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1.
Emission rates of biogenic volatile organic compounds emitted by the forests were estimated for five geographical regions as well as for all Switzerland. Monoterpene and isoprene emissions rates were calculated for each main tree species separately using the relevant parameters such as temperature, light intensity and leaf biomass density. Biogenic emissions from the forests were found to be about 23% of the total annual VOC emissions (anthropogenic and biogenic) in Switzerland. The highest emissions are in July and lowest in January. Calculations showed that the coniferous trees are the main sources of the biogenic emissions. The major contribution comes from the Norway spruce (picea abies) forests due to their abundance and high leaf biomass density. Although broad-leaved forests cover 27% of all the forests in Switzerland, their contribution to the biogenic emissions is only 3%. Monoterpenes are the main species emitted, whereas only 3% is released as isoprene. The highest emission rates of biogenic VOC are estimated to be in the region of the Alps which has the largest forest coverage in Switzerland and the major part of these forests consists of Norway spruce. The total annual biogenic VOC emission rate of 87 ktonnes y–1 coming from the forests is significantly higher than those from other studies where calculations were carried out by classifying the forests as deciduous and coniferous. The difference is attributed to the high leaf biomass densities of Norway spruce and fir (abies alba) trees which have a strong effect on the results when speciation of trees is taken into account. Besides the annual rate, emission rates were calculated for a specific period during July 4–6, 1991 when a photochemical smog episode was investigated in the Swiss field experiment POLLUMET. Emission rates estimated for that period agree well with those calculated for July using the average temperatures over the last 10 years.  相似文献   

2.
Airborne measurements of volatile organic compounds (VOC) were performed overthe tropical rainforest in Surinam (0–12 km altitude,2°–7° N, 54°–58° W) using the proton transferreaction mass spectrometry (PTR-MS) technique, which allows online monitoringof compounds like isoprene, its oxidation products methyl vinyl ketone,methacrolein, tentatively identified hydroxy-isoprene-hydroperoxides, andseveral other organic compounds. Isoprene volume mixing ratios (VMR) variedfrom below the detection limit at the highest altitudes to about 7 nmol/molin the planetary boundary layer shortly before sunset. Correlations betweenisoprene and its product compounds were made for different times of day andaltitudes, with the isoprene-hydroperoxides showing the highest correlation.Model calculated mixing ratios of the isoprene oxidation products using adetailed hydrocarbon oxidation mechanism, as well as the intercomparisonmeasurement with air samples collected during the flights in canisters andlater analysed with a GC-FID, showed good agreement with the PTR-MSmeasurements, in particular at the higher mixing ratios.Low OH concentrations in the range of 1–3 × 105molecules cm-3 averaged over 24 hours were calculated due to lossof OH and HO2 in the isoprene oxidation chain, thereby stronglyenhancing the lifetime of gases in the forest boundary layer.  相似文献   

3.
Assessment of Major Pools and Fluxes of Carbon in Indian Forests   总被引：3，自引：0，他引：3  
The major pools including phytomass, soil, litter, and fluxes of carbon (C)due to litterfall and landuse changes were estimated for Indian forests. Basedon growing stock-volume approach at the state and district levels, the Indianforest phytomass was estimated in the range of 3.8–4.3 PgC. The totalsoil organic pool in the top 1m depth was estimated as 6.8 PgC, usingestimated soil organic carbon densities and Remote Sensing (RS) based area byforest types. Based on 122 published Indian studies and RS-based forest area,the total litterfall carbon flux was estimated as 208.8 MgCha–1 yr–1.The cumulative net carbon flux (1880–1996) from Indian forests(1880–1996) due to landuse changes (deforestation, afforestation andphytomass degradation) was estimated as 5.4 PgC, using a simple book-keepingapproach. The mean annual net C flux due to landuse changes during1985–1996 was estimated as 9.0 TgC yr–1. For the recentperiod, the Indian forests are nationally a small source with some regionsacting as small sinks of carbon as well. The improved quantification of poolsand fluxes related to forest carbon cycle is important for understanding thecontribution of Indian forests to net carbon emissions as well as theirpotential for carbon sequestration in the context of the Kyoto protocol.  相似文献   

4.
Estimates of carbon emissions from the forest sector in Mexico are derived for the year 1985 and for two contrasting scenarios in 2025. The analysis covers both tropical and temperate closed forests. In the mid-1980s, approximately 804,000 ha/year of closed forests suffered major perturbations, of which 668,000 ha was deforestation. Seventy-five percent of total deforestation is concentrated in tropical forests. The resulting annual carbon balance from land-use change is estimated at 67.0 × 106 tons/year, which lead to net emissions of 52.3 × 106 tons/year accounting for the carbon uptake in restoration plantations and degraded forest lands. This last figure represents approximately 40% of the country's estimated annual total carbon emissions for 1985–1987. The annual carbon balance from the forest sector in 2025 is expected to decline to 28.0 × 106 t in the reference scenario and to become negative (i.e., a carbon sink), 62.0 × 106 t in the policy scenario. A number of policy changes are identified that would help achieve the carbon sequestration potential identified in this last scenario.  相似文献   

5.
Annual wet deposition of excess sulfate at Macquarie Island has been estimated from 5 months of rainwater composition data covering the Austral summer of 1985/86. The resulting figure of 2.1±0.6 mmol/m2/yr is at the low end of previous estimates of maritime excess sulfate deposition by precipitation. Within estimated uncertainty limits this figure is consistent with the DMS emission flux which would be predicted for latitude 50°–60° S, based solely on available Northern Hemispheric DMS measurements.Temporarily at the International Meteorological Institute, Stockholm University, S-106 91, Stockholm, Sweden.  相似文献   

6.
Emissions of biogenic volatile organic compounds (BVOC) were measured using a relaxed eddy accumulation (REA) technique on an above-canopy tower in a temperate forest (Changbai Mountain, Jilin province, China) during the 2010 and 2011 summer seasons. Solar global radiation and photosynthetically active radiation (PAR) were also measured. Based on PAR energy dynamic balance, an empirical BVOC emission and PAR transfer model was developed that includes the processes of BVOC emissions and PAR transfer above the canopy level, including PAR absorption and consumption, and scattering by gases, liquids, and particles (GLPs). Simulated emissions of isoprene and monoterpenes were in agreement with observations. The averages of the relative estimator biases for the flux were 39.3 % for isoprene, and 27.1 % for monoterpenes in the 2010 and 2011 growing seasons, with NMSE (normalized mean square error) values of 0.133 and 0.101, respectively. The observed and simulated mean diurnal variations of isoprene and monoterpenes in the 2010 and 2011 growing seasons were evaluated for the validation of the empirical model. Under observed atmospheric conditions, the sensitivity analysis showed that emissions of isoprene and monoterpenes were more sensitive to changes in PAR than to water vapor content or to the magnitude of the scattering factor. The emissions of isoprene and monoterpenes in the 2010 and 2011 growing seasons (from June to September) were estimated using this empirical model along with hourly observational data, with mean hourly emissions of 1.71 and 1.55 mg m?2 h?1 for isoprene, and 0.48 and 0.47 mg m?2 h?1 for monoterpenes in 2010 and 2011, respectively. As formaldehyde (HCHO) is considered as the main oxidation product of isoprene and monoterpenes, it is necessary to investigate the link between HCHO and BVOC emissions. GOME-2 HCHO vertical column densities (VCDs) can be used to estimate BVOC emission fluxes in the Changbai Mountain temperate forest.  相似文献   

7.
Experiments were conducted during the growing season of 1993 at a mixed deciduous forest in southern Ontario, Canada to investigate the atmospheric abundance of hydrocarbons from phytogenic origins, and to measure emission rates from foliage of deciduous trees. The most abundant phytogenic chemical species found in the ambient air were isoprene and the monoterpenes -pinene and -pinene. Prior to leaf-bud break during spring, ambient hydrocarbon mixing ratios above the forest remained barely above instrument detection limit (20 parts per trillion), but they became abundant during the latter part of the growing season. Peak isoprene mixing ratios reached nearly 10 parts per billion (ppbv) during mid-growing season while maximum monoterpene mixing ratios were close to 2 ppbv. Both isoprene and monoterpene mixing ratios exhibited marked diurnal variations. Typical isoprene mixing ratios were highest during mid-afternoon and were lowest during nighttime. Peak isoprene mixing ratios coincided with maximum canopy temperature. The diurnal pattern of ambient isoprene mixing ratio was closely linked to the local emissions from foliage. Isoprene emission rates from foliage were measured by enclosing branches of trees inside environment-controlled cuvette systems and measuring the gas mixing ratio difference between cuvette inlet and outlet airstream. Isoprene emissions depended on tree species, foliage ontogeny, and environmental factors such as foliage temperature and intercepted photosynthetically active radiation (PAR). For instance, young (<1 month old) aspen leaves released approximately 80 times less isoprene than mature (>3 months old) leaves. During the latter part of the growing season the amount of carbon released back to the atmosphere as isoprene by big-tooth and trembling aspen leaves accounted for approximately 2% of the photosynthetically fixed carbon. Significant isoprene mixing ratio gradients existed between the forest crown and at twice canopy height above the ground. The gradient diffusion approach coupled with similarity theory was used to estimate canopy isoprene flux densities. These canopy fluxes compared favorably with values obtained from a multilayered canopy model that utilized locally measured plant microclimate, biomass distribution and leaf isoprene emission rate data. Modeled isoprene fluxes were approximately 30% higher compared to measured fluxes. Further comparisons between measured and modeled canopy biogenic hydrocarbon flux densities are required to assess uncertainties in modeling systems that provide inventories of biogenic hydrocarbons.  相似文献   

8.
The effects of deep convection on the potential for forming ozone (ozone production potential) in the free troposphere have been simulated for regions where the trace gas composition is influenced by biomass burning. Cloud dynamical and photochemical simulations based on observations in 1980 and 1985 Brazilian campaigns form the basis of a sensitivity study of the ozone production potential under differing conditions. The photochemical fate of pollutants actually entrained in a cumulus event of August 1985 during NASA/GTE/ABLE 2A (Case 1) is compared to photochemical ozone production that could have occurred if the same storm had been located closer to regions of savanna burning (Case 2) and forest burning (Case 3). In each case studied, the ozone production potential is calculated for a 24-hour period following convective redistribution of ozone precursors and compared to ozone production in the absence of convection. In all cases there is considerably more ozone formed in the middle and upper troposphere when convection has redistributed NOx, hydrocarbons and CO compared to the case of no convection.In the August 1985 ABLE 2A event, entrainment of a layer polluted with biomass burning into a convective squall line changes the free tropospheric cloud outflow column (5–13 km) ozone production potential from net destruction to net production. If it is assumed that the same cloud dynamics occur directly over regions of savanna burning, ozone production rates in the middle and upper troposphere are much greater. Diurnally averaged ozone production following convection may reach 7 ppbv/day averaged over the layer from 5–13 km-compared to typical free tropospheric concentrations of 25–30 ppbv O3 during nonpolluted conditions in ABLE 2A. Convection over a forested region where isoprene as well as hydrocarbons from combustion can be transported into the free troposphere leads to yet higher amounts of ozone production.  相似文献   

9.
Biogenic Hydrocarbon Chemistry within and Above a Mixed Deciduous Forest   总被引：1，自引：0，他引：1  
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10.
Summary Wave-organized convective features in the southwest Indian Ocean are described using Hovmoller composites of satellite imagery, OLR anomalies and ECMWF precipitable water departures during the southern summer. Westward movement of large convective elements is noted in the 10–20°S latitude band in about half of the years between 1970 and 1984. A study of 47 convective systems from satellite imagery establishes the climatological features, including zonal propagation speeds for maritime systems in the range –2 to –4 m s–1, wavelengths of 25–35° longitude (3,000 km), lifespans of 10–20 days and convective areas of 7–10° longitude (800 km). Transient convective waves over the tropical SW Indian Ocean are slower and more diverse than their northern hemisphere counterparts. Interannual tendencies in the frequency and mode are studied. Wet summers over SE Africa correspond with an increased frequency of westward moving convective systems, whereas in dry summers convective systems tend to be quasi-stationary. INSAT data composites provide additional insight into the convective structure and show that tropical waves penetrated into southern Africa in February 1988. A more quantitative assessment of transient convective waves is provided by Hovmoller composites of OLR anomalies and precipitable water departures. Both display westward moving systems in 1976 and 1984 and highlight the wide variety and mixed mode character of convective waves. A case study is analyzed which illustrates the deepening of a moist, unstable layer coincident with the westward passage of a convective wave.With 12 Figures  相似文献   

11.
Humans seem to have doubled the global rate of terrestrial nitrogen fixation. Globally 50–70% (85 Tg, 1 Tg=1012 g) of the nitrogen supplied in fertilizer (80 Tg N/a) and leguminous crops (40–80 Tg N/a) are used to feed cattle. The aim of the present study was to derive some estimates of global N2O production from animal manure. As the parameter giving the most stable numerical basis for regional and global extrapolation we adopted the molar emission ratios of N2O to NH3. These ratios were measured in cattle, pig and chicken housings with different manure handling systems, in dung-heaps and in liquid manure storage tanks. Individual molar emission ratios from outside manure piles varied over two orders of magnitude, strongly dependent on the treatment of the manure. A median emission ratio of 1.6×10-2 (n=65) was obtained in cow-sheds with slatted floors and liquid manure stored underneath and a median ratio of 24×10-2 (n=31) was measured in a beef cattle housing with a solid manure handling system.We next extrapolated to global NH3 emissions from those estimated for Europe, using N uptake by the animals as a scaling factor. Multiplication with observed N2O to NH3 ratios next provided some estimates of regional and global N2O emissions. To account for the great variability of the emission ratios of N2O/NH3, we developed upper and lower case emission scenarios, based on lower and upper quartiles of measured emission ratios. The global emission from cattle and swine manure is in the range of 0.2–2.5 Tg N-N2O/a, representing 44+-39% of the annual atmospheric accumulation rate. This N2O emission arises from about 40 Tg N/a of cattle and pig manure stored in or at animal housings. We did not account for N2O emissions from another 50 Tg N/a excreted by grazing cattle, goats and sheep, and application of the manure to agricultural fields. Our study makes it clear that major anthropogenic N2O emissions may well arise from animal manure. The large uncertainty of emission ratios, which we encountered, show that much more intense research efforts are necessary to determine the factors that influence N2O emissions from domestic animal manure both in order to derive a more reliable global estimate of N2O release and to propose alternative waste treatment methods causing smaller N2O releases. In our studies we found large enhancements in N2O releases when straw was added to the manure, which is a rather common practice. In view of the ongoing discussion in Europe to re-install the traditional solid manure system (bed down cattle) for environmental and animal welfare reasons, it is noteworthy that our measurements indicate highest N2O release from this particulary system.In a similar manner, but based on a smaller data set, we also estimated the release of CH4 from cattle and swine manure and from liquid manure only to be about 9 Tg/year in good agreement with the estimate by the Environmental Protection Agency (1994) of 8.6+-2.6 Tg/year. A total annual methane release as high as 34 Tg/a was derived for solid and liquid cattle and pig manure from animals in housings.  相似文献   

12.
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13.
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   

14.
Potential Soil C Sequestration on U.S. Agricultural Soils   总被引：1，自引：0，他引：1  
Soil carbon sequestration has been suggested as a means to help mitigate atmospheric CO2 increases, however there is limited knowledge aboutthe magnitude of the mitigation potential. Field studies across the U.S. provide information on soil C stock changes that result from changes in agricultural management. However, data from such studies are not readily extrapolated to changes at a national scale because soils, climate, and management regimes vary locally and regionally. We used a modified version of the Intergovernmental Panel on Climate Change (IPCC) soil organic C inventory method, together with the National Resources Inventory (NRI) and other data, to estimate agricultural soil C sequestration potential in the conterminous U.S. The IPCC method estimates soil C stock changes associated with changes in land use and/or land management practices. In the U.S., the NRI provides a detailed record of land use and management activities on agricultural land that can be used to implement the IPCC method. We analyzed potential soil C storage from increased adoption of no-till, decreased fallow operations, conversion of highly erodible land to grassland, and increased use of cover crops in annual cropping systems. The results represent potentials that do not explicitly consider the economic feasibility of proposed agricultural production changes, but provide an indication of the biophysical potential of soil C sequestration as a guide to policy makers. Our analysis suggests that U.S. cropland soils have the potential to increase sequestered soil C by an additional 60–70 Tg (1012g) C yr– 1, over present rates of 17 Tg C yr–1(estimated using the IPCC method), with widespread adoption of soil C sequestering management practices. Adoption of no-till on all currently annually cropped area (129Mha) would increase soil C sequestration by 47 Tg C yr–1. Alternatively, use of no-till on 50% of annual cropland, with reduced tillage practices on the other 50%, would sequester less – about37 Tg C yr–1. Elimination of summer fallow practices and conversionof highly erodible cropland to perennial grass cover could sequester around 20 and 28Tg C yr–1, respectively. The soil C sequestration potentialfrom including a winter cover crop on annual cropping systems was estimated at 40Tg C yr–1. All rates were estimated for a fifteen-yearprojection period, and annual rates of soil C accumulations would be expected to decrease substantially over longer time periods. The total sequestration potential we have estimated for the projection period (83 Tg C yr–1) represents about 5% of 1999total U.S. CO2 emissions or nearly double estimated CO2 emissionsfrom agricultural production (43 Tg C yr–1). For purposes ofstabilizing or reducing CO2 emissions, e.g., by 7% of 1990 levels asoriginally called for in the Kyoto Protocol, total potential soil C sequestration would represent 15% of that reduction level from projected 2008 emissions(2008 total greenhouse gas emissions less 93% of 1990 greenhouse gasemissions). Thus, our analysis suggests that agricultural soil C sequestration could play a meaningful, but not predominant, role in helping mitigate greenhouse gas increases.  相似文献   

15.
In this paper we quantify the CH4, CO2 and NO x emissions during routine operations at a major oil and gas production facility, Prudhoe Bay, Alaska, using the concentrations of combustion by products measured at the NOAA-CMDL observatory at Barrow, Alaska and fuel consumption data from Prudhoe Bay. During the 1989 and 1990 measurement campaigns, 10 periods (called events) were unambiguously identified where surface winds carry the Prudhoe Bay emissions to Barrow (approximately 300 km). The events ranged in duration from 8–48 h and bring ambient air masses containing substantially elevated concentrations of CH4, CO2 and NO y to Barrow. Using the slope of the observed CH4 vs CO2 concentrations during the events and the CO2 emissions based on reported fuel consumption data, we calculate annual CH4 emissions of (24+/–8)×103 metric tons from the facility. In a similar manner, the annual NO x emissions are calculated to be (12+/–4)×103 metric tons, which is in agreement with an independently determined value. The calculated CH4 emissions represent the amount released during routine operations including leakage. However this quantity would not include CH4 released during non-routine operations, such as from venting or gas flaring.  相似文献   

16.
Two weather records kept at Nassau, Bahamas, from 1811 to 1837, and from 1838 to 1845, respectively, are analyzed and compared to 20th century reference periods. The average annual temperature of the period is 24.2°C (±0.65°C), which is 0.4°C lower than 1961–1990 and 0.1°C lower than 1901–1920, the coolest period in the 20th century. Cold periods occurred from 1812–1819 and 1835–1839. A warmer phase prevailed between these two episodes and another warm episode occurred in 1840–1842. Temperature fell after the volcanic eruptions of Tambora (April, 1815) and Coseguina (January, 1835). The maximum cooling after Tambora is estimated at 1.0°C (±0.56°) and after Coseguina is estimated at 0.4°C (±0.56°). The post-Tambora cooling is in line with previous estimates (Robock, personal communication). The 1810s were a period of extreme drought at Nassau and are unequalled in later years. Rainfall frequency was below contemporary (1812–1837) averages from 1812–1820 and 1836–1837 but was above average from 1821–1835. Moist (dry) periods occurred almost simultaneously with warm (cool) periods. The months of October, November, and April show the greatest (negative) deviations in precipitation frequency. Gale force winds were 85% more frequent than from 1901–1960. Much of this increase took place in the months of September through November and represents an increase in tropical cyclone frequency in the Nassau area above that of 1901–1960. Resultant winds show a tendency towards greater northerly components than in the 20th century, especially during the winter months. The increase in northerly wind components, temperatures below the 20th-century average, and reduction in rainfall frequency in the winter half of the year indicates a synoptic situation in which high pressure was more frequent over the southeast North American continent.  相似文献   

17.
A technique was developed that allows the determination of the stable carbon isotope ratio of isoprene in air. The method was used for a limited number of ambient measurements as well as laboratory studies of isoprene emitted from Velvet Bean (Mucana pruriens L. var. utilis), including the light and temperature dependence. The mean stable carbon isotope ratio ( 13C) of isoprene emitted from Velvet Bean (Mucana pruriens L. var. utilis) for all our measurements is –27.7 ± 2.0 (standard deviation for 23 data points). Our results indicate a small dependence of the stable carbon isotope ratios on leaf temperature and photosynthetic photon flux density (PPFD). The light dependence is 0.0026 ± 0.0012/( mol of photons m–2 s–1) for the studied range from 400 to 1700 mol of photons m–2 s–1. The temperature dependence is 0.16 ± 0.09/K. On average, the emitted isoprene is 2.6 ± 0.9 lighter than the leaf carbon. An uncertainty analysis of the possibility to use stable carbon isotope ratio measurements of isoprene for estimates of its mean photochemical age suggests that meaningful results can be obtained. This is supported by the results of a small number of measurements of the stable carbon isotope composition of ambient isoprene at different locations. The results range from approximately –29 to –16. They are consistent with vegetation emissions of isoprene that is slightly depleted in 13C relative to the plant material and enrichment of 13C in the atmosphere due to isotope fractionation associated with the reaction with OH-radicals. The stable carbon isotope ratio of ambient isoprene at locations directly influenced by isoprene emissions is very close to the values we found in our emission studies, whereas at sites located remote from isoprene emitting vegetation we find substantial enrichment of 13C. This suggests that stable carbon isotope ratio measurements will be a valuable, quantitative method to determine the extent of photochemical processing of isoprene in ambient air.  相似文献   

18.
Summary The diurnal variations of net radiation have been studied by analysing one year data measured at a tropical station, Osu (7.43° N, 4.58° E), in Nigeria. The maximum net daytime flux (which occurs around 14h local time) varies in the course of the year from 382.6±136.7Wm–2 in the wet season (April–October) to 480.3±61.8 Wm–2 in the dry season (November–March). The low values (and large fluctuations) of the hourly means recorded during the wet (monsoon) season are attributed to the important roles that the convective clouds and water vapour play in the atmospheric radiation budget, which is very pronounced in the tropical areas of West Africa.The daily amplitude of the net radiation is larger for the dry season (maximum in November) than it is for the wet season (minimum in July). A lag of about 2 hours is observed between the times when the maxima of the air temperature and the net radiation courses occur over the area.On leave from the Department of Physics, Obafemi Awolowo University, Ile-Ife, Nigeria.With 5 Figures  相似文献   

19.
A simple methane model is presented in which lifetime changes are expressed as a function of CH4 concentration and emissions of NOx CO and NMHCs. The model parameters define the relative sensitivities of lifetime to these determining factors. The parameterized model is fitted to results from five more complex atmospheric chemistry models and to 1990 IPCC concentration projections. The IPCC data and four of the five models are well fitted, implying that the models have similar relative sensitivities. However, overall sensitivities of lifetime to changes in atmospheric composition vary widely from model to model. The parameterized model is used to estimate the history of past methane emissions, lifetime changes and OH variations, with estimates of uncertainties. The pre-industrial lifetime is estimated to be 15–34% lower than today. This implies that 23–55% of past concentration changes are due to lifetime changes. Pre-industrial emissions are found to be much higher (220–330 TgCH4/y) than the best estimate of present natural emissions (155 TgCH4/y). The change in emissions since pre-industrial times is estimated to lie in the range 160–260 TgCH4/y, compared with the current best guess for anthropogenic emissions of 360 TgCH4/y. These results imply either that current estimates of anthropogenic emissions are too high and/or that there have been large changes in natural emissions. 1992 IPCC emissions scenarios are used to give projections of future concentration and lifetime changes, together with their uncertainties. For any given emissions scenario, these uncertainties are large. In terms of future radiative forcing and global-mean temperature changes over 1990–2100 they correspond to uncertainties of at least ±0.2 Wm–2 and ± 0.1° C, respectively.  相似文献   

20.
The fluxes of ozone and NOx out of the atmospheric boundary layer (ABL) over Europe are calculated in a mesoscale chemical transport model (MCT) and compared with the net chemical production or destruction of ozone and the emissions of precursors within the ABL for two 10 days' periods which had quite different synoptic situations and levels of photochemical activity (1–10 July 1991 (JUL91) and 26 October–4 November 1994 (ON94)). Over the European continent, about 8% of the NOx emissions were brought from the ABL to the free troposphere as NOx, while about 15% of the NOx emissions were brought to the free troposphere as NOy–NOx, i.e. as PAN or HNO3. The convection dominates over the synoptic scale vertical advection as a transport mechanism both for NOx and NOy out of the boundary layer in the summertime high pressure situation (JUL91), while in the fall situation (ON94) the convective part was calculated to be the smallest. NOx was almost completely transformed to NOy–NOx or removed within the ABL. Also for NOy the major part of the atmospheric cycle is confined to the ABL both for JUL91 and ON94. The vertical transport time out of the ABL is of the order of 100h both for the total model domain and over the European continent. The net convective exchange of ozone from the ABL is not a dominant process for the amount of ozone in the ABL averaged over 10 days and the whole domain, but convection reduces the maximum ozone concentration in episodes significantly. The ozone producing efficiency of NOx is calculated to increase with height to typically 15–20 in the upper half of the troposphere from around 5 in the ABL, but in the middle free troposphere the concentration of NOx is often too low to cause net chemical formation of ozone there.  相似文献   

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