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1.
Available data on halogenated molecules in the stratosphere will be reviewed. Presently vertical profiles of CFCl3 and CF2Cl2 in the stratosphere exist to 50 km altitude. Only measurements in the lower stratosphere are reported for the other major halocarbons, CCl4 and CH3Cl. Profiles of the product species ClO, Cl, HCl, and HF exist to about 35 km.Comparison with theoretical profiles from 1-D models shows generally good agreement except for ClO where the earliest measured concentrations exceed the calculated ones considerably. 相似文献
2.
Weekly air samples were collected at Cape Kumakahi (0 km) and at nearby Mauna Loa Observatory (3.4 km) which is above the boundary layer. EC/GC and GC/FID techniques were used to measure CH3I, CHCl3, CO and CH4, which are largely natural in origin, and C2Cl4, CCl4, CH3, CCl3, CCl3F (F-11), CCl2F2 (F-12), CHClF2 (F-22) and C2F3Cl3 (F-113), which are due to anthropogenic activities. It was found that all these gases are significantly (0.05) more abundant in the boundary layer than above it. 相似文献
3.
Interhemispheric transport is a key process affecting the accuracy of source quantification for species such as methane by inverse modelling, and is a source of difference among global three-dimensional chemistry transport models (CTMs). Here we use long-term observations of the atmospheric concentration of long-lived species such as CH3CCl3 and CFCl3 for testing three-dimensional chemistry transport models (CTMs); notably their ability to model the interhemispheric transport, distribution, trend, and variability of trace gases in the troposphere. The very striking contrast between the inhomogeneous source distribution and the nearly homogeneous trend, observed in the global ALE/GAGE experiments for both CH3CCl3 and CFCl3 illustrates an efficient interhemispheric transport of atmospherically long-lived chemical species. Analysis of the modelling data at two tropical stations, Barbados (13°N, 59°W) and Samoa (14°S, 124°W), show the close relationship between inter-hemispheric transport and cross-equator Hadley circulations. We found that cross-equator Hadley circulations play a key role in producing the globally homogeneous observed trends. Chemically, the most rapid interaction between CH3CCl3 and OH occurs in the northern summer troposphere; while the most rapid photolysis of CH3CCl3 and CFCl3, and the chemical reactions between CFCl3 and O(1D), take place in the southern summer stratosphere. Therefore, the cross-equator Hadley circulation plays a key role which regulates the southward flux of chemical species. The regulation by the Hadley circulations hence determines the amount of air to be processed by OH, O(1D), and ultraviolet photolysis, in both hemispheres. In summary, the dynamic regulation of the Hadley circulations, and the chemical processing (which crucially depends on the concentration of OH, O(1D), and on the intensity of solar insolation) of the air contribute to the seasonal variability and homogeneous growth rate of observed CH3CCl3 and CFCl3. 相似文献
4.
R. Krishna Rao Vupputuri 《Pure and Applied Geophysics》1978,117(3):448-485
two-dimensional time dependent model of the stratosphere incorporating the major interactions between radiative-photochemical and dynamical processes is described. The main prognostic equations considered are the thermodynamic equation and the general conservation equation for the minor chemical constituents representing the odd oxygen (O
x
=O+('D)+O3), odd hydrogen (HO
x
=HO+HO2), N2O, odd nitrogen (NO
x
=NO+NO2+HNO3), CF2Cl2, CFCl3 and odd chlorine (Cl
x
=Cl+ClO+HCl). The zonal wind and mean meridional circulations are determined diagnostically by the integration of the thermal wind equation and the stream function equation in the meridional plane espectively. The large scale eddy processes are parameterized in terms of zonal mean quantities using the generalized diffusion formulation on a sloping surface. The radiative heating and cooling and the hotochemical sources and sinks are incorporated in a form which allows for the major interactions among the minor trace constituents, temperature and mean circulation.Two integrations consisting of natural stratosphere and a stratosphere contaminated by the chlorofluoromethanes through lower boundary fluxes are carried out for 23 model years by changing the declination of the sun every day and using 6-hour time step. The model simulations of temperature, mean circulation, ozone, HO
x
, N2O and NO
x
in the meridional plane for the normal stratosphere, show satisfactory agreement with the available observations. Based on the results of second integration it is found that the injection of chlorofluoromethanes in the atmosphere at the estimated current production rates can lead to significant changes in the meridional distribution of ozone, temperature and NO
x
in the middle and upper stratosphere. The results also indicate that the percentage total ozone depletion increases from tropics to high latitudes and from summer to winter high latitudes. Also discussed are the results of additional experiments incorporating the reaction of HO2 with NO and the reactions involving ClNO3. 相似文献
5.
In the densely populated Wuppertal-Düsseldorf area the atmospheric concentrations of CCl2F2 and CCl3F near ground level were measured by ECGC and GC-MS method. Special systems for sampling and calibrating were developed. As mean concentration averages over the time period from December 1976 to May 1977 a value of 650±356 pptv was determined for CCl2F2 (F12) and of 490±279 pptv for CCl3F (F 11). 相似文献
6.
A. Hahne A. Volz D. H. Ehhalt H. Cosatto W. Roether W. Weiss B. Kromer 《Pure and Applied Geophysics》1978,116(2-3):575-582
Depth profiles of the chlorofluoromethanes (CFM), CFCl3 and CF2Cl2, have been obtained together with tritium profiles from water samples collected in the Norwegian Sea between surface and 2800 m depth. CFM analysis was performed by vacuum extraction of the dissolved gases from 500 ml samples of seawater and subsequent gaschromatographic measurement. The CFM concentration decreases with depth to about 10 percent of surface concentration at depths below 2000 m. The same behaviour is found for the tritium content. From a correlation of the CFM and tritium concentration the upper limit of the preindustrial atmospheric CFM levels can be estimated to 5 percent of the present day concentrations. 相似文献
7.
The vertical distribution of the methane concentration in the stratosphere is related to its dissociation by two simultaneous daytime reactions with excited oxygen atoms O(1D) and with OH radicals and depends on the stratospheric eddy diffusion coefficient.Dissociation of CH4 in the lower stratosphere leads to the production of CO molecules while in the upper stratosphere thepphotodissociation of CO2 molecules is an additional process to the CO production.In the upper stratosphere (40±10 km) there is an equilibrium between the formation and destruction processes of carbon monoxide which leads to a minimum of its mixing ratio. There is an increase of the CO mixing ratio in the troposphere and mesosphere compared with that of the stratosphere.The vertical distribution of the CO mixing ratio is closely related to the eddy diffusion coefficient in the whole stratosphere but the absolute values of the hydroxyl radical concentration also determine the values of the CO mixing ratio. 相似文献
8.
With the aid of a one-dimensional steady-state, stratospheric model we have calculated ozone changes coused by atmosphric injections of NOx, N2O and chlorofluoromethanes. Adopting the fast rate constant, for the reaction HO2+NO»OH+NO2 measured by Howard and Evenson, we calculate much smaller perturbations of the ozone layer by NOx and N2O additions than previously estimated, but about two times larger ozone reductions as a result of continued emissions of chlorofluoromethanes, CF2Cl2 and CFCl3.The model results are sensitive to adopted values for the rate coefficients for the reactions HO2+O3»OH+2O2 and OH+HO2»H2O+O2 and the eddy diffusion profile near the tropopause. More accurate assessments of ozone perturbations require the development of photochemical models that incorporate meteorological processes in more than one dimension. 相似文献
9.
Stratospheric profiles of CH4 and H2 over eastern Texas have been derived up to 31 km altitude from air samples collected aboard a balloon and analyzed by gas chromatography. For H2, contamination during flight and measurement presented a problem which has been resolved only recently. The earlier profiles require corrections which are rather large for the highest altitudes.The three profiles indicate an increase of the H2 concentration in the lower stratosphere from about 0.5 p.p.m. per volume at the tropopause to about 0.8 p.p.m. at around 27 km altitude. Above that altitude the H2 concentration decreases again. An air sample collected between 44 and 62 km by a rocket-borne cryogenic sampler had an H2 concentration of 0.4 p.p.m.The five CH4 profiles showed a decrease in CH4 concentration with altitude generally with a steeper gradient directly above the tropopause and a weaker gradient at higher altitudes reaching 0.9 p.p.m. at 30 km altitude. The CH4 concentration in the rocket sample was 0.25 p.p.m., in good agreement with the gradient obtained from the balloon samples.The National Center for Atmospheric Research is sponsored by the National Science Foundation. 相似文献
10.
Real-time N2O measurements have been madein situ at the South Pole, Antarctica, north and south of the equator from on board the Alpha Helix and over the Pacific Ocean on several aircraft flights from the U.S. to New Zealand, Australia and 90°S. In addition, an automated EC-GC has been operated for the past year intermittently monitoring N2O in surface air at a rural site in the wheatlands of eastern Washington state. The data obtained are consistent and in agreement with the data obtained from the analyses of a large number of samples collected both from ground stations and a variety of aircraft flights made in the southern and northern hemisphere. The observed global data show no interhemispheric differences. The present concentration of N2O in the troposphere is measured to be 330±3 ppbv. Its vertical distribution in the troposphere is very uniform. A small decrease (2–3 percent) across the tropopause is characteristically observed in the high altitude Learjet flights. 相似文献
11.
The consumption of both methane and carbon monoxide in the lower stratosphere is due predominantly to reaction with OH radicals. The possibility of deriving OH concentration from measurements of the decrease of CH4 and CO mixing ratios above the tropopause is explored. The observations and the basic chemistry are briefly summarized. Simple one-dimensional diffusion models are employed to derive expressions for the decrease of CH4 and CO mixing ratios with altitude above the tropopause, and the influence of important parameters is discussed. Vertical air velocities resulting from large-scale organized mean motion and from synoptic variations are shown to distort the concentration altitude profiles of methane and carbon monoxide, respectively. Suitable averaging of observational data is required to eliminate the effects due to vertical motion. Then a reliable value for the effective OH number density should be obtainable. At present an estimate of 4×106 molecules/cm3 is derived. 相似文献
12.
110 samples from two swimming-pools were gas-chromatographically investigated for halogenated hydrocarbons. In spite of varying chlorine concentrations between 0.1 and 2.5 mg/l Cl2 the bacteriological results were unobjectionable. The total of the haloforms was between 1.2 and 182 μg/l, with the average value of 90 μg/l. Besides CHCl3, CHBrCl2, CHBr2Cl and CCl3NO2 there were observed other, still unidentified compounds in the chlorinated bathing water which clearly are successive products of disinfection, too. The water treatment by flocculation and filtration does not bring about any elimination of trihalomethanes. Of special importance is the occurrence of trichloronitromethane in concentrations of 0.13 … 1.2 μg/l, whose LC50 in the Daphnia test is 189 μg/l, at a threshold concentration of 160 μg/l. To limit the pollution of water and air to a minimum, specific conditions must be adhered to in the operation of indoor swimming-pools. 相似文献
13.
Innovative Environmental Tracer Techniques for Evaluating Sources of Spring Discharge from a Carbonate Aquifer Bisected by a River 总被引：2，自引：0，他引：2
Littlefield Springs discharge about 1.6 m3/s along a 10‐km reach of the Virgin River in northwestern Arizona. Understanding their source is important for salinity control in the Colorado River Basin. Environmental tracers suggest that Littlefield Springs are a mixture of older groundwater from the regional Great Basin carbonate aquifer and modern (post‐1950s) seepage from the Virgin River. While corrected 14C apparent ages range from 1 to 9 ka, large amounts of nucleogenic 4He and low 3He/4He ratios suggest that the carbonate aquifer component is likely even older Pleistocene recharge. Modeled infiltration of precipitation, hydrogeologic cross sections, and hydraulic gradients all indicate recharge to the carbonate aquifer likely occurs in the Clover and Bull Valley Mountains along the northern part of the watershed, rather than in the nearby Virgin Mountains. This high‐altitude recharge is supported by relatively cool noble‐gas recharge temperatures and isotopically depleted δ2H and δ18O. Excess (crustal) SF6 and 4He precluded dating of the modern component of water from Littlefield Springs using SF6 and 3H/3He methods. Assuming a lumped‐parameter model with a binary mixture of two piston‐flow components, Cl?/Br?, Cl?/F?, δ2H, and CFCs indicate the mixture is about 60% Virgin River water and 40% groundwater from the carbonate aquifer, with an approximately 30‐year groundwater travel time for Virgin River seepage to re‐emerge at Littlefield Springs. This suggests that removal of high‐salinity sources upstream of the Virgin River Gorge would reduce the salinity of water discharging from Littlefield Springs into the Virgin River within a few decades. 相似文献
14.
The groundwater of the Korba plain represents major water resources in Tunisia. The Plio‐Quaternary unconfined aquifer of the Cap‐Bon (north‐east Tunisia) is subject to the intensive agricultural activities and high groundwater pumping rates due to the increasing of the groundwater extraction. The degradation of the groundwater quality is characterized by the salinization phenomena. Groundwater were sampled and analysed for physic‐chemical parameters: Ca2+, Mg2+, Na+, K+, Cl‐, SO42‐, HCO3‐, NO3‐, pH, electrical conductivity (EC), and the temperature (T°). The hydrochemical analysis is coupled with the calculation of the saturation indexes (SI gypsum, SI halite, SI calcite and SI dolomite), ionic derivation and with the ion correlations compared to chloride concentrations: Na+/ Cl‐, Ca2+/ Cl‐ and Mg2+/ Cl‐ ratios. Seawater fractions in the groundwater were calculated using the chloride concentration. Those processes can be used as indicators of seawater intrusion progression. EC methods were also conducted to obtain new informations on the spatial scales and dynamics of the fresh water–seawater interface of coastal groundwater exchange. The mixing zone between freshwater and saltwater was clearly observed from the EC profile in the investigated area where a strong increase in EC with depth was observed, corresponding to the freshwater and saltwater interface. Results of hydrochemical study revealed the presence of direct cation exchange linked to seawater intrusion and dissolution processes associated with cations exchange. These results, together with EC investigation, indicated that the groundwater is affected by seawater intrusion and is still major actor as a source of salinization of the groundwater in Korba coastal plain. Further isotopic and hydrological investigations will be necessary to identify and more understood the underlying mechanisms. Copyright © 2012 John Wiley & Sons, Ltd. 相似文献
15.
The acidic discharge from Cement Creek, containing elevated concentrations of dissolved metals and sulphate, mixed with the circumneutral‐pH Animas River over a several hundred metre reach (mixing zone) near Silverton, CO, during this study. Differences in concentrations of Ca, Mg, Si, Sr, and SO42? between the creek and the river were sufficiently large for these analytes to be used as natural tracers in the mixing zone. In addition, a sodium chloride (NaCl) tracer was injected into Cement Creek, which provided a Cl? ‘reference’ tracer in the mixing zone. Conservative transport of the dissolved metals and sulphate through the mixing zone was verified by mass balances and by linear mixing plots relative to the injected reference tracer. At each of seven sites in the mixing zone, five samples were collected at evenly spaced increments of the observed across‐channel gradients, as determined by specific conductance. This created sets of samples that adequately covered the ranges of mixtures (mixing ratios, in terms of the fraction of Animas River water, %AR). Concentratis measured in each mixing zone sample and in the upstream Animas River and Cement Creek were used to compute %AR for the reference and natural tracers. Values of %AR from natural tracers generally showed good agreement with values from the reference tracer, but variability in discharge and end‐member concentrations and analytical errors contributed to unexpected outlier values for both injected and natural tracers. The median value (MV) %AR (calculated from all of the tracers) reduced scatter in the mixing plots for the dissolved metals, indicating that the MV estimate reduced the effects of various potential errors that could affect any tracer. Copyright © 2006 John Wiley & Sons, Ltd. 相似文献
16.
Materials of expedition studies in 2013 in the Prielbrus’e National Park were used to analyze the concentrations of a wide range of pollutants (SO42-, Cl?, Na+, K+, F?, Mn, Cu, Zn, Pb, Cr, Ni, NO3-, NH4+) in the water of mountain rivers forming the main artery of the region, the Baksan R. The analyzed data characterize seasonal variations in pollutant concentrations at seven sampling sections and their dynamics along the river down to the 35th km from the source in different seasons. 相似文献
17.
Sarah K. Fortner W. Berry Lyons Andrew G. Fountain Kathleen A. Welch Natalie M. Kehrwald 《水文研究》2009,23(21):2987-2996
We present concentrations of environmentally available (unfiltered acidified 2% v/v HNO3) As, Cu, Cd, Pb, V, Sr, and major ions including Ca2+, Cl?, and SO42? in a July 2005 and a March 2006 shallow snow profile from the lower Eliot Glacier, Mount Hood, Oregon, and its proglacial stream, Eliot Creek. Low enrichment factors (EF) with respect to crustal averages suggests that in fresh March 2006 snow environmentally available elements are derived primarily from lithogenic sources. Soluble salts occurred in lower and less variable concentrations in July 2005 snow than March 2006. Conversely, environmentally available trace elements occurred in greater and more variable concentrations in July 2005 than March 2006 snow. Unlike major solutes, particulate‐associated trace elements are not readily eluted during the melt season. Additionally, elevated surface concentrations suggest that they are likely added throughout the year via dry deposition. In a 1‐h stream sampling, ratios of dissolved (<0·45 µm) V:Cl?, Sr:Cl?, and Cu:Cl? are enriched in the Eliot Stream with respect to their environmentally available trace element to Cl? ratios in Eliot Glacier snow, suggesting chemical weathering additions in the stream waters. Dissolved Pb:Cl? is depleted in the Eliot Stream with respect to the ratio of environmentally available Pb to Cl? in snow, corresponding to greater adsorption onto particles at greater pH values. Copyright © 2009 John Wiley & Sons, Ltd. 相似文献
18.
An airborne downward-pointing water vapor lidar provides two-dimensional, simultaneous curtains of atmospheric backscatter and humidity along the flight track with high accuracy and spatial resolution. In order to improve the knowledge on the coupling between clouds, circulation and climate in the trade wind region, the DLR (Deutsches Zentrum für Luft- und Raumfahrt) water vapor lidar was operated on board the German research aircraft HALO during the NARVAL (Next Generation Aircraft Remote Sensing for Validation Studies) field experiment in December 2013. Out of the wealth of about 30 flight hours or 25,000 km of data over the Tropical Atlantic Ocean east of Barbados, three ~ 2-h-long, representative segments from different flights were selected. Analyses of Meteosat Second Generation images and dropsondes complement this case study. All observations indicate a high heterogeneity of the humidity in the lowest 4 km of the tropical troposphere, as well as of the depth of the cloud (1–2 km thick) and sub-cloud layer (~ 1 km thick). At the winter trade inversion with its strong humidity jump of up to 9 g/kg in water vapor mixing ratio, the mixing ratio variance can attain 9 (g/kg)2, while below it typically ranges between 1 and 3 (g/kg)2. Layer depths and partial water vapor columns within the layers vary by up to a factor of 2. This affects the total tropospheric water vapor column, amounting on average to 28 kg/m2, by up to 10 kg/m2 or 36%. The dominant scale of the variability is given by the extent of regions with higher-than-average humidity and lies between 300 and 600 km. The variability mainly stems from the alternation between dry regions and moisture lifted by convection. Occasionally, up to 100-km large dry regions are observed. In between, convection pushes the trade inversion upward, sharpening the vertical moisture gradient that is colocated with the trade inversion. In most of the water vapor profiles, this gradient is stronger than the one located at the top of the sub-cloud layer. Lidar observations in concert with models accurately reproducing the observed variability are expected to help evaluate the role these findings play for climate. 相似文献
19.
S. C. Scott 《Bulletin of Volcanology》1983,46(4):393-412
The March 1981 eruption of Mount Etna occurred on the northern slopes of the volcano in an area previously inactive for more
than 400 a. A radial fissure system extending 7.5 km and producing 20±2×106 m3 of basic hawaiite lava, opened at 2600 m a.s.l. on 17th March and migrated downslope to 1125 m a.s.l. where activity ceased
on 23rd March. Gravity evidence points to the draining of a radial storage-dyke, located between sea-level and +1 km a.s.l.
Whole-rock chemistry and petrography suggests that the magma in the dyke was a hybrid supporting crystal and compositional
gradients developed as a result of progressively greater mixing of residual 1979 basic hawaiite magma with fresh basic hawaiite
magma during permissive filling of the dyke around September 1980. These mixing gradients caused the eruption to display a
significant contrast in the concentrations of Al2O3, Sr, CaO, MgO and Fe2O3 (total) between early, high-altitude and later, low-altitude products. The fresh magma which entered the high-level system
around September 1980 ascended rapidly from a deep storage region at 16–24 km depth.
On a FMA plot, the composition range of the 1981 lava lies at the end of a temporal variation trend defined by the composition
of successive flank eruptions back to 1971 and appears to be repeated by successive eruptions between 1923 and 1949. This
suggest that the chemistry of historic lavas may, in a general way, reflect the evolution path of magma in the deep storage
region despite masking of detail by high-level processes such as mixing. These temporal trends may, if real, reflect successive
batches of freshly generated magma from the mantle source region entering into and subsequently differentiating within the
deep storage region.
Paper presented to the Symp. on Formation and Evolution of Magma Chambers: Physical and Chemical Processes, 18th IUGGIAVCEI
Gen. Assembly, Hamburg, F.R.G., August 1983. 相似文献
20.
A. N. Gruzdev 《Geomagnetism and Aeronomy》2014,54(5):633-639
Using spectral, cross-spectral, and regression methods, we analyzed the effect of the 11-year cycle of solar activity on the ozone content in the stratosphere and lower mesosphere via satellite measurement data obtained with the help of SBUV/SBUV2 instruments in 1978–2003. We revealed a high coherence between the ozone content and solar activity level on the solar cycle scale. In much of this area, the ozone content varies approximately in phase with the solar cycle; however, in areas of significant gradients of ozone mixing ratio in the middle stratosphere, the phase shift between ozone and solar oscillations can be considerable, up to π/2. This can be caused by dynamical processes. The altitude maxima of ozone sensitivity to the 11-year solar cycle were found in the upper vicinity of the stratopause (50–55 km), in the middle stratosphere (35–40 km), and the lower stratosphere (below 25 km). Maximal changes in ozone content in the solar cycle (up to 10% and more) were found in winter and spring in polar regions. 相似文献