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Rate constants of two elementary bimolecular reactions involved in the oxidation of methane were determined by monitoring the exponential growth of CO flame band emission behind incident shocks in three suitably chosen gas mixtures.
Rate constants of two elementary bimolecular reactions involved in the oxidation of methane have been determined by monitoring the exponential growth of CO flame band emission behind incident shocks in three suitably chosen gas mixtures. The data do not support a mechanism which invokes the four center process CH3 + O2 yields CH2O + OH for the reaction of methyl with oxygen.
Growth constants, obtained by measuring the blue CO flame band emission behind incident shock waves, were obtained for two elementary bimolecular reactions involved in the oxidation of methane. Gas mixtures containing small amounts of CH4 with varying amounts of CO, O2, and in one case CO2, diluted with argon, were investigated, and exponential growth constants were derived from plots of the logarithm of observed light intensity versus gas time. The rate constant for the reaction O + CH4 yields CH3 + OH was found to be 1.9 times 10 to the 14th exp(-5900/T) cu cm per mole per sec in the range 1300-2000 K; for the reaction CH3 + O2 yields CH3O + O, the rate constant was determined to be 2.4 times 10 to the 13th exp(-14,500/T) cu cm per mole per sec in the range 1200 to 1900 K.
Data are presented from the 1977 Intertropical Convergence Zone (ITCZ) Experiment conducted in the Panama Canal Zone in July 1977. Measurements were made daily over a 16-day period when the ITCZ moved across the Canal Zone. Two aircraft (Learjet and U-2) flew daily and provided data from horizontal traverses at several altitudes to 21.3 km of ozone, temperature, pressure, water vapor, aerosols, fluorocarbons, methane, nitrous oxide, nitric oxide, and nitric acid. Balloonsondes flown four times per day provided data on ozone, wind fields, pressure, temperature, and humidities to altitudes near 30 km. Rocketsondes provided daily data to altitudes near 69 km. Satellite photography provided detailed cloud information. Descriptions of individual experiments and detailed compilations of all results are provided.
The carbon monoxide cycle is studied by incorporating the known and hypothetical sources and sinks in a tracer model that uses the winds generated by a general circulation model. Photochemical production and loss terms, which depend on OH radical concentrations, are calculated in an interactive fashion. The computed global distribution and seasonal variations of CO are compared with observations to obtain constraints on the distribution and magnitude of the sources and sinks of CO, and on the tropospheric abundance of OH. The simplest model that accounts for available observations requires a low latitude plant source of about 1.3 x 10 to the 15th g/yr, in addition to sources from incomplete combustion of fossil fuels and oxidation of methane. The globally averaged OH concentration calculated in the model is 750,000/cu cm. Models that calculate globally averaged OH concentrations much lower than this nominal value are not consistent with the observed variability of CO. Such models are also inconsistent with measurements of CO isotopic abundances, which imply the existence of plant sources.
A high resolution spectral radiative transfer model of the troposphere for computing downwelling radiance and flux density at the surface in the 5-200 micron region has been developed. The model is fast and accurate and takes into consideration all major and minor constituents active in this region, namely, water vapor, carbon dioxide, ozone, nitrous oxide, and methane. It uses the quasi-random band model of absorption for computing atmospheric transmittances due to various bands. Continuum absorption by water vapor in the 8-14 micron region has also been taken into account. The model has been used to examine the sensitivity of downwelling flux to variations of surface water vapor pressure (or surface relative humidity), water vapor scale-height and concentrations of other gaseous constituents of the atmosphere. In addition, sensitivity to changes in a number of cloud parameters, namely, fractional cloud cover, cloud height, and high-cloud emissivity, has also been examined. Results obtained with the present model compare well with those from the empirical and semi-empirical correlations. The present work demonstrates, for the first time, the feasibility of using a high-resolution narrow-band model for computing this flux for a meteorological application.
An interpretation of global ozone changes deduced from satellite data obtained since 1979 is presented, based on two-dimensional model simulations. The study shows that a depletion in total ozone of the order of 2 percent and a reduction in ozone density near 40 km of 7 to 12 percent over the 1979-1986 period are consistent with the observed increase in trace gas densities (chlorofluorocarbons, methane, nitrous oxide, carbon dioxide) and the simultaneous decrease in solar activity during this period. The model also suggests that ozone variations of solar and anthropogenic origins between 1979 and 1986 were of similar magnitude but that the ozone response to trace gas emissions increases substantially with latitude while the solar signal in ozone is present lower in the atmosphere and is nearly independent of latitude.
A low temperature electrolysis process has been developed for the treatment of solid waste material and urine. Experiments are described in which organic materials are oxidized directly at the surface of an electrode. Also, hypochlorite is generated electrochemically from chloride component of urine. Hypochlorite can act as a strong oxidizing agent in solution. The oxidation takes place at 30-60 C and the gaseous products from the anodic reaction are carbon dioxide, nitrogen, oxygen. Hydrogen is formed at the cathode. Carbon monoxide, and nitrogen oxides and methane were not detected in the off gases. Chlorine was evolved at the anode in relatively low amounts.
A new two-dimensional model of the stratosphere and the mesosphere was formulated in transformed Eulerian coordinates, in which dynamics, radiation, and chemistry are treated interactively. The model includes a detailed radiative scheme which derives the diabatic heating rates consistently with calculated distributions of temperature and trace species densities. Results are presented on the present-day and perturbed atmosphere, showing that the calculated distributions of source gases, such as nitrous oxide and methane, are very sensitive to the calculated (and parameterized) dynamical quantities, and that species produced in the atmosphere, like carbon monoxide and odd nitrogen, can provide valuable information on the role of atmospheric transport.
The conference on The Climate Impact of Solar Variability, was held at Goddard Space Flight Center from April 24 to 27, 1990. In recent years they developed a renewed interest in the potential effects of increasing greenhouse gases on climate. Carbon dioxide, methane, nitrous oxide, and the chlorofluorocarbons have been increasing at rates that could significantly change climate. There is considerable uncertainty over the magnitude of this anthropogenic change. The climate system is very complex, with feedback processes that are not fully understood. Moreover, there are two sources of natural climate variability (volcanic aerosols and solar variability) added to the anthropogenic changes which may confuse our interpretation of the observed temperature record. Thus, if we could understand the climatic impact of the natural variability, it would aid our interpretation and understanding of man-made climate changes.
An inductively coupled plasma discharge apparatus operating at 13.56 MHz and with electrical power up to 2.5 kW was constructed. The efficiency of this device to destroy various gases expected to be carried aboard the Space Station was tested. By expressing the efficiency of the device in terms of G-value (the number of molecules decomposed per 100 eV of energy absorbed), the results are compared with known efficiencies of ionizing radiation to destroy these same gases. In the case of ammonia, it was found that in the inductively coupled device, the destruction efficiency, G(-NH3) varied from 6.0 to 32.0 molecules/100 eV, depending on conditions. It was also found that capacitatively coupled discharges were less efficient in destroying NH2 than the inductively coupled discharge. In the case NH2 destruction, it was found that the G(-NH3) was a qualitative guide to the efficiencies of plasmas. The plasma device was also used to destroy nitrous oxide and methane. It is shown how the G-value for the destruction of any gas can be computed theoretically from a knowledge of the electron velocity distribution, the various electron molecule scattering cross sections, and the rate constants for the reactions of secondary species.
This study presents various approaches to parameterizing the broadband transmission functions for utilization in numerical climate models. One-parameter scaling is applied to approximate a nonhomogeneous path with an equivalent homogeneous path, and the diffuse transmittances are either interpolated from precomputed tables or fit by analytical functions. Two-parameter scaling is applied to parameterizing the carbon dioxide and ozone transmission functions in both the lower and middle atmosphere. Parameterizations are given for the nitrous oxide and methane diffuse transmission functions.
We have constructed a regional budget for boundary layer carbon monoxide over the central United States (32.5 deg - 50 deg N, 90 deg - 105 deg W), emphasizing a detailed evaluation of deep convective vertical fluxes appropriate for the month of June. Deep convective venting of the boundary layer (upward) dominates other components of the CO budget, e.g., downward convective transport, loss of CO by oxidation, anthropogenic emissions, and CO produced from oxidation of methane, isoprene, and anthropogenic nonmethane hydrocarbons (NMHCs). Calculations of deep convective venting are based on the method pf Pickering et al.(1992a) which uses a satellite-derived deep convective cloud climatology along with transport statistics from convective cloud model simulations of observed prototype squall line events. This study uses analyses of convective episodes in 1985 and 1989 and CO measurements taken during several midwestern field campaigns. Deep convective venting of the boundary layer over this moderately polluted region provides a net (upward minus downward) flux of 18.1 x 10(exp 8) kg CO/month to the free troposphere during early summer. Shallow cumulus and synoptic-scale weather systems together make a comparable contribution (total net flux 16.2 x 10(exp 8) kg CO/month). Boundary layer venting of CO with other O3 precursors leads to efficient free troposheric O3 formation. We estimate that deep convective transport of CO and other precursors over the central United States in early summer leads to a gross production of 0.66 - 1.1 Gmol O3/d in good agreement with estimates of O3 production from boundary layer venting in a continental-scale model (Jacob et al., 1993a, b). On this respect the central U.S. region acts as s `chimney' for the country, and presumably this O3 contributes to high background levels of O3 in the eastern United States and O3 export to the North Atlantic.
Total reactive nitrogen (NO(y)), nitrous oxide (NO2), methane (CH4), and ozone (03) were measured on board a balloon launched from Aire sur l'Adour (44 deg N, 0 deg W), France on October 12, 1994. Generally, NO(y) was highly anti-correlated with N2O and CH4 at altitudes between 15 and 32 km. The linear NO(y) - N2O and NO(y) - CH4 relationships obtained by the present observations are very similar to those obtained on board ER-2 and DC-8 aircraft previously at altitude below 20 km in the northern hemisphere. They also agree well with the data obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument at 41 deg N in November 1994. Slight departures from linear correlations occurred around 29 km, where N2O and CH4 mixing ratios were larger than typical midlatitude values, suggesting horizontal transport of tropical airmasses to northern midlatitudes in a confined altitude region.
An overview of Airborne Arctic Stratospheric Expedition 2 is given. Effects of Pinatubo aerosol on stratospheric ozone at mid-latitudes, in situ measurements of ClO and ClO/HCl ratio, balloon-borne measurements of ClO, NO, and O3 in a volcanic cloud, and new observations of the NO(y)/N2O correlation in the lower stratosphere are discussed. Among other topics addressed are the following: in situ tracer correlations of methane, nitrous oxide, and ozone as observed aboard the DC-8, in situ measurements of changes in stratospheric aerosol and the N2O-aerosol relationship inside and outside of the polar vortex, measurements of halogenated organic compounds near the tropical tropopause, and airborne brightness measurements of the polar winter troposphere.
This is a theoretical research project aimed at: (1) development, testing, and refining of inverse methods for determining regional and global transient source and sink strengths for long lived gases important in ozone depletion and climate forcing, (2) utilization of inverse methods to determine these source/sink strengths which use the NCAR/Boulder CCM2-T42 3-D model and a global 3-D Model for Atmospheric Transport and Chemistry (MATCH) which is based on analyzed observed wind fields (developed in collaboration by MIT and NCAR/Boulder), (3) determination of global (and perhaps regional) average hydroxyl radical concentrations using inverse methods with multiple titrating gases, and, (4) computation of the lifetimes and spatially resolved destruction rates of trace gases using 3-D models. Important goals include determination of regional source strengths of methane, nitrous oxide, and other climatically and chemically important biogenic trace gases and also of halocarbons restricted by the Montreal Protocol and its follow-on agreements and hydrohalocarbons used as alternatives to the restricted halocarbons.
At the time this proposal was submitted, recent publications had suggested an important role for transport of midlatitude air into the tropical lower stratosphere. Most of these studies had employed data that gave only a time-averaged picture, making it difficult to determine the nature of the transport processes responsible for the observed behavior. We proposed to analyze observations of long-lived trace gases, such as nitric acid, methane, nitrous oxide, and chlorofluorocarbons, made from the Upper Atmosphere Research Satellite, to investigate the seasonal behavior of mixing between the midlatitudes and tropics. We planned to construct probability distributions of the concentrations of these species over small altitude ranges and to compare them to expectations based on modeled mean concentrations and knowledge of instrument precision. Differences from expectation were to be analyzed with respect to meteorological parameters to determine whether wave activity may have induced apparent mixing.
We report progress in the first year, and summarize proposed work for the second year of the three-year dynamical-chemical modeling project devoted to: (a) development, testing, and refining of inverse methods for determining regional and global transient source and sink strengths for long lived gases important in ozone depletion and climate forcing, (b) utilization of inverse methods to determine these source/sink strengths using either MATCH (Model for Atmospheric Transport and Chemistry) which is based on analyzed observed wind fields or back-trajectories computed from these wind fields, (c) determination of global (and perhaps regional) average hydroxyl radical concentrations using inverse methods with multiple titrating gases, and (d) computation of the lifetimes and spatially resolved destruction rates of trace gases using 3D models. Important goals include determination of regional source strengths of methane, nitrous oxide, methyl bromide, and other climatically and chemically important biogenic/anthropogenic trace gases and also of halocarbons restricted by the Montreal protocol and its follow-on agreements and hydrohalocarbons now used as alternatives to the restricted halocarbons.