throughout the year, indicates a predominant input from the northern hemisphere. Seasonal measurements in the northern hemisphere showed maximum CCl2 = CCl2 concentrations occurring in the late summer. This distinct seasonal variation is strongly coupled to the atmompheric abundance of hydroxyl radical, the only important species responsible for CCl2 = CCl2 removal. With the estimated global CCl2 =CCl2 emissions, the lifetime is calculated to be about 5.4 months which is in good agreement with the 4.0 month estimate obtained from the inverse ratio of its measured hydroxyl reaction rate constant compared with that of methyl-chloroform CH3CCl3.

Wang, Charles J.-L.↗
DOE OSTI2016

Effects of defined mixtures of persistent organic pollutants (POPs) on multiple cellular responses in the human hepatocarcinoma cell line, HepG2, using high content analysis screening

Persistent organic pollutants (POPs) are toxic substances, highly resistant to environmental degradation, which can bio-accumulate and have long-range atmospheric transport potential. Most studies focus on single compound effects, however as humans are exposed to several POPs simultaneously, investigating exposure effects of real life POP mixtures on human health is necessary. A defined mixture of POPs was used, where the compound concentration reflected its contribution to the levels seen in Scandinavian human serum (total mix). Several sub mixtures representing different classes of POPs were also constructed. The perfluorinated (PFC) mixture contained six perfluorinated compounds, brominated (Br) mixture contained seven brominated compounds, chlorinated (Cl) mixture contained polychlorinated biphenyls and also p,p’-dichlorodiphenyldichloroethylene, hexachlorobenzene, three chlordanes, three hexachlorocyclohexanes and dieldrin. Human hepatocarcinoma (HepG2) cells were used for 2 h and 48 h exposures to the seven mixtures and analysis on a CellInsight™ NXT High Content Screening platform. Multiple cytotoxic endpoints were investigated: cell number, nuclear intensity and area, mitochondrial mass and membrane potential (MMP) and reactive oxygen species (ROS). Both the Br and Cl mixtures induced ROS production but did not lead to apoptosis. The PFC mixture induced ROS production and likely induced cell apoptosis accompanied by the dissipation of MMP. Synergistic effects were evident for ROS induction when cells were exposed to the PFC + Br mixture in comparison to the effects of the individual mixtures. No significant effects were detected in the Br + Cl, PFC + Cl or total mixtures, which contain the same concentrations of chlorinated compounds as the Cl mixture plus additional compounds; highlighting the need for further exploration of POP mixtures in risk assessment. - Highlights: • High content analysis (HCA) is a novel approach for determining toxicity of complex mixtures. • Multiple cytotoxic endpoints were investigated for defined mixtures of persistent organic pollutants (POPs). • POP mixtures are based on levels relevant to human exposure. • POP mixtures can increase ROS induction and impact mitochondrial health, which could result in apoptosis. • HCA can detect pre-lethal and reversible signs of cellular stress.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2011

Study of the VOC emissions from a municipal solid waste storage pilot-scale cell: Comparison with biogases from municipal waste landfill site

Highlights: > Follow-up of the emission of VOCs in a municipal waste pilot-scale cell during the acidogenesis and acetogenesis phases. > Study from the very start of waste storage leading to a better understanding of the decomposition/degradation of waste. > Comparison of the results obtained on the pilot-scale cell with those from 3 biogases coming from the same landfill site. > A methodology of characterization for the progression of the stabilization/maturation of waste is finally proposed. - Abstract: The emission of volatile organic compounds (VOCs) from municipal solid waste stored in a pilot-scale cell containing 6.4 tonnes of waste (storage facility which is left open during the first period (40 days) and then closed with recirculation of leachates during a second period (100 days)) was followed by dynamic sampling on activated carbon and analysed by GC-MS after solvent extraction. This was done in order to know the VOC emissions before the installation of a methanogenesis process for the entire waste mass. The results, expressed in reference to toluene, were exploited during the whole study on all the analyzable VOCs: alcohols, ketones and esters, alkanes, benzenic and cyclic compounds, chlorinated compounds, terpene, and organic sulphides. The results of this study on the pilot-scale cell are then compared with those concerning three biogases from a municipal waste landfill: biogas (1) coming from waste cells being filled or recently closed, biogas (2) from all the waste storage cells on site, and biogas (3) which is a residual gas from old storage cells without aspiration of the gas. The analysis of the results obtained revealed: (i) a high emission of VOCs, principally alcohols, ketones and esters during the acidogenesis; (ii) a decrease in the alkane content and an increase in the terpene content were observed in the VOCs emitted during the production of methane; (iii) the production of heavier alkanes and an increase in the average number of carbon atoms per molecule of alkane with the progression of the stabilisation/maturation process were also observed. Previous studies have concentrated almost on the analysis of biogases from landfills. Our research aimed at gaining a more complete understanding of the decomposition/degradation of municipal solid waste by measuring the VOCs emitted from the very start of the landfill process i.e. during the acidogenesis and acetogenesis phases.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

Versatile, ultra-low sample volume gas analyzer using a rapid, broad-tuning ECQCL and a hollow fiber gas cell

We describe a versatile mid-infrared (Mid-IR) spectroscopy system developed to measure the concentration of a wide range of gases with an ultra-low sample size. The system combines a rapidly-swept external cavity quantum cascade laser (ECQCL) with a hollow fiber gas cell. The ECQCL has sufficient spectral resolution and reproducibility to measure gases with narrow features (e.g., water, methane, ammonia, etc.), and also the spectral tuning range needed to measure volatile organic compounds (VOCs), (e.g., aldehydes, ketones, hydrocarbons), sulfur compounds, chlorine compounds, etc. The hollow fiber is a capillary tube having an internal reflective coating optimized for transmitting the Mid-IR laser beam to a detector. Sample gas introduced into the fiber (e.g., internal volume = 0.6 ml) interacts strongly with the laser beam, and despite relatively modest path lengths (e.g., L ~ 3 m), the requisite quantity of sample needed for sensitive measurements can be significantly less than what is required using conventional IR laser spectroscopy systems. Example measurements are presented including quantification of VOCs relevant for human breath analysis with a sensitivity of ~2 picomoles at a 1 Hz data rate.

broad-tuning↗
NASA NTRS1978

A kinetics investigation of several reactions involving chlorine containing compounds

The technique of flash photolysis-resonance fluorescence was utilized to study nine reactions of stratospheric importance. The tropospheric degradation reactions of seven halogenated hydrocarbons were studied to assess their possible influx into the stratosphere. There are reactions of either Cl, OH, or O(3P) species with hydrogenated species, O3 or chlorinated compounds. Apart from the kinetic measurements, the quantum yield for the production of O(1D) from O3 in the crucial wavelength region of 293 to 316.5 nm was studied by utilizing a narrow wavelength laser as the photolysis source. The product formation was monitored by measuring the fluorescence of NO2 formed through O(1D) reaction with N2O followed by NO reaction with O3 to give NO2.

Davis, D. D.↗
NASA NTRS1980

Stratospheric ozone decrease due to chlorofluoromethane photolysis - Predictions of latitude dependence

A two-dimensional model is used to predict the 1990 reduction in ozone due to the chlorine compounds formed by chlorofluoromethane (CFM) photolysis when the CFM release rate is held constant at the 1975 value. The predicted globally averaged ozone reduction of 3.5% is similar to that predicted by one-dimensional models that did not include chlorine nitrate chemistry, and used lower values for the reactions rates of NO + HO2 yielding NO2 + OH and O3 + HO2 yielding OH + 2O2. When the 5.7 ppbv increase in chlorine compounds predicted by one-dimensional models to occur under steady-state conditions is simulated by the two-dimensional model, a 26% decrease in atmospheric ozone is predicted. The latitude dependence of the ozone reduction is discussed in terms of the relevant photochemical reaction and transport. The chemical reactions that most strongly influence the meridional dependence of the ozone depletion are identified as those associated with the reactions of chlorine monoxide and atomic oxygen, the recombination of ozone and atomic oxygen, and the photodissociation of molecular oxygen.

Borucki, W. J.↗
NASA NTRS1999

Chemistry Experiments

The purpose of the chemistry component of the model comparison is to assess to what extent differences in the formulation of chemical processes explain the variance between model results. Observed concentrations of chemical compounds are used to estimate to what degree the various models represent realistic situations. For readability, the materials for the chemistry experiment are reported in three separate sections. This section discussed the data used to evaluate the models in their simulation of the source gases and the Nitrogen compounds (NO(y)) and Chlorine compounds (Cl(y)) species.

Brasseur, Guy↗
NASA NTRS1992

Upper-atmosphere Aerosols: Properties and Natural Cycles

The middle atmosphere is rich in its variety of particulate matter, which ranges from meteorite debris, to sulfate aerosols, to polar stratospheric ice clouds. Volcanic eruptions strongly perturb the stratospheric sulfate (Junge) layer. High-altitude 'noctilucent' ice clouds condense at the summer mesopause. The properties of these particles, including their composition, sizes, and geographical distribution, are discussed, and their global effects, including chemical, radiative, and climatic roles, are reviewed. Polar stratospheric clouds (PSCs) are composed of water and nitric acid in the form of micron-sized ice crystals. These particles catalyze reactions of chlorine compounds that 'activate' otherwise inert chlorine reservoirs, leading to severe ozone depletions in the southern polar stratosphere during austral spring. PSCs also modify the composition of the polar stratosphere through complex physiocochemical processes, including dehydration and denitrification, and the conversion of reactive nitrogen oxides into nitric acid. If water vapor and nitric acid concentrations are enhanced by high-altitude aircraft activity, the frequency, geographical range, and duration of PSCs might increase accordingly, thus enhancing the destruction of the ozone layer (which would be naturally limited in geographical extent by the same factors that confine the ozone hole to high latitudes in winter). The stratospheric sulfate aerosol layer reflects solar radiation and increases the planetary albedo, thereby cooling the surface and possibly altering the climate. Major volcanic eruptions, which increase the sulfate aerosol burden by a factor of 100 or more, may cause significant global climate anomalies. Sulfate aerosols might also be capable of activating stratospheric chlorine reservoirs on a global scale (unlike PCSs, which represent a localized polar winter phenomenon), although existing evidence suggests relatively minor perturbations in chlorine chemistry. Nevertheless, if atmospheric concentrations of chlorine (associated with anthropogenic use of chlorofluorocarbons) continue to increase by a factor of two or more in future decades, aircraft emissions of sulfur dioxide and water vapor may take on greater significance.

Turco, Richard P.↗
NASA NTRS1975

Microwave spectra of some chlorine and fluorine compounds

A computer-controlled microwave spectrometer was used to catalog reference spectra for chemical analysis. Tables of absorption frequencies, peak absorption intensities, and integrated intensities are shown for 21 organic compounds which contain chlorine, fluorine, or both.

White, W. F.↗
NASA NTRS1993

Physical chemistry of the H2SO4/HNO3/H2O system - Implications for polar stratospheric clouds

Polar stratospheric clouds (PSCs) play a key role in stratospheric ozone depletion. Surface-catalyzed reactions on PSC particles generate chlorine compounds that photolyze readily to yield chlorine radicals, which in turn destroy ozone very efficiently. The most prevalent PSCs form at temperatures several degrees above the ice frost point and are believed to consist of HNO3 hydrates; however, their formation mechanism is unclear. Results of laboratory experiments are presented which indicate that the background stratospheric H2SO4/H2O aerosols provide an essential link in this mechanism: These liquid aerosols absorb significant amounts of HNO3 vapor, leading most likely to the crystallization of nitric acid trihydrate (NAT). The frozen particles then grow to form PSCs by condensation of additional amounts of HNO3 and H2O vapor. Furthermore, reaction probability measurements reveal that the chlorine radical precursors are formed readily at polar stratospheric temperatures not just on NAT and ice crystals, but also on liquid H2SO4 solutions and on solid H2SO4 hydrates. These results imply that the chlorine activation efficiency of the aerosol particles increases rapidly as the temperature approaches the ice frost point regardless of the phase or composition of the particles.

Molina, M. J.↗
NASA NTRS1982

The chlorine budget of the troposphere

It has been hypothesized that chlorine compounds in the stratosphere could photodissociate and release atomic chlorine which catalytically destroys ozone. For an accurate assessment of the possibility of stratospheric ozone depletion, it will be necessary to know the chlorine budget of the entire atmosphere, including the troposphere and the stratosphere. Most chlorine species in the atmosphere are emitted at the surface and diffuse upward. Measurements involving chlorine are reviewed and photochemical calculations are discussed. It is found that between 0.1-1.0 ppbv of inorganic chlorine is present at the surface and about 0.02 ppbv (parts per billion by volume) at the tropopause. Most of the inorganic chlorine is believed to be in the form of HCl, and thus natural in origin. For organic chlorine the corresponding numbers are 1.9 ppbv and 1.7 ppbv, respectively. At the surface approximately 32% of the organic chlorine is natural and 68% anthropogenic.

Augustsson, T. R.↗
NASA NTRS1991

Polar stratospheric clouds and ozone depletion

A review is presented of investigations into the correlation between the depletion of ozone and the formation of polar stratospheric clouds (PSCs). Satellite measurements from Nimbus 7 showed that over the years the depletion from austral spring to austral spring has generally worsened. Approximately 70 percent of the ozone above Antarctica, which equals about 3 percent of the earth's ozone, is lost during September and October. Various hypotheses for ozone depletion are discussed including the theory suggesting that chlorine compounds might be responsible for the ozone hole, whereby chlorine enters the atmosphere as a component of chlorofluorocarbons produced by humans. The three types of PSCs, nitric acid trihydrate, slowly cooling water-ice, and rapidly cooling water-ice clouds act as important components of the Antarctic ozone depletion. It is indicated that destruction of the ozone will be more severe each year for the next few decades, leading to a doubling in area of the Antarctic ozone hole.

Toon, Owen B.↗
DOE OSTI2025

Integrated low-temperature PVC and polyolefin upgrading

Polyolefins and their chlorinated derivatives such as polyvinyl chloride (PVC) are among the most prevalent plastics in global production and waste streams. Traditional waste-to-energy methods such as incineration and pyrolysis, as well as most chemical upcycling methods for PVC utilization, require thorough, high-temperature dechlorination to prevent the release of toxic chlorinated compounds. Here, we present here a strategy for upgrading discarded PVC into chlorine-free fuel range hydrocarbons and hydrogen chloride in a single-stage process catalyzed by chloroaluminate ionic liquids. This approach offsets endothermic dechlorination and carbon-carbon bond cleavage with exothermic alkylation and hydrogen transfer by isobutane or isopentane in a low-temperature tandem process. The light isoalkanes are available from refinery processes and partly from recycling of the product stream. This process is suitable for handling real-world mixed and contaminated PVC and polyolefin waste streams.

Zhang, Wei [East China Normal Univ. (ECNU), Shangh↗