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1.
The set of high-resolution infrared solar observations made with the Atmospheric Trace Molecule Spectroscopy (ATMOS)-Fourier transform spectrometer from onboard Spacelab 3 (30 April-1 May 1985) has been used to evaluate the total budgets of the odd chlorine and fluorine chemical families in the stratosphere. These budgets are based on volume mixing ratio profiles measured for HCl, HF, CH3Cl, ClONO2, CCl4, CCl2F2, CCl3F, CHClF2, CF4, COF2, and SF6 near 30° north latitude. When including realistic concentrations for species not measured by ATMOS, i.e., the source gases CH3CCl3 and C2F3Cl3 below 25 km, and the reservoirs ClO, HOCl and COFCl between 15 and 40 km (five gases actually measured by other techniques), the 30° N zonal 1985 mean total mixing ratio of chlorine, Cl, was found to be equal to (2.58±0.10) ppbv (parts per billion by volume) throughout the stratosphere, with no significant decrease near the stratopause. The results for total fluorine indicate a slight, but steady, decrease of its volume mixing ratio with increasing altitude, around a mean stratospheric value of (1.15±0.12) ppbv. Both uncertainties correspond to one standard deviation. These mean springtime 1985 stratospheric budgets are commensurate with values reported for the tropospheric Cl and F concentrations in the early 1980s, when allowance is made for the growth rates of their source gases at the ground and the time required for tropospheric air to be transported into the stratosphere. The results are discussed with emphasis on conservation of fluorine and chlorine and the partitioning among source, sink, and reservoir gases throughout the stratosphere.  相似文献   

2.
The concentrations of H+, nitrate (NO3 -), and sulfate (SO4 2-) in rainwater and their temporal changes were analyzed on the basis of continuous observation from 1 July 1991 to 30 June 1992 at a suburb of Nagoya, Japan. The yearly average for pH was 4.4. In general, an increasing pH with increase in precipitation amount was observed for rain events. Relatively high pH rainwater was sometimes observed at the beginning of rainfall, even though high concentrations of NO3 - and SO4 2- were involved. The high pH values were considered to be caused by the neutralization process with particulate matter containing cations. The yearly averaged ratio of equivalent concentration of nitrate to sulfate (N/S) in rainwater was 0.58. In the early stage of rain, the N/S value was usually more than 1.0 due to the difference of scavenging process between NO3 - and SO4 2-. High values of N/S ranging from 5 to 10 were found under the atmospheric conditions of calm winds and low humidity, during which it is possible that atmospheric particles float for a long time in the air before a rain event. The adsorption of NO3 - in the early stage of rainfall by particulate matter was suggested from the difference in scavenging processes of NO3 - and SO4 2-. A possible scavenging process, called limb cloud scavenging, is presented to explain the interaction of particles and nitrate ions at the early stage of rain. In limb cloud scavenging, the repeated migration of cloud particles or raindrops between the inside and outside of clouds increases the absorption of ions to a highly condensed level, thus increasing the N/S value of rainwater. The influence of global scale seasonal phenomena with large amounts of particulates, such as typhoons or Asian dust storms, was also studied.  相似文献   

3.
Modelling studies were performed with the multiphase mechanism RACM-MIM2ext/CAPRAM 3.0i to investigate the tropospheric multiphase chemistry in deliquesced particles and non-precipitating clouds using the SPACCIM model framework. Simulations using a non-permanent cloud scenario were carried out for two different environmental conditions focusing on the multiphase chemistry of oxidants and other linked chemical subsystems. Model results were analysed by time-resolved reaction flux analyses allowing advanced interpretations. The model shows significant effects of multiphase chemical interactions on the tropospheric budget of gas-phase oxidants and organic compounds. In-cloud gas-phase OH radical concentration reductions of about 90 % and 75 % were modelled for urban and remote conditions, respectively. The reduced in-cloud gas-phase oxidation budget increases the tropospheric residence time of organic trace gases by up to about 30 %. Aqueous-phase oxidations of methylglyoxal and 1,4-butenedial were identified as important OH radical sinks under polluted conditions. The model revealed that the organic C3 and C4 chemistry contributes with about 38 %/48 % and 8 %/9 % considerably to the urban and remote cloud / aqueous particle OH sinks. Furthermore, the simulations clearly implicate the potential role of deliquescent particles to operate as a reactive chemical medium due to an efficient TMI/HOx,y chemical processing including e.g. an effective in-situ formation of OH radicals. Considerable chemical differences between deliquescent particles and cloud droplets, e.g. a circa 2 times more efficient daytime iron processing in the urban deliquescent particles, were identified. The in-cloud oxidation of methylglyoxal and its oxidation products is identified as efficient sink for NO3 radicals in the aqueous phase.  相似文献   

4.
A unified chemistry-aerosol-climate model is applied in this work to compare climate responses to chang- ing concentrations of long-lived greenhouse gases(GHGs,CO2,CH4,N2O),tropospheric O3,and aerosols during the years 1951–2000.Concentrations of sulfate,nitrate,primary organic carbon(POA),secondary organic carbon(SOA),black carbon(BC)aerosols,and tropospheric O3 for the years 1950 and 2000 are obtained a priori by coupled chemistry-aerosol-GCM simulations,and then monthly concentrations are in- terpolated ...  相似文献   

5.
Atmospheric nitric acid measurements by ACIMS (Active Chemical Ionization Mass Spectrometry) are based on ion-molecule reactions of CO3 -(H2O) n and NO3 -(H2O) n with HNO3. We have studied these reactions in the laboratory using a flow tube apparatus with mass spectrometric detection of reactant and product ions. Both product ion distributions and rate coefficients were measured. All reactions were investigated in an N2-buffer (1–3 hPa) at room temperature. The reaction rate coefficients of OH-, O2 -, O3 -, CO4 -, CO3 -, CO3 -H2O, NO3 -, and NO3 -H2O were measured relative to the known rate k=3.0×10-9 cm3 s-1 for the reaction of O- with HNO3. The main product ion of the reaction of CO3 -H2O with HNO3 was found to be (CO3HNO3)- supporting a previous suggestion made on the basis of balloon-borne ACIMS measurements. For the reaction of bare CO3 - with HNO3 three product ions were observed, namely NO3 -, (NO3OH)-, and (CO3HNO3)-. The reaction rate coefficients for CO3 -H2O (1.7×10-9 cm3 s-1) and NO3 -H2O (1.6×10-9 cm3 s-1) were found to be close to the collision rate. The measured k values for bare CO3 - (1.3×10-9 cm3 s-1) and NO3 - (0.7×10-9 cm3 s-1) are somewhat smaller. The collisional dissociations of CO3 -(H2O) n , NO3 -(H2O) n (n=1, 2), (CO3HNO3)- and (NO3HNO3)-, occasionally influencing ACIMS measurements, were also studied. Fragment ion distributions were measured using a triple quadrupole mass spectrometer. The results showed that previous stratospheric nitric acid measurements were unimpaired from collisional dissociation processes whereas these processes played a major role during previous tropospheric measurements leading to an underestimation of nitric acid concentrations. Previous ACIMS HNO3 detection was also affected by the conversion of CO3 -(H2O) n to NO3 -(H2O) n due to ion source-produced neutral radicals. A novel ACIMS ion source was developed in order to avoid these problems and to improve the ACIMS method.  相似文献   

6.
A photochemical box model is used to simulate seasonal variations in concentrations of sulfur compounds at latitude 40° S. It is assumed that the hydroxyl radical (OH) addition reaction to sulfur in the dimethyl sulfide (DMS) molecule is the predominant pathway for methanesulfonic acid (MSA) production, and that the rate constant increases as the air temperature decreases. Concentration of the nitrate radical (NO3) is a function of the DMS flux, because the reaction of DMS with NO3 is the most important loss mechanism of NO3. While the diurnally averaged concentration of OH in winter is a factor of about 8 smaller than in summer, due to the weak photolysis process, the diurnally averaged concentration of NO3 in winter is a factor of about 4–5 larger than in summer, due to the decrease of DMS flux. Therefore, at middle and high latitudes in winter, atmospheric DMS is mainly oxidized by the reaction with NO3. The calculated ratio of the MSA to SO2 production rates is smaller in winter than in summer, and the MSA to non-sea-salt sulfate (nssSO4 2-) molar ratio varies seasonally. This result agrees with data on the seasonal variation of the MSA/nssSO4 2- molar ratio obtained at middle and high latitudes. The calculations indicate that during winter the reaction of DMS with NO3 is likely to be a more important sink of NOx (NO+NO2) than the reaction of NO2 with OH, and to serve as a significant pathway of the HNO3 production. If dimethyl sulfoxide (DMSO) is produced through the OH addition reaction and is heterogeneously oxidized in aqueous solutions, half of the nssSO4 2- produced in summer may be through the oxidation process of DMSO. It is necessary to further investigate the oxidation products by the reaction of DMS with OH, and the possibility of the reaction of DMS with NO3 during winter.  相似文献   

7.
In part two of this series of papers on the IMS model, we present the chemistry reaction mechanism usedand compare modelled CH4, CO, and O3 witha dataset of annual surface measurements. The modelled monthly and 24-hour mean tropospheric OH concentrationsrange between 5–22 × 105 moleculescm–3, indicating an annualaveraged OH concentration of about 10 × 105 moleculescm–3. This valueis close to the estimated 9.7 ± 0.6 × 105 moleculescm–3 calculated fromthe reaction of CH3CCl3 with OH radicals.Comparison with CH4 generally shows good agreementbetween model and measurements, except for the site at Barrow where modelledwetland emission in the summer could be a factor 3 too high.For CO, the pronounced seasonality shown in the measurements is generally reproduced by the model; however, the modelled concentrations are lower thanthe measurements. This discrepancy may due to lower the CO emission,especially from biomass burning,used in the model compared with other studies.For O3, good agreement between the model and measurements is seenat locations which are away from industrial regions. The maximum discrepancies between modelled results and measurementsat tropical and remote marine sites is about 5–10 ppbv,while the discrepancies canexceed 30 ppbv in the industrial regions.Comparisons in rural areas at European and American continental sites arehighly influenced by the local photochemicalproduction, which is difficult to model with a coarse global CTM.The very large variations of O3 at these locations vary from about15–25 ppbv in Januaryto 55–65 ppbv in July–August. The observed annual O3amplitude isabout 40 ppbv compared with about 20 ppbv in the model. An overall comparison of modelled O3 with measurements shows thatthe O3seasonal surface cycle is generally governed bythe relative importance of two key mechanisms that drivea springtime ozone maximum and asummertime ozone maximum.  相似文献   

8.
Products and mechanisms for the gas-phase reactions of NO3 radicals with CH2=CHCl, CH2=CCl2, CHCl=CCl2,cis-CHCl=CHCl andtrans-CHCl=CHCl in air have been studied. The experiments were carried out at 295±2 K and 740±5 Torr in a 480-L Teflon-coated reaction chamber and at 295±2 K and 760±5 Torr in a 250-L stainless steel reactor. NO3 was generated by the thermal dissociation of N2O5. Experiments with15NO3 and CD2CDCl have also been performed. The initially formed nitrate peroxynitrates decay into carbonyl compounds, nitrates, HCl and ClNO2. In adidtion, there are indications of nitrooxy acid chlorides being produced. The reactions with CH2=CCl2 and CHCl=CCl2 are more complex due to release of chlorine atoms which eventually lead to formation of chloroacid chlorides.A general reaction mechanism is proposed and the observed concentration-time profiles of reactants and products are simulated for each compound. The rate constants for the initial step of NO3 addition to the chloroethenes are determined as: (2.6±0.5, 9.4±0.9, 2.0±0.4 and 1.4±0.4) × 10–16 cm3 molecule–1 s–1 for CH2=CHCl, CH2=CCl2, CHCl=CCl2 andcis-CHCl=CHCl, respectively.  相似文献   

9.
Nitrite oxidation in the tropospheric aqueous phase by freezing was evaluated by freezing a field sample. Nitrite oxidation by dissolved oxygen in the freezing process is much faster than by other oxidation processes, such as reactions with ozone, hydrogen peroxide or dissolved oxygen in an aqueous solution at pHs 3 to –6. At pH 4.5 and 25°C, the lifetime of nitrite in the aqueous phase is ca. 1 hr in oxidation by ozone (6×10-10 mol dm-3), ca. 10 hr in oxidation by H2O2 (2×10-4 mol dm-3), and 7.5 hr (Fischer and Warneck, 1996) in photodissociation at midday in summer. Under the same conditions at a temperature below 0°C, the lifetime of nitrite in the freezing process is estimated as ca. 2 sec when the droplets are frozen within a second. The reaction by freezing is affected by the presence of salts, such as NaCl or KCl, or orgnaic compounds, such as methanol or acetone. The results of freezing a field rain or fog sample showed that nitrite oxidation proceeds below pH 6, and the conversion ratio of nitrate from nitrite increases with decreasing pH. The oxidation of nitrite by freezing was also observed in freezing fog particles generated by an ultrasonic humidifier. The ratios of the concentrations of ions in the winter sample to those in the summer sample (or those in the fog sample) were almost the same values. However, the concentration of nitrite in the winter sample was lower than that estimated by the ratios of other ions. From the present study, it seems that the freezing process plays an important role in the nitrite sink process in the tropospheric aqueous phase.  相似文献   

10.
A comprehensive study on the chemistry of deposition and the concentration of tropospheric ozone and particulate sulfate in the ocean atmosphere was carried out for the data sets in 1990’s. It is important to study the atmospheric situation over the past years as well as the latest, especially in the East Asian region where emission amount of anthropogenic air pollutants have increased year by year due to rapid economic growth. The survey was conducted for 5 years in East Asia and West Oceania (35°N–35°S, 100–135°E) in August and September in 1990’s. The purpose of the survey was to study and understand the chemistry of deposition and the concentration of tropospheric ozone and particulate sulfate in the ocean atmosphere comprehensively in one project. Rainfall over the ocean was insufficiently neutralized. Gas and aerosol over the ocean were mature, i.e., well-mixed, during the period of the transportation. The characteristic latitudinal dependence was observed in the tropospheric ozone concentration, namely, higher in the southern hemisphere and lower in the northern hemisphere (approximately 25 ppb in the 10–40°S region and 5–15 ppb in the 20–40°N region). On the other hand, high concentrations of tropospheric ozone of over 30 ppb were observed in the northern hemisphere, which was attributable to the long-range transportation. The TSP concentration was approximately under the level of 40 μg m?3 irrespectively of the latitude; in contrast, the nss-SO4 2- concentration showed a clear latitudinal dependence, i.e., higher in the northern hemisphere and lower in the southern hemisphere. The background levels of the nss-SO4 2- concentration were approximately 0.5 μg m?3 in the 10–40°S region and 2–3 μg m?3 and 4–5 μg m?3 in the 0–20°N and 20–40°N regions, respectively.  相似文献   

11.
A study of marine aerosols over the Pacific Ocean   总被引：1，自引：0，他引：1  
Aerosol samples were collected on a Pacific cruise from 47°N to 55°S. Particle morphology, concentrations, and size distributions were analyzed with an electron microscope; elemental compositions of individual particles were determined with an X-ray energy spectrometer; and chemical compositions of bulk samples were measured with an ion chromatograph. Temporal and spatial variations of aerosol physico-chemical characteristics were studied in relation to ocean currents and atmospheric parameters. The results show that number and mass concentrations of primary particles depend mainly on surface wind speeds. However the ratios between the major ions, e.g., Na+, Cl-, and Mg++, are similar to the ratios in seawater regardless of location or meteorological conditions. The concentrations of secondary aerosols, e.g., non-seasalt sulfate, nitrate, and ammonium particles, show maxima at upwelling regions, such as along the California coast, at the Equator, and near the Chatham Rise where ascending motion brings nutrient-riched deep water into the surface layer. The number concentrations of small sulfate particles and large nitrate-coated particles showed diurnal variations with maxima in the early afternoon and minima at night, indicating that the particles are the products of photo-chemical reactions. Their precursor gases, e.g., CH3SCH3, NO, and NH3 are known to be released from seawater in upwelling regions where biological activities thrive.  相似文献   

12.
A box model, involving simple heterogeneous reaction processes associated with the production of non-sea-salt sulfate (nss-SO 4 2– ) particles, is used to investigate the oxidation processes of dimethylsulfide (DMS or CH3SCH3) in the marine atmosphere. The model is applied to chemical reactions in the atmospheric surface mixing layer, at intervals of 15 degrees latitude between 60° N and 60° S. Given that the addition reaction of the hydroxyl radical (OH) to the sulfur atom in the DMS molecule is faster at lower temperature than at higher temperature and that it is the predominant pathway for the production of methanesulfonic acid (MSA or CH3SO3H), the results can well explain both the increasing tendency of the molar ratio of MSA to nss-SO 4 2– toward higher latitudes and the uniform distribution with latitude of sulfur dioxide (SO2). The predicted production rate of MSA increases with increasing latitude due to the elevated rate constant of the addition reaction at lower temperature. Since latitudinal distributions of OH concentration and DMS reaction rate with OH are opposite, a uniform production rate of SO2 is realized over the globe. The primary sink of DMS in unpolluted air is caused by the reaction with OH. Reaction of DMS with the nitrate radical (NO3) also reduces DMS concentration but it is less important compared with that of OH. Concentrations of SO2, MSA, and nss-SO 4 2– are almost independent of NO x concentration and radiation field. If dimethylsulfoxide (DMSO or CH3S(O)CH3) is produced by the addition reaction and further converted to sulfuric acid (H2SO4) in an aqueous solution of cloud droplets, the oxidation process of DMSO might be important for the production of aerosol particles containing nss-SO 4 2– at high latitudes.  相似文献   

13.
The multi-channel reactions (1) CCl3CH2OH+Cl→ products and (2) CCl3CH2OH+OH→ products have been investigated by using the dual-level direct dynamics method. Two reaction channels, i.e., methylene- and hydroxyl-hydrogen abstraction, are identified for each reaction. The optimized geometries and frequencies of the stationary points are calculated at the B3LYP/6-311G(d,p) and MP2/6-311G(d,p) levels. Higher-level energies are obtained at the MC-QCISD and G3(MP2) levels based on the B3LYP and MP2 geometries, respectively, as well as by the CCSD(T)/6-31G(d)+CF method using the B3LYP geometries. Complexes with energies lower than those of the reactants are located at the entrance of each reaction channel. The rate constants for each reaction channel are evaluated by using the canonical variational transition state theory (CVT) incorporating the small-curvature tunneling (SCT) correction in a temperature range of 200–2000 K at the MC-QCISD//B3LYP/6-311G(d,p) level. The agreement of the calculated rate constants and experimental values for two reactions is seen to be remarkably good. Theoretical results indicate that in a low temperature range, the branching ratio to the hydroxyl-H-abstraction channel for both reactions is found negligible. The reactions proceed practically via methylene-H-abstraction yielding the products of CCl3CHOH+HCl and CCl3CHOH+H2O, respectively; while for reaction of CCl3CH2OH+Cl, hydroxyl-H-abstraction channel appears to be probable with the increase of temperature. The enthalpies of formation for the CCl3CH2OH, CCl3CHOH, and CCl3CH2O species are evaluated via isodesmic reactions at several levels.  相似文献   

14.
In this study, the chemical and physical losses of nitrogen oxides (NOx) over the Korean peninsula were discussed in order to better understand the effects of the NOx losses on the tropospheric NO2 columns. Initially, it was found that the physical loss processes due to dry and wet depositions had almost negligible impacts on the NOx loss processes over the Korean peninsula. In contrast, the hourly NOx chemical column losses were large at ??1014 molecules cm?2 h?1. The amounts of NOx removed for 1 hour account for approximately 33?C35% of the episode-averaged tropospheric NO2 columns during summer over the Korean peninsula. The NOx chemical column loss rates were 24.1?C70.9 times larger than the NOx physical column loss rates. In a budget analysis of the NOx chemical column losses, HNO3 formation via the reaction of OH + NO2 had the largest contribution toward the NOx chemical losses (42?C55% during fall and winter seasons; 76?C77% during spring; 92?C93% during summer). Large amounts of NOx were also removed by heterogeneous nitrate formation via N2O5 condensation during the cold seasons (42?C56%) over the Korean peninsula. The columnar NOx chemical losses took place mainly due to the two chemico-physical reaction processes, and also showed seasonal variations. PAN (Peroxyacetyl Nitrate) is another NO2 reservoir of potential importance. If the influence of the PAN-related chemistry on the NOx budget is considered, it can result in an approximate 69% increase in the NOx chemical column loss during summer. Such increases in the amounts of NOx removed for 1 hour due to the formation of PAN were equivalent to 56?C58% of the episode-averaged tropospheric NO2 columns during summer over the Korean peninsula. Such active NOx chemical losses during summer are another main factor for the tropospheric NO2 columns exhibiting their smallest values during summer.  相似文献   

15.
大气污染严重威胁了我国陆地生态系统的固碳能力,但随着减污降碳协同治理的快速推进,减缓大气污染将有利于提升陆地碳汇,并切实推动碳达峰碳中和目标的实现。为了更好地理解大气污染与生态系统固碳的关系,本文以主要空气污染物臭氧（O3）为例,基于田间控制实验的整合分析、剂量响应关系及机理模型三种评估方法综述了近地层O3污染对植被碳固定影响的最新进展。尽管不同作物种类以及品种、不同功能型木本植物对O3的响应有着显著的差异,且各种方法的评估结果也不尽相同,但目前O3浓度造成我国粮食作物减产、森林生产力降低已是不争的事实。持续升高的O3浓度将严重威胁我国陆地生态系统的固碳能力。利用我国作物和树木的O3剂量响应方程进行评估的结果表明,在CO2减排和O3污染协同治理下,预计2060年我国树木生物量和作物产量将比当前显著提高,增加陆地生态系统碳汇,助力碳中和目标。最后,对如何提高O3污染环境下植物固碳能力也进行了展望。  相似文献   

16.
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17.
Static flux chamber measurements of CCl4 uptake by soils in boreal, subtropical and tropical forests have been used to reassess the sink strength for this ozone depleting chemical. Happell and Roche (Geophys. Res. Lett. 30(2), 1088–1091, 2003) used flux estimates from soil concentration gradients to calculate a partial CCl4 atmospheric lifetime (τsoil) of 90 years. More recently, it is has been assumed that a better estimate of τsoil is 195 years (Montzka et al. 2011). In the work here, the rate of CCl4 uptake was calculated from 453 flux chamber measurements using an exponential fit to the chamber CCl4 concentration change with time. This analysis indicated that the flux rate estimate in Happell and Roche (Geophys. Res. Lett. 30(2) 1088–1091, 2003) was overestimated by 2.75, yielding a new estimate of τsoil for CCl4 of 245 years. Significant correlations of CCl4 uptake to temperature, soil moisture, or time of year were not observed. This work provides additional evidence that CCl4 uptake by soils is a common process and needs to be considered when developing an atmospheric budget for this compound.  相似文献   

18.
Abstract

We describe a one‐dimensional (1‐D) numerical model developed to simulate the chemistry of minor constituents in the stratosphere. The model incorporates most of the chemical species presently found in the upper atmosphere and has been used to investigate the effect of increasing chlorofluorocarbon (CFC) emissions on ozone (O3).

Our calculations confirm previous results that O3 depletions in the 20–25 km region, the region of the O3 maximum, are very sensitive to the relative abundances of Clx and NOy in the lower stratosphere for high Clx amounts. The individual abundances of lower stratospheric Clx and NOy amounts are very sensitive to upper tropospheric mixing ratios, which, in turn, are determined largely by surface input fluxes and heterogeneous loss processes. Thus the behaviour of column O3 depletions at high Clx levels is greatly affected, albeit indirectly, by tropospheric processes. For high Clx levels the Ox flux from the stratosphere to the troposphere is dramatically reduced, leading to a large reduction in tropospheric O3. Some of the variation between different published 1‐D model results is most likely due to this critical dependence of O3 depletion on NOy‐Clx ratios.

Model simulations of time‐dependent CFC effects on ozone indicate that if CFCs were to remain at constant 1980 emission rates while N2O increased at 0.25% a?1 and CH4 increased at 1% a?1, we could expect a 2.2% decrease in total column O3 (relative to the 1980 atmosphere) by the year 2000. However, if CFC emission rates were to increase by 3% a?1 (current estimates are 5–6% a?1), we would predict a depletion of 2.7% by the year 2000. The calculations for times beyond the year 2000 suggest that the effects on total O3 will begin to accelerate. If methyl chloroform emissions are added at 7% a?1 (current estimates are 7–9% a?1) to the above CFC‐N2O‐CH4 scenario we calculate total O3 depletions by the year 2000 that are 41% larger than those calculated without. This suggests that if the emissions of methyl chloroform continue to increase at their present rate then methyl chloroform could have a significant effect upon total O3.  相似文献   

19.
Methane,carbon monoxide and methylchloroform in the southern hemisphere   总被引：1，自引：0，他引：1  
New observational data on CH4, CO and CH3CCl3 in the southern hemisphere are reported. The data are analysed for long term trends and seasonal cycles. CH3CCl3 data are used to scale the OH fields incorporated in a two dimensional model, which in turn, is used to constrain the magnitude of a global CH4 source function. The possible causes of observed seasonality of CH3CCl3, CH4 and CO are identified, and several other aspects of observed CH4 variability are discussed.Possible future research directions are also given.  相似文献   

20.
Seven years of daily gas chromatographic measurements of CCl4 at the five globally distributed ALE/GAGE surface sites are reported. It is determined that CCl4 has been accumulating in the atmosphere at a rate of 1.3±0.1%/yr over the period 1978–1985 and that the releases of CCl4 into the atmosphere have remained fairly constant, with the smallest releases in 1981–1982. Using an inversion scheme based on a nine box model of the atmosphere, we infer a CCl4 lifetime of approximately 40 yr, an inventory on 1 July 1978 of (2.08±0.07)×109 kg and an average rate of release over the period 1978–1985 of (0.9±0.9)×107 kg/yr. These results produce excellent agreement with a release scenario derived from global production estimates for CCl4 and the major CCl4 byproduct, the chlorofluorocarbons. However, to obtain this consistency, it is necessary that our current ALE/GAGE absolute calibration standard be reduced approximately 25% thus bringing it into agreement with measurements by Yokohata et al. (1985) and Hanst et al. (1975).  相似文献   

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