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1.
Based on an estimated global fuel consumption of 2.57 × 1015g(C) y–1 and the assumption thatthe fossil fuel burned in Austria is globallyrepresentative, an upper limit of 0.021 (+150%, –50%)Tg y–1 for global CH3CN emission dueto fossil fuel burning was obtained from the relativeenhancement of the concentrations of toluene, benzene,and acetonitrile (methyl cyanide) during strong,short-term traffic pollution. This is less than 6% ofthe total global budget of CH3CN, which is dominatedby an emission rate of 0.8 Tg y–1 from biomassburning.  相似文献   

2.
The stable carbon isotope ratios of nonmethane hydrocarbons (NMHC) and methyl chloride emitted from biomass burning were determined by analyzing seven whole air samples collected during different phases of the burning process as part of a laboratory study of wood burning. The average of the stable carbon isotope ratios of emitted alkanes, alkenes and aromatic compounds is identical to that of the burnt fuel; more than 50% of the values are within a range of ±1.5 of thecomposition of the burnt fuel wood. Thus for the majority of NMHC emitted from biomass burning stable carbon isotope ratio of the burnt fuel a good first order approximation for the isotopic composition of the emissions. Of the more than twenty compounds we studied, only methyl chloride and ethyne differed in stable carbon isotope ratios by more than a few per mil from the composition of the fuel. Ethyne is enriched in 13C by approximately 20–30, and most of the variability can beexplained by a dependence on flame temperature. The 13C values decreaseby 0.019 /K (±0.0053/K) with increasing temperature. Methyl chloride is highly depleted in 13C, on average by25. However the results cover a wide range of nearly 30. Specifically, in two measurements with wood from Eucalyptus (Eucalyptus delegatensis) as fuel we observed the emission of extremely light methyl chloride (–68.5and–65.5). This coincides with higher than average emission ratiosfor methyl chloride (15.5 × 10–5 and 18 ×10–5 mol CH3Cl/mol CO2). These high emission ratios are consistent with the highchlorine content of the burnt fuel, although, due to the limited number of measurements, it would be premature to generalize these findings. The limited number of observations also prevents any conclusion on a systematic dependence between chlorine content of the fuel, emission ratios and stable carbon isotope ratio of methyl chloride emissions. However, our results show that a detailed understanding of the emissions of methyl chloride from chloride rich fuels is important for understanding its global budget. It is also evident that the usefulness of stable carbon isotope ratios to constrain the global budget of methyl chloride will be complicated by the very large variability of the stable carbon isotope ratio of biomass burning emissions. Nevertheless, ultimately the large fractionation may provide additional constraints for the contribution of biomass burning emissions to the atmospheric budget of methyl chloride.  相似文献   

3.
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   

4.
We measured CO2, CO, CH4, H2, and NO2 in air masses polluted by savanna fires over Côte d'Ivoire, western Africa. Elevated concentrations of these trace gases were found in fire plumes and also in extensive haze layers. Trace gas mixing ratios ranged as high as 605 ppmv for CO2, 14.8 ppmv for CO, 2.7 ppmv for CH4, 4.2 ppmv for H2, and 25 ppbv for NO2. We compare our emission ratios to those obtained in previous field and laboratory studies. The emission ratios, expressed as an average and as a range or as an average only, were: dCO/dCO2 5.3×10–2 (3–18×10–2); dCH4/dCO 5.3×10–2; dH2/dCO 2.4×10–1 and dNO2/dCO2 1.8×10–4 (1.5–2.2×10–4). The values found match those found during similar measurements, though our results point to rather vigorous burning in the savanna of western Africa.  相似文献   

5.
The annual trace gas emissions from a West African rural region were calculated using direct observations of gas emissions and burning practices, and the findings compared to the guidelines published by the IPCC. This local-scale study was conducted around the village of Dalun in the Northern Region of Ghana, near the regional capital of Tamale. Two types of fires were found in the region – agricultural fires andwildfires. Agricultural fires are intentionally set in order to remove shrub and crop residues; wildfires are mostly ignited by herders to remove inedible grasses and to promote the growth of fresh grass. An agricultural fire is ignited with a fire front moving against the wind (backfire), whereas a wildfire moves with the wind (headfire). Gas emissions (CO2, CO and NO) weremeasured by burning eight experimental plots, simulating both headfires and backfires. A common method of evaluating burning conditions is to calculate modified combustion efficiency (MCE), which expresses the percentage of the trace gases released as CO2. Modified combustion efficiency was95% in the wildfires burned as headfires, but only 90% in the backfires.The burned area in the study region was determined by classifying a SPOT HRV satellite image taken about two months into the dry season. Fires were classified as either old burned areas or new burned areas as determined by the gradient in moisture content in the vegetation from the onset of the dry season. Classified burned areas were subsequently divided into two classes depending on whether the location was in the cultivated area or in the rangeland area, this sub-classification thus indicating whether the fire had been burned as a backfire or headfire. Findings showed that the burned area was 48% of the total region, and that the ratio of lowland wildfiresto agricultural fires was 3:1. The net trace gas release from the classified vegetation burnings were extrapolated to 26–46×108 gCO2, 78–302×106 g CO,17–156×105 g CH4,16–168×105 g NMHC and 11–72×103 NOx. Calculation of the emissionsusing proposed IPCC default values on burned area and average biomass resulted in a net emission 5 to 10 times higher than the measured emission values. It was found that the main reason for this discrepancy was not the emission factorsused by the IPCC, but an exaggerated fuel load estimate.  相似文献   

6.
Carbonyl sulfide emissions from biomass burning have been studied during field experiments conducted both in an African savanna area (Ivory Coast) and rice fields, central highland pine forest and savanna areas in Viet-Nam. During these experiments CO2, CO and C2H2 or CH4 have also been also monitored. COS values range from 0.6 ppbv outside the fires to 73 ppbv in the plumes. Significant correlations have been observed between concentrations of COS and CO (R 2=0.92,n=25) and COS and C2H2 (R 2=0.79,n=26) indicating a COS production during the smoldering combustion. COS/CO2 emission factors (COS/CO2) during field experiments ranged from 1.2 to 61×10–6 (11.4×10–6 mean value). COS emission by biomass burning was estimated to be up to 0.05 Tg S/yr in tropics and up to 0.07 Tg S/yr on a global basis, contributing thus about 10% to the global COS flux. Based on the S/C ratio measured in the dry plant biomass and the COS/CO2 emission factor, COS can account for only about 7% of the sulfur emitted in the atmosphere by biomass burning.  相似文献   

7.
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   

8.
In situ AGAGE GC-MS measurements of methyl bromide (CH3Br) and methyl chloride (CH3Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr−1 (CH3Br) and 2.6% yr−1 (CH3Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH3Br and CH3Cl also show annual decreases in their baseline mixing ratios of 2.5% yr−1 and 1.5% yr−1, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH3Br) and 541.3 ± 1.1 ppt (CH3Cl). Although CH3Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH3Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).  相似文献   

9.
Rate constants for the gas-phase reactions of OH radicals, NO3 radicals and O3 with the C7-carbonyl compounds 4-methylenehex-5-enal [CH2=CHC(=CH2)CH2CH2CHO], (3Z)- and (3E)-4-methylhexa-3,5-dienal [CH2=CHC(CH3)=CHCH2CHO] and 4-methylcyclohex-3-en-1-one, which are products of the atmospheric degradations of myrcene, Z- and E-ocimene and terpinolene, respectively, have been measured at 296 ± 2 K and atmospheric pressure of air using relative rate methods. The rate constants obtained (in cm3 molecule–1 s–1 units) were: for 4-methylenehex-5-enal, (1.55 ± 0.15) × 10–10, (4.75 ± 0.35) × 10–13 and (1.46 ± 0.12) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3Z)-4-methylhexa-3,5-dienal: (1.61 ± 0.35) × 10–10, (2.17 ± 0.30) × 10–12, and (4.13 ± 0.81) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3E)-4-methylhexa-3,5-dienal: (2.52 ± 0.65) × 10–10, (1.75 ± 0.27) × 10–12, and (5.36 ± 0.28) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; and for 4-methylcyclohex-3-en-1-one: (1.10 ± 0.19) × 10–10, (1.81 ± 0.35) × 10–12, and (6.98 ± 0.40) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively. These carbonyl compounds are all reactive in the troposphere, with daytime reaction with the OH radical and nighttime reaction with the NO3 radical being predicted to dominate as loss processes and with estimated lifetimes of about an hour or less.  相似文献   

10.
Tropical forest conversion, shiftingcultivation and clearing of secondary vegetation makesignificant contributions to global emissions ofgreenhouse gases today, and have the potential forlarge additional emissions in future decades. Globally, an estimated 3.1×109 t of biomasscarbon of these types is exposed to burning annually,of which 1.1×109 t is emitted to the atmospherethrough combustion and 49×106 t is converted tocharcoal (including 26–31×106 t C of blackcarbon). The amount of biomass exposed to burningincludes aboveground remains that failed to burn ordecompose from clearing in previous years, andtherefore exceeds the 1.9×109 t of abovegroundbiomass carbon cleared on average each year. Above-and belowground carbon emitted annually throughdecomposition processes totals 2.1×109 t C. Atotal gross emission (including decomposition ofunburned aboveground biomass and of belowgroundbiomass) of 3.41×109 t C year-1 resultsfrom clearing primary (nonfallow) and secondary(fallow) vegetation in the tropics. Adjustment fortrace gas emissions using IPCC Second AssessmentReport 100-year integration global warming potentialsmakes this equivalent to 3.39×109 t ofCO2-equivalent carbon under a low trace gasscenario and 3.83×109 t under a high trace gasscenario. Of these totals, 1.06×109 t (31%)is the result of biomass burning under the low tracegas scenario and 1.50×109 t (39%) under thehigh trace gas scenario. The net emissions from allclearing of natural vegetation and of secondaryforests (including both biomass and soil fluxes) is2.0×109 t C, equivalent to 2.0–2.4×109 t of CO2-equivalent carbon. Adding emissions of0.4×109 t C from land-use category changesother than deforestation brings the total for land-usechange (not considering uptake of intact forest,recurrent burning of savannas or fires in intactforests) to 2.4×109 t C, equivalent to 2.4–2.9×109 t of CO2-equivalent carbon. The totalnet emission of carbon from the tropical land usesconsidered here (2.4×109 t C year-1)calculated for the 1981–1990 period is 50% higherthan the 1.6×109 t C year-1 value used by the Intergovernmental Panel on Climate Change. The inferred (= `missing') sink in the global carbonbudget is larger than previously thought. However,about half of the additional source suggested here maybe offset by a possible sink in uptake by Amazonianforests. Both alterations indicate that continueddeforestation would produce greater impact on globalcarbon emissions. The total net emission of carboncalculated here indicates a major global warmingimpact from tropical land uses, equivalent toapproximately 29% of the total anthropogenic emissionfrom fossil fuels and land-use change.  相似文献   

11.
A global three-dimensional chemical transport model has been used to identify and evaluate possible candidates for the `missing' surface source required to balance the atmospheric budget of methyl bromide. Both natural and anthropogenic emissions of methyl bromide are `coloured' in the model, thus allowing the global CH3Br distribution to be broken-down into its source components. These coloured CH3Br tracers are then combined in various ways to create one base-line emission scenario and five further plausible scenarios. The additional emission scenarios are specifically designed to test whether the geographical distribution and seasonal cycles of additional vegetation and/or increased biomass burning emissions are consistent with atmospheric observations of methyl bromide mixing ratios. Due to an imbalance in our current understanding of the methyl bromide budget, simulated CH3Br mixing ratios from the base-line emission scenario are significantly lower than atmospheric measurements. Both the inclusion of a vegetation source in the tropics and a double strength biomass burning source substantially improve the agreement between model simulations and atmospheric measurements compared with the base-line emission scenario. While measurement data provides useful information on global fluxes and regional CH3Br seasonal cycles, small differences between the simulated seasonal cycles of different emission scenarios makes it difficult to distinguish between the relative likelihoods of model scenarios containing a tropical vegetation source or an increased biomass burning source. Further measurements performed in continental mid-to-high northern latitudes, central-southern Africa and South America would be of particular benefit in future attempts to constrain the location and magnitude of the natural terrestrial sources of methyl bromide.  相似文献   

12.
Semi-continuous measurements of CFCl3, CF2Cl2, CCl4, CH3CCl3 and N2O were made at Adrigole, Ireland as part of the Atmospheric Lifetime Experiment (ALE). Clean, baseline air from the Atlantic Ocean was measured approximately 70% of the time; pollution events from Europe, for the remainder. The two final years of ALE data from Adrogole give a five-year record from July 1978 to June 1983. This paper extends previous work on the relative enhancements of trace gases during pollution episodes and presents (1) unambiguous identification of elevated levels of N2O concurrent with halocarbon pollution events, (2) detection of trends in emission of CH3CCl3, (3) discovery of seasonal variations in emission of CF2Cl2, CCl4 and CH3CCl3, (4) characterization of typical summer and winter pollution episodes, and (5) identification of weather patterns over Europe that are associated with high concentrations of CFCs at Adrigole. Some of these results assume that CFCl3 represents a uniform, well buffered source from the continent. The latter two results are particularly useful in the testing and calibration of three-dimensional chemical transport models. Observed enhancements are marginally consistent with estimates of halocarbon use by the chemical industry. The source of nitrous oxide correlated with halocarbons is 0.8 Tg(N)/yr from Europe alone and represents approximately 10% of the global stratospheric loss.  相似文献   

13.
Biomass burning has important impacts on atmospheric chemistry and climate. Fires in tropical forests and savannas release large quantities of trace gases and particulate matter. Combustion of biofuels for cooking and heating constitutes a less spectacular but similarly widespread biomass burning activity. To provide the groundwork for a quantification of this source, we determined in rural Zimbabwe the emissions of CO2, CO, and NO from more than 100 domestic fires fueled by wood, agricultural residues, and dung. The results indicate that, compared to open savanna fires, emissions from domestic fires are shifted towards products of incomplete combustion. A tentative global analysis shows that the source strength of domestic biomass burning is on the order of 1500 Tg CO2–C yr–1, 140 Tg CO–C yr–1, and 2.5 Tg NO–N yr–1. This represents contributions of about 7 to 20% to the global budget of these gases.  相似文献   

14.
The flux of CH4 and CO2 from termite nests into the atmosphere has been measured in a broad-leafed-type savannah in South Africa. Measurements were carried out on nests of species of six genera, i.e., Hodotermes, Macrotermes, Odontotermes, Trinervitermes, Cubitermes, and Amitermes. The flux rates of CH4 relative to the flux rate of CO2 in terms of carbon obtained for the individual species showed ratios of 2.9×10-3, 7.0×10-4, 6.7×10-5, 8.7×10-3, 2.0×10-3 and 4.2×10-3, respectively. Using data published on the assimulation efficiencies of termites, the flux of carbon as CH4 accounts for 6.0×10-5 to 2.6×10-3 of the carbon ingested which results in a global CH4 emission by termites of 2 to 5×1012 g/yr. Methane is decomposed in the soil with average decomposition rates of 52 g/m2/h. The annual CH4 consumption in the tropics and subtropics is estimated to be 21×1012 g which exceeds the CH4 emission rate by termites.  相似文献   

15.
The relative rate technique has been used to measure rate constants for the reaction of chlorine atoms with peroxyacetylnitrate (PAN), peroxypropionylnitrate (PPN), methylhydroperoxide, formic acid, acetone and butanone. Decay rates of these organic species were measured relative to one or more of the following reference compounds; ethene, ethane, chloroethane, chloromethane, and methane. Using rate constants of 9.29×10–11, 5.7×10–11, 8.04×10–12, 4.9×10–13, and 1.0×10–13 cm3 molecule–1 sec–1 for the reaction of Cl atoms with ethene, ethane, chloroethane, chloromethane, and methane respectively, the following rate constants were derived, in units of cm3 molecule–1 s–1: PAN, <7×10–15; PPN, (1.14±0.12)×10–12; HCOOH, (2.00±0.25)×10–13; CH3OOH, (5.70±0.23)×10–11; CH3COCH3, (2.37±0.12)×10–12; and CH3COC2H5, (4.13±0.57)×10–11. Quoted errors represent 2 and do not include possible systematic errors due to errors in the reference rate constants. Experiments were performed at 295±2 K and 700 torr total pressure of nitrogen or synthetic air. The results are discussed with respect to the previous literature data and to the modelling of nonmethane hydrocarbon oxidation in the atmosphere.In recent discussions with Dr. R. A. Cox of Harwell Laboratory, UKAEA, we learnt of a preliminary value for the rate constant of the reaction of Cl with acetone of (2.5±1.0)×10–12 cm3 molecule–1 sec–1 measured by R. A. Cox, M. E. Jenkin, and G. D. Hayman using molecular modulation techniques. This value is in good agreement with our results.  相似文献   

16.
A global data set on the geographic distribution and seasonality of freshwater wetlands and rice paddies has been compiled, comprising information at a spatial resolution of 2.5° by latitude and 5° by longitude. Global coverage of these wetlands total 5.7×106 km2 and 1.3×106 km2, respectively. Natural wetlands have been grouped into six categories following common terminology, i.e. bog, fen, swamp, marsh, floodplain, and shallow lake. Net primary productivity (NPP) of natural wetlands is estimated to be in the range of 4–9×1015 g dry matter per year. Rice paddies have an NPP of about 1.4×1015 g y–1. Extrapolation of measured CH4 emissions in individual ecosystems lead to global methane emission estimates of 40–160 Teragram (1 Tg=1012 g) from natural wetlands and 60–140 Tg from rice paddies per year. The mean emission of 170–200 Tg may come in about equal proportions from natural wetlands and paddies. Major source regions are located in the subtropics between 20 and 30° N, the tropics between 0 and 10° S, and the temperate-boreal region between 50 and 70° N. Emissions are highly seasonal, maximizing during summer in both hemispheres. The wide range of possible CH4 emissions shows the large uncertainties associated with the extrapolation of measured flux rates to global scale. More investigations into ecophysiological principals of methane emissions is warranted to arrive at better source estimates.  相似文献   

17.
Since 1978, a measuring station has been operated at Cape Point (34°21 S, 18°29 E). In this article, results of measurements of CO, CFCl3, CCl4, O3, N2O and CH4 are presented as monthly means and analyzed with respect to long-term trends and seasonal variations. For CO and CH4, very similar seasonal variations have been observed, indicating strong interrelations between these two gases. For CO and O3, no significant changes of the mean annual concentrations can be established for the observation periods of 10 and 5 years, respectively. The measurements yield a growth rate of 9.1 pptv yr-1 for CFCl3 (1980–1987) and 0.6 ppbv yr-1 for N2O (1983–1987). The concentration increases of CH4 (10.3 ppbv yr-1 for 1983–1987) and of CCl4 (2.1 pptv yr-1 for 1980–1988) are analyzed for temporal changes during the last years.Presented at the Second Conference on Baseline Observations in Atmospheric Chemistry (SABOAC II) in Melbourne, Australia, November 1988.  相似文献   

18.
The following Henry's law constants (K H/mol2kg-2atm-1) for HNO3 and the hydrohalic acids have been evaluated from available partial pressure and other thermodynamic data from 0°–40°C, 1 atm total pressure: HNO 3 , 40°C–5.85×105; 30°C–1.50×106; 25°C–2.45×106; 20°C–4.04×106; 10°C–1.15×107; 0°C–3.41×107. HF, 40°C–3.2; 30°C–6.6; 25°C–9.61; 20°C–14.0; 10°C–32.0; 0°C–76. HCl, 40°C–4.66×105; 30°C–1.23×106; 25°C–2.04×106; 20°C–3.37×106; 10°C–9.71×106; 0°C–2.95×107. HBr, 40°C–2.5×108; 30°C–7.5×108; 25°C–1.32×109; 20°C–2.37×109; 10°C–8.10×109; 0°C–3.0×1010. HI, 40°C–5.2×108; 30°C–1.5×109; 25°C–2.5×109; 20°C–4.5×109; 10°C–1.5×1010; 0°C–5.0×1010. Simple equilibrium models suggest that HNO3, CH3SO3H and other acids up to 10x less soluble than HCl displace it from marine seasalt aerosols. HF is displaced preferentially to HCl by dissolved acidity at all relative humidities greater than about 80%, and should be entirely depleted in aged marine aerosols.  相似文献   

19.
Aerosol chemical composition and trace gas measurements were made at twolocations on the northeastern peninsula of Tenerife during the ACE-2HILLCLOUD experiment, between 28 June and 23 July 1997. Measurementswere made of coarse (#gt;2.5 m aerodynamic diameter) and fine (#lt; 2.5m) aerosol Cl–, NO3 –,SO4 2–, non-sea saltSO4 2– (NSSS),CH3SO3 – (MSA) andNH4 +, and gas phase dimethylsulphide (DMS), HCl,HNO3, SO2, CH3COOH, HCOOH andNH3. Size distributions were measured using a cascadeimpactor. Results show that in marine air masses NSSS and MSA wereformed via DMS oxidation, with additional NSSS present in air massescontaining a continental component. Using a Eulerian box model approachfor aerosols transported between upwind and downwind sites, a mean NSSSproduction rate of 4.36 × 10–4 gm–3 s–1 was calculated for daytimeclear sky periods (highest insolation), with values for cloudy periodsduring daytime and nighttime of 3.55 × 10–4 and2.40 × 10–4 g m–3s–1, respectively. The corresponding rates for MSA were6.23 × 10–6, 8.49 × 10–6and 6.95 × 10–6 g m–3s–1, respectively. Molar concentration ratios forMSA/NSSS were 8.7% (1.8–18.2%) and 1.9%(1.3–3.5%) in clean and polluted air masses, respectively.Reactions occurring within clouds appeared to have a greater influenceon rates of MSA production, than of NSSS, while conversely daytime gasphase reactions were more important for NSSS. For MSA, nighttimein-cloud oxidation rates exceeded rates of daytime gas phase productionvia OH oxidation of DMS. NSSS, MSA and ammonium had trimodal sizedistributions, with modes at 0.3, 4.0 and >10.0 m (NSSS andNH4 +), and 0.3, 1.5 and 4.0 m (MSA). Nosignificant production of other aerosol species was observed, with theexception of ammonium, which was formed at variable rates dependent onneutralisation of the aerosol with ammonia released from spatiallynon-uniform surface sources. Seasalt components were mainly present incoarse particles, although sub-micrometre chloride was also measured.Losses by deposition exceeded calculated expectations for all species,and were highest for the seasalt fraction and nitrate.  相似文献   

20.
This assessment of the atmospheric methane budget for the African Continent is based on a set of experimental data obtained in tropical Africa including methane emission from various biogenic sources, and biomass burning, and methane consumption in savanna and forest soils. Emission rates from the various sources, uptake rates of soils, and complementary data from the litterature allow calculation of regional methane fluxes by means of different data bases. Biomass burning, animals and natural wetlands are the three dominant sources of methane in Africa while rice paddy fields and termites appear as minor sources. The total methane emission is estimated to be in the range 20–40 MT of CH4 per year, methane uptake by soils being less than 2 MT per year. Net methane emission from the African continent accounts for less than 10% of global emissions from terrestrial ecosystems.  相似文献   

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