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1.
Abstract

A coupled 1‐D radiative‐convective and photochemical diffusion model is used to study the influence of ozone photochemistry on changes in the vertical temperature structure and surface climate resulting from the doubling of atmospheric CO2, N2O, CH4 and increased stratospheric aerosols owing to the El Chichón volcanic eruption. It is found when CO2 alone is doubled, that the total ozone column increases by nearly 6% and the resulting increase in the solar heating contributes a smaller temperature decrease in the stratosphere (up to 4 K near the stratopause level). When the concentration of CO2, N2O and CH4 are simultaneously doubled, the total ozone column amount increases by only 2.5% resulting in a reduced temperature recovery in the stratosphere. Additional results concerning the effect of the interaction of ozone photochemistry with the stratospheric aerosol cloud produced by the El Chichón eruption show that it leads to a reduction in stratospheric ozone, which in turn has the effect of increasing the cooling at the surface and above the cloud centre while causing a slight warming below in the lower stratosphere.  相似文献   

2.
Abstract

To evaluate future climate change in the middle atmosphere and the chemistry–climate interaction of stratospheric ozone, we performed a long-term simulation from 1960 to 2050 with boundary conditions from the Intergovernmental Panel on Climate Change A1B greenhouse gas scenario and the World Meteorological Organization Ab halogen scenario using the chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). In addition to this standard simulation we performed five sensitivity simulations from 2000 to 2050 using the rerun files of the simulation mentioned above. For these sensitivity simulations we used the same model setup as in the standard simulation but changed the boundary conditions for carbon dioxide (CO2), methane (CH4), nitrous oxide (N2O), and ozone-depleting substances (ODS). In the first sensitivity simulation we fixed the mixing ratios of CO2, CH4, and N2O in the boundary conditions to the amounts for 2000. In each of the four other sensitivity simulations we fixed the boundary conditions of only one of CO2, CH4, N2O, or ODS to the year 2000.

In our model simulations the future evolution of greenhouse gases leads to significant cooling in the stratosphere and mesosphere. Increasing CO2 mixing ratios make the largest contributions to this radiative cooling, followed by increasing stratospheric CH4, which also forms additional H2O in the upper stratosphere and mesosphere. Increasing N2O mixing ratios makes the smallest contributions to the cooling. The simulated ozone recovery leads to warming of the middle atmosphere.

In the EMAC model the future development of ozone is influenced by several factors. 1) Cooler temperatures lead to an increase in ozone in the upper stratosphere. The strongest contribution to this ozone production is cooling due to increasing CO2 mixing ratios, followed by increasing CH4. 2) Decreasing ODS mixing ratios lead to ozone recovery, but the contribution to the total ozone increase in the upper stratosphere is only slightly higher than the contribution of the cooling by greenhouse gases. In the polar lower stratosphere a decrease in ODS is mainly responsible for ozone recovery. 3) Higher NOx and HOx mixing ratios due to increased N2O and CH4 lead to intensified ozone destruction, primarily in the middle and upper stratosphere, from additional NOx; in the mesosphere the intensified ozone destruction is caused by additional HOx. In comparison to the increase in ozone due to decreasing ODS, ozone destruction caused by increased NOx is of similar importance in some regions, especially in the middle stratosphere. 4) In the stratosphere the enhancement of the Brewer-Dobson circulation leads to a change in ozone transport. In the polar stratosphere increased downwelling leads to additional ozone in the future, especially at high northern latitudes. The dynamical impact on ozone development is higher at some altitudes in the polar stratosphere than the ozone increase due to cooler temperatures. In the tropical lower stratosphere increased residual vertical upward transport leads to a decrease in ozone.  相似文献   

3.
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   

4.
A mean meridional circulation model of the stratosphere, incorporating radiative heating and photochemistry of the oxygen‐hydrogen‐nitrogen atmosphere, is used to simulate the meridional distributions of O3, HOX, N2O,NOX, temperature and the three components of mean motion for the summer and winter seasons under steady‐state conditions. The results are generally in good agreement with the available observations in the normal stratosphere. The model has been applied to assess the effects of water vapour and nitrogen oxide perturbations resulting from aircraft emissions in the stratosphere. It is found that a fleet of 500 Boeing‐type sst's, flying at 20 km and 45°N in the summer hemisphere and inserting NOx at a rate of 1.8 megatons per year, has the effect of reducing the global total ozone by 14.7%. Similar calculations for 342 Concorde/TU‐114's, cruising at 17 km and injecting NOx at a rate of 0.35 megatons per year, show a global‐average total‐ozone reduction of 1.85%. Although water vapour is considered important, because of its ability to convert NO2 into HNO3, the direct effect on global‐average total‐ozone reduction resulting from the 100% increase in the stratospheric water content is less than 1%. The changes in the chemical structure (HO^NO^), temperature, and mean motions associated with the ozone reduction are also investigated in the case of the 1.8‐megaton‐per‐year NOX perturbation. It is shown that the reduced meridional temperature gradient in the middle and upper stratosphere resulting from the NOx perturbation leads to the weakening of the tropical easterly jet in the summer hemisphere and mid‐latitude westerlies in the winter season.

The sensitivity of the model solutions to an alternate choice of input parameters (diffusion coefficients and solar photodissociation data) is tested and the main deficiency of the model is pointed out.  相似文献   

5.
Summary In this paper we briefly describe the characteristics and the performance of our 1-D Muenster Climate Model. The model system consists of coupled models including gas cycle models, an energy balance model and a sea level rise model. The chemical feedback mechanisms among greenhouse gases are not included. This model, which is a scientifically-based parameterized simulation model, is used here primarily to help assess the effectiveness of various plausible policy options in mitigating the additional man-made greenhouse warming and the resulting sea level rise.For setting priorities it is important to assess the effectiveness of the various measures by which the greenhouse effect can be reduced. To this end we take a Scenario Business-as-Usual as a reference case (Leggett et al., 1992) and study the mitigating effects of the following four packages of measures: The Copenhagen Agreements on CFC, HCFC, and halon reduction (GECR, 1992), the Tropical Forest Preservation Plan of the Climate Enquete-Commission of the German Parliament on CO2 reduction (ECGP, 1990), a detailed reduction scheme for energy-related CO2 (ECGP, 1990), and a preliminary scheme for CH4, CO, and N2O reduction (Bach and Jain, 1992–1993).The required reduction depends, among others, on the desired climate and ecosystem protection. This is defined by the Enquete-Commission and others as a mean global rate of surface temperature change of ca. 0.1 °C per decade — assumed to be critical to many ecosystems — and a mean global warming ceiling of ca. 2 °C in 2100 relative to 1860.Our results show that the Copenhagen Agreements, the Tropical Forest Preservation Plan, the energy-related CO2 reduction scheme, and the CH4 and N2O reduction schemes could mitigate the anthropogenic greenhouse warming by ca. 12%, 6%, 35%, and 9% respectively. Taken together, all four packages of measures could reduce the man-made greenhouse effect by more than 60% until 2100; i.e. over the climate sensitivity range 2.5 °C (1.5 to 4.5) for 2 × CO2, the warming could be reduced from 3.5 °C (2.4 to 5.0) without specific measures to 1.3 °C (0.9 to 2.0) with the above packages of measures; and likewise, the mean global sea level rise could be reduced from 65 cm (46 to 88) without specific measures to 32 cm (22 to 47) with the above measures.Finally, the model results also emphasize the importance of trace gases other than CO2 in mitigating additional man-made greenhouse warming. According to our preliminary estimates, CH4 could in the short term make a sizable contribution to the reduction of the greenhouse effect (because of its relatively short lifetime of 10 yr), as could N2O in the medium and long term (with a relatively long lifetime of 150 yr).With 7 Figures  相似文献   

6.
Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr3, CH2BrCl, CHBr2Cl, CHBrCl2, and CH2Br2) and CH3Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO x and NO x . Globally, the impact of bromine chemistry on tropospheric O3 is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O3 burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH3OOH, H2O2).  相似文献   

7.
A one-dimensional coupled climate and chemistry model has been developed to estimate past and possible future changes in atmospheric temperatures and chemical composition due to human activities. The model takes into account heat flux into the oceans and uses a new tropospheric temperature lapse rate formulation. As found in other studies, we estimate that the combined greenhouse effect of CH4, O3, CF2Cl2, CFCl3 and N2O in the future will be about as large as that of CO2. Our model calculates an increase in average global surface temperatures by about 0.6°C since the start of the industrial era and predicts for A.D. 2050 a twice as large additional rise. Substantial depletions of ozone in the upper stratosphere by between 25% and 55% are calculated, depending on scenario. Accompanying temperature changes are between 15°C and 25°C. Bromine compounds are found to be important, if no rigid international regulations on CFC emissions are effective. Our model may, however, concivably underestimate possible effects of CFCl3, CF2Cl2, C2F3Cl3 and other CFC and organic bromine emissions on lower stratospheric ozone, because it can not simulate the rapid breakdown of ozone which is now being observed worldwide. An uncertainty study regarding the photochemistry of stratospheric ozone, especially in the region below about 25 km, is included. We propose a reaction, involving excited molecular oxygen formation from ozone photolysis, as a possible solution to the problem of ozone concentrations calculated to be too low above 45 km. We also estimate that tropospheric ozone concentrations have grown strongly in the northern hemisphere since pre-industrial times and that further large increases may take place, especially if global emissions of NOx from fossil fuel and biomass burning were to continue to increase. Growing NOx emissions from aircraft may play an important role in ozone concentrations in the upper troposphere and low stratosphere.  相似文献   

8.
《大气与海洋》2013,51(4):283-299
Abstract

The Middle Atmosphere Nitrogen TRend Assessment (MANTRA) series of high‐altitude balloon flights is being undertaken to investigate changes in the concentrations of northern hemisphere mid‐latitude stratospheric ozone, and of nitrogen and chlorine compounds that play a role in ozone chemistry. Four campaigns have been carried out to date, all from Vanscoy, Saskatchewan, Canada (52°01'N, 107°02'W, 511.0 m). The first MANTRA mission took place in August 1998, with the balloon flight on 24 August 1998 being the first Canadian launch of a large high‐altitude balloon in about fifteen years. The balloon carried a payload of instruments to measure atmospheric composition, and made measurements from a float altitude of 32–38 km for one day. Three of these instruments had been flown on the Stratoprobe flights of the Atmospheric Environment Service (now the Meteorological Service of Canada) in the 1970s and early 1980s, providing a link to historical data predating the onset of mid‐latitude ozone loss.

The primary measurements obtained from the balloon‐borne instruments were vertical profiles of ozone, NO2, HNO3, HCl, CFC‐11, CFC‐12, N2O, CH4, temperature, and aerosol backscatter. Total column measurements of ozone, NO2, SO2, and aerosol optical depth were made by three ground‐based spectrometers deployed during the campaign. Regular ozonesonde and radiosonde launches were also conducted during the two weeks prior to the main launch in order to characterize the local atmospheric conditions (winds, pressure, temperature, humidity) in the vicinity of the primary balloon flight. The data have been compared with the Model for Evaluating oZONe Trends (MEZON) chemical transport model, the University of California at Irvine photochemical box model, and the Canadian Middle Atmosphere Model (CMAM) to test our current understanding of model photochemistry and mid‐latitude species correlations. This paper provides an overview of the MANTRA 1998 mission, and serves as an introduction to the accompanying papers in this issue of Atmosphere‐Ocean that describe specific aspects and results of this campaign.  相似文献   

9.
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   

10.
未来甲烷排放增加对平流层水汽和全球臭氧的影响   总被引：3，自引：0，他引：3  
利用一个耦合的大气化学-气候模式(WACCM3)研究了地表甲烷排放增加对平流层水汽和全球臭氧变化的影响.结果表明,如果地表甲烷的排放量在2000年的基础上增加50%(达到政府间气候变化专门委员会A1B排放情景中2050年的值),平流层水汽体积分数将平均增加约0.8×10-6.南半球平流层甲烷转化为水汽的效率比北半球高.在北半球平流层中,1mol甲烷分子可以转化为约1.63mol的水汽分子,而在南半球1mol甲烷分子大概可以转化为约1.82mol的水汽分子.甲烷排放增加50%将使全球中低纬度地区以及北半球高纬度地区的臭氧柱总量增加1%-3%,使南半球高纬度地区臭氧柱总量增加近8%,而秋季(南半球春季)南极地区臭氧柱总量增加幅度可高达20%,南极臭氧的这种显着增加主要是由于甲烷增加造成的化学反馈所致.在北半球中高纬度地区,甲烷增加引起的臭氧变化主要与甲烷氧化导致的水汽增加有关.研究还表明,未来甲烷排放增加对臭氧的恢复作用其实与溴化物排放的减少一样重要.  相似文献   

11.
Airborne measurements of stratospheric ozone and N2O from the SCIAMACHY (Scanning Imaging Absorption Spectrometer) Validation and Utilization Experiment (SCIA-VALUE) are presented. The campaign was conducted in September 2002 and February–March 2003. The Airborne Submillimeter Radiometer (ASUR) observed stratospheric constituents like O3 and N2O, among others, spanning a latitude from 5°S to 80°N during the survey. The tropical ozone source regions show high ozone volume mixing ratios (VMRs) of around 11 ppmv at 33 km altitude, and the altitude of the maximum VMR increases from the tropics to the Arctic. The N2O VMRs show the largest value of 325 ppbv in the lower stratosphere, indicating their tropospheric origin, and they decrease with increasing altitude and latitude due to photolysis. The sub-tropical and polar mixing barriers are well represented in the N2O measurements. The most striking seasonal difference found in the measurements is the large polar descent in February–March. The observed features are interpreted with the help of SLIMCAT and Bremen Chemical Transport Model (CTMB) simulations. The SLIMCAT simulations are in good agreement with the measured O3 and N2O values, where the differences are within 1 ppmv for O3 and 15 ppbv for N2O. However, the CTMB simulations underestimate the tropical middle stratospheric O3 (1–1.5 ppmv) and the tropical lower stratospheric N2O (15–30 ppbv) measurements. A detailed analysis with various measurements and model simulations suggests that the biases in the CTMB simulations are related to its parameterised chemistry schemes.  相似文献   

12.
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13.
Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1∘ × 1∘) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1∘ × 1∘ provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO3, N2O, and NO y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10−3 to 10−2 cm−3) refines the agreement with in situ ozone, N2O and NO y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl2O2 absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl2O2 absorption cross-sections.  相似文献   

14.
Methyl Chloride (CH3Cl) is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion (Carpenter et al. 2014). In the global CH3Cl budget, the atmospheric CH3Cl emissions is predominantly maintained by natural sources, of which magnitudes have been relatively well-constrained. However, significant uncertainties still remain in the CH3Cl emission strengths from anthropogenic sources. High-frequency and high-precision in situ measurements of atmospheric CH3Cl concentrations obtained since 2008 at Gosan station (a remote background site in the East Asia) reveal significant pollution events superimposed on the seasonally varying regional background levels. Back trajectory statistics showed that air masses corresponding to the observed CH3Cl enhancement largely originated from regions of intensive industrial activities in China. Based on an inter-species correlation method, estimates of CH3Cl emissions from manufacturing industries including coal combustion, use of feedstocks, or process agents in chemical production for China (2008–2012) are 297 ± 71 Gg yr.?1 in 2008 to 480 ± 99 Gg yr.?1 in 2009, followed by a gradual decrease of about 25% between 2009 and 2012 (398 ± 92 Gg yr.?1 for 2010; 286 ± 68 Gg yr.?1 for 2011; 358 ± 92 Gg yr.?1 for 2012). The annual average of industrial CH3Cl emissions for 2008–2012 (363 ± 85 Gg yr.?1) in China is comparable to the known total global anthropogenic CH3Cl emissions accounting only for coal combustion and indoor biofuel use. This may suggest that unless emissions from the chemical industry are accounted for, global anthropogenic emissions of CH3Cl have been substantially underestimated. In particular, since industrial production and use of CH3Cl have not been regulated under the Montreal Protocol (MP) or its successor amendments, continuous monitoring of Chinese CH3Cl outflow is important to properly evaluate its anthropogenic emissions.  相似文献   

15.
Summary A coupled 1-D time-dependent radiative-convective-photochemical diffusion model which extends from the surface to 60 km is used to investigate the potential impact of greenhouse trace gas emissions on long-term changes in global climate, atmospheric ozone and surface UV-B radiation, taking into accoont the influence of aerosol loading into the atmosphere from major volcanic eruptions, of thermal inertia of the upper mixed layer of the ocean and of other radiativephotochemical feedback mechanisms. Experiments are carried out under global and annual average insolation and cloudiness conditions. The transient calculations are made for three different growth scenarios for increase in trace gas concentrations. Scenario 1, which begins in 1850, uses the best estimate values for future trace gas concentrations of CO2, CH4, N2O, CFC-11, CFC-12 and tropospheric O3, based on current observational trends. Scenarios 2 and 3, which begin in 1990, assume lower and upper ranges, respectively, of observed growth rates to estimate future concentrations.The transient response of the model for Scenario 1 suggests that surface warming of the ocean mixed layer of about 1 K should have taken place between 1850 and 1990 due to a combined increase of atmospheric CO2 and other trace gases. For the three scenarios considered in this study, the cumulative surface warming induced by all major trace gases for the period 1850 to 2080 ranges from 2.7 K to 8.2 K with the best estimate value of 5 K. The results indicate that the direct and the indirect chemistry-climate interactions of non-CO2 trace gases contribute significantly to the cumulative surface warming (up to 65% by the year 2080). The thermal inertia of a mixed layer of the ocean is shown to have the effect of delaying equilibrium surface warming by almost three decades with an e-folding time of about 5 years. The volcanic aerosols which would result from major volcanic eruptions play a significant role by interrupting the long-term greenhouse surface warming trend and replacing it by a temporary cooling on a time scale of a decade or less. Furthermore, depending on the scenario used, a reduction in the net ozone column could result in an increase in the solar UV-B radiation at the surface by as much as 300% towards the end of 21st century.With 14 Figures  相似文献   

16.
This paper provides estimates of emissions of two important but often not well-characterized greenhouse gas (GHG) emissions related to transportation energy use: methane (CH4) and nitrous oxide (N2O). The paper focuses on emissions of CH4 and N2O from motor vehicles because unlike emissions of CO2, which are relatively easy to estimate, emissions of CH4 and N2O are a function of many complex aspects of combustion dynamics and of the type of emission control systems used. They therefore cannot be derived easily and instead must be determined through the use of published emission factors for each combination of fuel, end-use technology, combustion conditions, and emission control system. Furthermore, emissions of CH4 and N2O may be particularly important with regard to the relative CO2-equivalent GHG emissions of the use of alternative transportation fuels, in comparison with the use of conventional fuels. By analyzing a database of emission estimates, we develop emission factors for N2O and CH4 from conventional vehicles, in order to supplement recent EPA and IPCC estimates, and we estimate relative emissions of N2O and CH4 from different alternative fuel passenger cars, light-duty trucks, and heavy-duty vehicles.  相似文献   

17.
Nitrogen compounds are produced by biological reactions and by industrial processes from the abundant nitrogen gas (N2) in the atmosphere. The formation of compounds from atmospheric nitrogen is called fixation. In nature, nitrogen compounds undergo many conversions, but under aerobic conditions, characterized by the presence of oxygen, they tend to be converted to the nitrate (NO 3 - ) form. Under anaerobic conditions, characterized by the absence of oxygen, the nitrate is denitrified, and the nitrogen contained therein is converted into nitrogen gas (N2) and nitrous oxide (N2O), which escape into the atmosphere. The nitrous oxide diffuses into the stratosphere, where it decomposes to yield nitrogen gas and small amounts of nitric oxide (NO) and nitrogen dioxide (NO2), which react with ozone (O3) to convert it to oxygen (O2). The ozone in the stratosphere is produced by the reaction of light with oxygen and is destroyed primarily by reactions with the nitrogen oxides.As long as the production and destruction are equal, the ozone in the stratosphere is maintained at a constant concentration. Increased nitrogen fixation will lead to increased denitrification, increased amount of nitrous oxide moving into the stratosphere, and a reduction in ozone concentration.Ozone in the stratosphere attenuates the ultraviolet light received from the sun. As the ozone concentration decreases, more ultraviolet light will reach the surface of the earth. The fear is that this additional radiation will have detrimental effects on living organisms and possibly on the climate.Because the global use of fixed nitrogen in fertilizers has increased greatly in recent years and in 1974 amounted to almost 40 million metric tons, the eventual generation of nitrous oxide from the fertilizer nitrogen after application to the soil has been cited as a potential environmental hazard. In response to this concern, this document estimates nitrogen fixation, nitrous oxide production, and ozone reduction based on two methods of calculation and on various increases in nitrogen fixation. Uncertainties and information gaps in the nitrogen cycle are pointed out.This document does not review either the projected biological effects of ozone depletion or the stratospheric chemistry of ozone. These topics are dealt with at length in other studies.World fixation of nitrogen in 1974, expressed in millions of metric tons per year (MT/yr), was estimated to be as follows.Most of the estimates given are based on inadequate data; consequently, actual amounts may be significantly different from those shown. The study of nitrogen fixed in the oceans has not progressed far enough to permit reliable estimates. However, estimates of the amount of nitrogen fixed for fertilizer and other industrial uses in 1974 are considered reliable. The trend of industrial fixation of nitrogen offers some indication of the trend in total amount of nitrogen fixed. It is estimated that 174 MT of nitrogen were fixed by all processes in 1950. Total fixation in 1850 could have been 150 MT of nitrogen.Nitrous oxide-nitrogen production on land is estimated as 5 to 10 MT/yr; published estimates of production in the ocean, however, range from less than 1 to 100 MT/yr. The higher value was based on reported supersaturation of ocean waters with nitrous oxide.Two methods of estimating the decrease in ozone concentration in the stratosphere were used. Method I is based on nitrogen fixation. It involves the assumptions that the relative increase in production of nitrous oxide is proportional to the relative increase in total nitrogen fixation and that sufficient time has elapsed for the rate of denitrification to come to equilibrium with fixation; i.e., the lag time between increased fixation and increased denitrification has passed. This method, using fixation estimated for 1950 as a base, suggests that the reduction in ozone would be 5.8 and 11.5% as a consequence of increased fixation of 50 and 100 MT of nitrogen per year, respectively.Method II is based on nitrous oxide evolution. It involves the assumption that the global rate of production of nitrous oxide is 100 MT/yr (based on supersaturation of this gas in the ocean and on changes in measured concentrations of nitrous oxide in the atmosphere). Method II leads to estimates of ozone reduction much lower than those from Method I. For example, on the assumption that global production of nitrous oxide-nitrogen is 100 MT/yr and that 5% of the nitrogen denitrified is released as nitrous oxide, the estimated ozone reduction is 1% with an increase of 100 MT/yr in nitrogen fixation. This method is forced to assume an unknown source of nitrous oxide in the ocean and an unknown sink for nitrous oxide in the troposphere.There are great uncertainties in many of the estimates that have been made for nitrogen fixation and for nitrous oxide production, and there are many information gaps that need to be filled before the question of the effects of increased nitrogen fixation on the ozone layer can be answered. Perhaps the biggest information needs are in the areas of nitrogen transformations and the quantities of nitrous oxide produced in the ocean. Other needs deal with the complexities of the nitrogen cycle on land. The lag time between fixation by various processes and denitrification must be known as a basis for estimating how soon predicted effects based on equilibrium conditions can be expected. Concentrations of nitrous oxide and their fluctuations in the troposphere (lower atmosphere) need to be monitored to provide an index to variations and increases in production. Improved models are needed to relate the ozone concentration in the stratosphere to nitrogen fixation and nitrous oxide production on earth.In spite of the uncertainties in the predictions of the effects of increased fixation of nitrogen on stratospheric ozone, the potential hazard is sufficiently serious that, in addition to research on the various phases of the global nitrogen cycle that impinge upon the nitrous oxide-ozone question, research on the efficiency of use of all fixed forms of nitrogen should be worthwhile. Editor's Note: Although the data for sources, sinks, reservoirs, and rate processes in this article are undergoing rapid revision presently, it, nonetheless, is one of the clearest statements of the physics, chemistry, and biology of the fertilizer/ozone problem available to date.This report was developed by eleven scientists (see Appendix 1 for names and affiliations) representing the subject matter areas of atmospheric chemistry, chemical engineering, environmental science and chemistry, microbiology, oceanography, plant genetics, soil biochemistry, soil physics, and soil chemistry. This task force of scientists chaired by Parker F. Pratt, met under the auspices of the Council for Agricultural Science and Technology (CAST), whose headquarters office is at the Department of Agronomy, Iowa State University, Ames, Iowa 50011, U.S.A. The task force met in Denver, Colorado from October 23 to 25, 1975, to prepare a first draft of the report. The chairman then prepared a revised version and returned it to members of the task force for review and comment. A second revision was then prepared and returned for further comment. Finally, the report was edited and reproduced for transmittal through the U.S. Congressional Committees concerned with the matter of ozone depletion. It was originally issued as a CAST Report Number 53, January, 1976, but had not been formally published heretofore.  相似文献   

18.
The MAGICC (Model for the Assessment of Greenhouse gas Induced Climate Change) model simulation has been carried out for the 2000–2100 period to investigate the impacts of future Indian greenhouse gas emission scenarios on the atmospheric concentrations of carbon dioxide, methane and nitrous oxide besides other parameters like radiative forcing and temperature. For this purpose, the default global GHG (Greenhouse Gases) inventory was modified by incorporation of Indian GHG emission inventories which have been developed using three different approaches namely (a) Business-As-Usual (BAU) approach, (b) Best Case Scenario (BCS) approach and (c) Economy approach (involving the country’s GDP). The model outputs obtained using these modified GHG inventories are compared with various default model scenarios such as A1B, A2, B1, B2 scenarios of AIM (Asia-Pacific Integrated Model) and P50 scenario (median of 35 scenarios given in MAGICC). The differences in the range of output values for the default case scenarios (i.e., using the GHG inventories built into the model) vis-à-vis modified approach which incorporated India-specific emission inventories for AIM and P50 are quite appreciable for most of the modeled parameters. A reduction of 7% and 9% in global carbon dioxide (CO2) emissions has been observed respectively for the years 2050 and 2100. Global methane (CH4) and global nitrous oxide (N2O) emissions indicate a reduction of 13% and 15% respectively for 2100. Correspondingly, global concentrations of CO2, CH4 and N2O are estimated to reduce by about 4%, 4% and 1% respectively. Radiative forcing of CO2, CH4 and N2O indicate reductions of 6%, 14% and 4% respectively for the year 2100. Global annual mean temperature change (incorporating aerosol effects) gets reduced by 4% in 2100. Global annual mean temperature change reduces by 5% in 2100 when aerosol effects have been excluded. In addition to the above, the Indian contributions in global CO2, CH4 and N2O emissions have also been assessed by India Excluded (IE) scenario. Indian contribution in global CO2 emissions was observed in the range of 10%–26%, 6%–36% and 10%–38% respectively for BCS, Economy and BAU approaches, for the years 2020, 2050 and 2100 for P50, A1B-AIM, A2-AIM, B1-AIM & B2-AIM scenarios. CH4 and N2O emissions indicate about 4%–10% and 2%–3% contributions respectively in the global CH4 and N2O emissions for the years 2020, 2050 and 2100. These Indian GHG emissions have significant influence on global GHG concentrations and consequently on climate parameters like RF and ∆T. The study reflects not only the importance of Indian emissions in the global context but also underlines the need of incorporation of country specific GHG emissions in modeling to reduce uncertainties in simulation of climate change parameters.  相似文献   

19.
采用漂浮通量箱法和扩散模型法同步地观测了模拟内陆水体在不同条件下的CH4和N2O的水-气交换通量,旨在比较两类方法取得结果的异同。结果显示:这两类方法所测得的绝大多数CH4排放通量都与水中溶解氧呈显著线性负相关(显著性系数P0.001)。同时N2O排放通量与表层水温及水中铵态氮、硝态氮、溶解碳和溶解氧的关系可用包含所有上述水环境因素的Arrhenius动力学方程来表达,这些因素可以共同解释86%~90%的N2O通量变化(P0.0001),且不同方法测定的N2O通量的表观活化能和对表层水温的敏感系数分别介于47~59 kJ mol-1和1.92~2.27之间;扩散模型法所获得的CH4和N2O通量分别是箱法测定值的13%~175%和15%~240%,差异程度因模型而异;不同模型取得通量间相差20%~1200%,平均相差2.3倍。上述结果表明:仅用一种模型方法来取得CH4或N2O排放通量易形成较大偏差;不同扩散模型法和箱法测定的通量在反映CH4和N2O排放的内在规律方面具有一致性,但它们对真实气体通量的测量是否都存在不同程度的系统误差,尚需进一步研究。  相似文献   

20.
Anthropogenic emissions of methane (CH4) and nitrous oxide (N2O) from livestock agriculture (enteric fermentation, animal waste management systems, and pasture manure) and plant growing of the Russia (CH4 emissions from rice fields, direct and indirect N2O emissions from agricultural lands) are considered. In 2004, the total emissions of these greenhouse gases in the agricultural sector amounted to 1.4 × 105 thousand t CO2-equivalent, which corresponds to 45% of the 1990 level (3.1 × 105 thousand t CO2-equivalent). In 2004, the contribution of N2O to the total agricultural emissions was approximately twice (67.0%) that of CH4 (33.0%). Direct N2O emissions from agricultural soils (0.5 × 105 thousand t CO2-equivalent) and CH4 emissions from the internal fermentation of domestic animals (0.4 × 105 thousand t CO2-equivalent) are the most significant sources in the agricultural sector of the Russian Federation. In 2004, all these agricultural sources emitting methane and nitrous oxide contributed about 7% CO2-equivalent to the total emission of the anthropogenic greenhouse gases in Russia.  相似文献   

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