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1.
张仁健 《气象学报》2002,60(5):620-624
应用作者建立的全球二维大气化学模式 ,采用 2种CH4 排放源的长期增长方案 ,同时考虑了CH4 排放源以及对OH自由基浓度有重要影响的CO和NOx 排放源的长期变化 ,模拟了CH4 和OH从 1840～ 2 0 2 0年的长期变化趋势。考虑了世界人口增长的排放源方案可以更好地模拟CH4 的长期变化 ,模拟结果表明 ,工业革命前的大气CH4 浓度和年排放总量分别为 76 0× 10 -9(V/V)和 2 80× 10 9kg ,1991年大气CH4 的浓度和年排放总量分别为16 11.9× 10 -9(V/V)和 5 33 .9× 10 9kg ,对流层OH自由基数浓度从 1840年的 7.17× 10 5分子数 /cm3 下降到 1991年的 5 .79× 10 5分子数 /cm3,降低了 19%。工业革命以来大气CH4 的增长一方面是由于CH4 排放源的增长 ,另一方面是由于大气OH浓度的下降。  相似文献   

2.
应用初步建立的全球二维大气化学模式,对工业革命以来甲烷的长期变化进行了模拟研究。模式将CH4、CO和NOx排放源方案进行了参数化。在考虑了CH4排放源以及对OH浓度有重要影响的CO和NOx排放源的长期变化的基础上,模拟了CH4和OH浓度自1840年到20世纪90年代的长期变化趋势。结果表明,工业革命前的大气甲烷体积分数和年排放总量分别为760×10-9和280Tg,1991年大气甲烷的体积分数和年排放总量分别为1611.9×10-9和533.9Tg。而对流层中OH的数密度则由1840年的7.17×105cm-3变化到1991年的5.79×105cm-3,下降了19%。如果CH4、CO及NOx这三种排放源继续按给定的方案增长,那么到2020年大气甲烷的体积分数和年排放总量将增加为2090.7×10-9和966.2Tg,而OH的数密度将为5.47×105cm-3,比1840年降低24%。  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.
Atmospheric hydroxyl (OH), hydroperoxy (HO2), total peroxy (HO2 and organic peroxy radicals, RO2) mixing ratios and OH reactivity (first order OH loss rate) were measured at a rural site in central Pennsylvania during May and June 2002. OH and HO2 mixing ratios were measured with laser induced fluorescence (LIF); HO2 + RO2 mixing ratios were measured with chemical ionization mass spectrometry (CIMS). The daytime maximum mixing ratios were up to 0.6 parts per trillion by volume (pptv) for OH, 30 pptv for HO2, and 45 pptv for HO2 + RO2. A parameterized RACM (Regional Atmospheric Chemistry Mechanism) box model was used to predict steady state OH, HO2 and HO2 + RO2 concentrations by constraining the model to the measured OH reactivity and previously measured volatile organic compound (VOC) distributions. The averaged model calculations are generally in good agreement with the observations. For OH, the model matched the observations for day and night, with an average observed-to-modeled ratio of 0.80. In previous studies such as PROPHET98, nighttime NO was near 0 pptv and observed nighttime OH was significantly larger than modeled OH. In this study, nighttime observed and modeled OH agree to within measurement and model uncertainties because the main source of the nighttime OH was the reaction HO2 + NO → OH + NO2, with the NO being continually emitted from the surrounding fertilized corn field. The observed-to-modeled ratio for HO2 is 1.0 on average, although daytime HO2 is underpredicted by a factor of 1.2 and nighttime HO2 is over-predicted by a factor of ∼2. The average measured and modeled HO2 + RO2 agree well during daytime, but the modeled value is about twice the measured value during nighttime. While measured HO2 + RO2 values agree with modeled values for NO mixing ratios less than a few parts per billion by volume (ppbv), it increases substantially above the expected value for NO greater than a few ppbv. This observation of the higher-than-expected HO2 + RO2 with the CIMS technique confirms the observed increase of HO2 above expected values at higher NO mixing ratios in HO2 measurements with the LIF technique. The maximum instantaneous O3 production rate calculated from HO2 and RO2 reactions with NO was as high as 10–15 ppb h−1 at midday; the total daily O3 production varied from 13 to 113 ppbv d−1 and was 48 ppbv d−1 on average during this campaign.  相似文献   

5.
A two-dimensional global chemistry model is developed to study the distribution and long-term trends of methane. The model contains 34 species and 104 chemical and photochemical reactions. Using the model, the long-term trends of CH4, CO and OH in atmosphere are simulated, comparison between the model and observations shows that the simulation is successful. Experiments are done to investigate the causes of dramatic decrease in the growth rate of CH4 in 1992 such as OH increase due to stratospheric ozone depletion, decrease of temperature in the troposphere due to Mount Pinatubo eruption and descendent of CH4 sources fluxes. A new explanation is proposed and verified by this model that the decrease of CO emission plays an important role for the abnormal growth rate of CH4 in 1992. We find that the decreases of CH4 and CO emissions are the main reasons for the sudden decrease of growth rate of CH4 in 1992, which account for 73% and 27% respectively.  相似文献   

6.
杨栋  申双和  张弥  李旭辉  肖薇 《气象科学》2014,34(3):325-334
目前温室气体清单的编制主要基于IPCC方法,该方法用于特定城市或区域清单编制时可能会引起较大的不确定性,而目前对城市/区域尺度清单的不确定性的分析还存在很大的欠缺。本文通过南京市和长三角温室气体排放因子甄选,应用IPCC方法计算了2009年南京市和长三角的人为温室气体排放量,并以其为个例利用蒙特卡洛方法开展城市和区域尺度的温室气体人为排放清单不确定性的初步探究。研究结果表明:南京市CH4和CO2排放量的95%的概率分布范围分别为(1.08~1.86)×105t和(6.50~7.41)×107t,不确定性分别为-21.74%~34.78%和-7.01%~5.87%;长三角CH4和CO2排放量的95%的概率分布范围分别为(4.07~5.89)×106t和(1.62~1.82)×109t,不确定性分别为-15.60%~22.24%和-6.04%~5.34%。  相似文献   

7.
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   

8.
Ocean emissions of inorganic and organic iodine compounds drive the biogeochemical cycle of iodine and produce reactive ozone-destroying iodine radicals that influence the oxidizing capacity of the atmosphere. Di-iodomethane (CH2I2) and chloro-iodomethane (CH2ICl) are the two most important organic iodine precursors in the marine boundary layer. Ship-borne measurements made during the TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOC) field campaign in the east tropical Pacific Ocean in January/February 2012 revealed strong diurnal cycles of CH2I2 and CH2ICl in air and of CH2I2 in seawater. Both compounds are known to undergo rapid photolysis during the day, but models assume no night-time atmospheric losses. Surprisingly, the diurnal cycle of CH2I2 was lower in amplitude than that of CH2ICl, despite its faster photolysis rate. We speculate that night-time loss of CH2I2 occurs due to reaction with NO3 radicals. Indirect results from a laboratory study under ambient atmospheric boundary layer conditions indicate a k CH2I2+NO3 of ≤4 × 10?13 cm3 molecule?1 s?1; a previous kinetic study carried out at ≤100 Torr found k CH2I2+NO3 of 4 × 10?13 cm3 molecule?1 s?1. Using the 1-dimensional atmospheric THAMO model driven by sea-air fluxes calculated from the seawater and air measurements (averaging 1.8 +/? 0.8 nmol m?2 d?1 for CH2I2 and 3.7 +/? 0.8 nmol m?2 d?1 for CH2ICl), we show that the model overestimates night-time CH2I2 by >60 % but reaches good agreement with the measurements when the CH2I2 + NO3 reaction is included at 2–4 × 10?13 cm3 molecule?1 s?1. We conclude that the reaction has a significant effect on CH2I2 and helps reconcile observed and modeled concentrations. We recommend further direct measurements of this reaction under atmospheric conditions, including of product branching ratios.  相似文献   

9.
A new version of an atmospheric pressure chemical ionisation mass spectrometer has been developed for ground based in situ atmospheric measurements of OH and total peroxy (HO2 + organic peroxy) radicals. Based on the previously developed principle of chemical conversion of OH radicals to H2SO4 in reaction with SO2 and detection of H2SO4 using an ion molecule reaction with NO3─, the new instrument is equipped with a turbulent chemical conversion reactor allowing for measurements in moderately polluted atmosphere at NO concentrations up to several ppb. Unlike other similar devices, where the primary NO3─ ions are produced using radioactive ion sources, the new instrument is equipped with a specially developed corona discharge ion source. According to laboratory measurements, the overall accuracy and detection limits are estimated to be, respectively, 25% and 2 × 105 molecule cm-3 for OH and 30% and 1 × 105 molecule cm-3 for HO2 at 10 min integration times. The detection limit for measurements of OH radicals under polluted conditions is 5 × 105 molecules cm-3 at 10 min integration times. Examples of ambient air measurements during a field campaign near Paris in July 2007 are presented demonstrating the capability of the new instrument, although with reduced performance due to the employment of non isotopic SO2.  相似文献   

10.
Summary  Measurements of landscape-scale methane emission were made over an aapa mire near Kaamanen in Finnish Lapland (69° 8′ N, 27° 16′ E, 155 m ASL). Emissions were measured during the spring thaw, in summer and in autumn. No effect of water table position on CH4 emission was found as the water table remained at or above the surface of the peat. Methane emission fluxes increased with surface temperature from which an activation energy of −99 kJ mol−1 was obtained. Annual emission from the site, modelled from temperature regression and short-term flux measurements made in three separate years, was calculated to be 5.5 ± 0.4 g CH4 m−2 y−1 of which 0.6 ± 0.1 g CH4 m−2 y−1 (11%) was released during the spring thaw which lasted 20 to 30 days. The effect of global warming on the CH4 budget of the site was estimated using the central scenario of the SILMU (Finnish Research Programme on Climate Change) model which predicts annual mean temperature increases of 1.2, 2.4 and 4.4 °C in 2020, 2050 and 2100, respectively. Maximum enhancements in CH4 emission due to warming were calculated to be 18, 40 and 84% for 2020, 2050 and 2100, respectively. Actual increases may be smaller because prediction of changes in water table are highly uncertain. Received September 17, 1999 Revised October 16, 2000  相似文献   

11.
In recent studies, proxy XCH4 retrievals from the Japanese Greenhouse gases Observing SATellite (GOSAT) have been used to constrain top-down estimation of CH4 emissions. Still, the resulting interannual variations often show significant discrepancies over some of the most important CH4 source regions, such as China and Tropical South America, by causes yet to be determined. This study compares monthly CH4 flux estimates from two parallel assimilations of GOSAT XCH4 retrievals from 2010 to 2019 based on the same Ensemble Kalman Filter (EnKF) framework but with the global chemistry transport model (GEOS-Chem v12.5) being run at two different spatial resolutions of 4° × 5° (R4, lon × lat) and 2° × 2.5° (R2, lon × lat) to investigate the effects of resolution-related model errors on the derived long-term global and regional CH4 emission trends. We found that the mean annual global methane emission for the 2010s is 573.04 Tg yr –1 for the inversion using the R4 model, which becomes about 4.4 Tg yr –1 less (568.63 Tg yr –1) when a finer R2 model is used, though both are well within the ensemble range of the 22 top-down results (2008–17) included in the current Global Carbon Project (from 550 Tg yr –1 to 594 Tg yr –1). Compared to the R2 model, the inversion based on the R4 tends to overestimate tropical emissions (by 13.3 Tg yr –1), which is accompanied by a general underestimation (by 8.9 Tg yr –1) in the extratropics. Such a dipole reflects differences in tropical–mid-latitude air exchange in relation to the model’s convective and advective schemes at different resolutions. The two inversions show a rather consistent long-term CH4 emission trend at the global scale and over most of the continents, suggesting that the observed rapid increase in atmospheric methane can largely be attributed to the emission growth from North Africa (1.79 Tg yr –2 for R4 and 1.29 Tg yr –2 for R2) and South America Temperate (1.08 Tg yr –2 for R4 and 1.21 Tg yr –2 for R2) during the first half of the 2010s, and from Eurasia Boreal (1.46 Tg yr –2 for R4 and 1.63 Tg yr –2 for R2) and Tropical South America (1.72 Tg yr–2 for R4 and 1.43 Tg yr –2 for R2) over 2015–19. In the meantime, emissions in Europe have shown a consistent decrease over the past decade. However, the growth rates by the two parallel inversions show significant discrepancies over Eurasia Temperate, South America Temperate, and South Africa, which are also the places where recent GOSAT inversions usually disagree with one other.  相似文献   

12.
Changes in methane emissions into the atmosphere from terrestrial ecosystems are assessed with models for the European and Asian parts of Russia using the model unit of a methane cycle and calculations with a regional climate model. The calculations were performed for the present-day base period (1991–2000), for the middle (2041–2050), and late (2091–2100) 21st century using the SRES A2 anthropogenic emission scenario. The average emissions for the base period were equal to 8 Mt CH4/year for the European part of Russia and 10 Mt CH4/year for the Asian part. By the middle of the 21st century, they increased up to 11 and 13 Mt CH4/year, and by the late 21st century, up to 14 and 17 Mt CH4/year. These tendencies are associated with the increased warm period of the soil and dependence of the integral methane production on temperature. It is predicted that the maximum depth of freezing will lessen in the southern regions of the European and Asian parts of Russia by the late 21st century.  相似文献   

13.
Using long path UV absorption spectroscopy we have measured OH concentrations close to the earth's surface. The OH values observed at two locations in Germany during 1980 through 1983 range from 0.7×106 to 3.2×106 cm-3. Simultaneously we measured the concentrations of O3, H2O, NO, NO2, CH4, CO, and the light non methane hydrocarbons. We also determined the photolysis rates of O3 and NO2. This allows calculations of OH using a zero dimensional time depdendent model. The modelled OH concentrations significantly exceed the measured values for low NO x concentrations. It is argued that additional, so far unidentified. HO x loss reactions must be responsible for that discrepancy.  相似文献   

14.
At the atmosphere simulation chamber SAPHIR in Jülich both Laser-Induced Fluorescence Spectroscopy (LIF) and Long-Path Differential Optical Laser Absorption Spectroscopy (DOAS) are operational for the detection of OH radicals at tropospheric levels. The two different spectroscopic techniques were compared within the controlled environment of SAPHIR based on all simultaneous measurements acquired in 2003 (13 days). Hydroxyl radicals were scavenged by added CO during four of these days in order to experimentally check the calculated precisions at the detection limit. LIF measurements have a higher precision (σ= 0.88×106 cm–3) and better time resolution (Δt = 60 s), but the DOAS method (σ= 1.24×106 cm–3, Δt = 135 s) is regarded as primary standard for comparisons because of its good accuracy. A high correlation coefficient of r = 0.95 was found for the whole data set highlighting the advantage of using a simulation chamber. The data set consists of two groups. The first one includes 3 days, where the LIF measurements yield (1 – 2) ×106 cm–3 higher OH concentrations than observed by the DOAS instrument. The experimental conditions during these days are characterized by increased NOx concentration and a small dynamic range in OH. Excellent agreement is found within the other group of 6 days. The regression to the combined data of this large group yields unity slope without a significant offset.  相似文献   

15.
Presented is a detailed comparison of CH4 and δ13C–CH4 measurements with simulations of the global transport model TM3. Experimental data were obtained during campaigns along the Trans-Siberian railroad in the framework of the TROICA project. Two summer (1999 and 2001) and one spring (2003) expeditions are evaluated. Model simulations include sensitivity tests to further investigate the isotopic composition of natural gas and emissions from Siberian wetlands. Comparison of the average mixing ratio of methane and its isotopic composition (δ13C) has been performed for different geographic zones, including the European part of Russia, Western Siberia and Central Siberia. Simulations are in reasonable agreement with the measurements for the European part of Russia and confirm a high contribution of natural gas to the observed methane levels. An increase of emission from bogs shifts the simulated methane isotopic composition closer to the observations. The relative importance of the Western Siberia emissions in current inventories is underestimated in comparison with other wetland regions in the former USSR. Simulated average mixing ratios are in a good agreement with the observations in Central Siberia, while 13C(CH4) values tend to be higher than measured in all considered scenarios. These results point to a bias in the modeled source mixture over Russia, which could be repaired by shifting emissions from isotopically heavy methane sources (e.g. coal, oil or biomass burning) to light sources (e.g. wetlands, ruminants, waste treatment). Alternatively, the average isotopic signature of Siberian wetlands may be lighter than expected.  相似文献   

16.
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   

17.
In the present study, an attempt has been made to examine the governing photochemical processes of surface ozone (O3) formation in rural site. For this purpose, measurements of surface ozone and selected meteorological parameters have been made at Anantapur (14.62°N, 77.65°E, 331 m asl), a semi-arid zone in India from January 2002 to December 2003. The annual average diurnal variation of O3 shows maximum concentration 46 ppbv at noon and minimum 25 ppbv in the morning with 1σ standard deviation. The average seasonal variation of ozone mixing ratios are observed to be maximum (about 60 ppbv) during summer and minimum (about 22 ppbv) in the monsoon period. The monthly daytime and nighttime average surface ozone concentration shows a maximum (55 ± 7 ppbv; 37 ± 7.3 ppbv) in March and minimum (28 ± 3.4 ppbv; 22 ± 2.3 ppbv) in August during the study period. The monthly average high (low) O3 48.9 ± 7.7 ppbv (26.2 ± 3.5 ppbv) observed at noon in March (August) is due to the possible increase in precursor gas concentration by anthropogenic activity and the influence of meteorological parameters. The rate of increase of surface ozone is high (1.52 ppbv/h) in March and lower (0.40 ppbv/h) in July. The average rate of increase of O3 from midnight to midday is 1 ppbv/h. Surface temperature is highest (43–44°C) during March and April months leading to higher photochemical production. On the other hand, relative humidity, which is higher during the rainy season, shows negative correlation with temperature and ozone mixing ratio. It can be seen that among the two parameters are measured, correlation of surface ozone with wind speed is better (R 2=0.84) in compare with relative humidity (R 2=0.66).  相似文献   

18.
The aqueous phase acid-catalyzed reaction of methanol (CH3OH) with nitric acid (HNO3) to yield methyl nitrate (CH3ONO2) under atmospheric conditions has been investigated using gas-phase infrared spectroscopy. Reactions were conducted in aqueous sulfuric acid solutions (50.5–63.6 wt.%) with [CH3OH] = 0.00005–0.005 M and [HNO3] = 0.02–0.21 M, at 278.2–328.6 K. Methyl nitrate production rates increased linearly with CH3OH and HNO3 concentrations and exponentially with sulfuric acid weight percent within the regime studied. Rates increased linearly with nitronium ion concentration, indicating that the reaction involves as the nitrating agent under these conditions. At 298 K, the rate of methyl nitrate production can be calculated from k obs [CH3OH][HNO3], where k obs  = 2.337 × 10−13(exp(0.3198*wt.% H2SO4)) when the solubility of CH3ONO2 in acidic solution is approximated by H* for pure water. The temperature dependence of the rate coefficient is related to solution composition, with activation energies of 59 and 49 kJ/mol at 51.1 and 63.6 wt.% H2SO4, respectively, when k is calculated from rate. The temperature dependence has also been parameterized for application to the atmosphere, but the small quantities of present in aerosol particles will result in methyl nitrate production rates too small to be of significance under most atmospheric conditions. An erratum to this article can be found at  相似文献   

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

20.
The surface level measurements of O3, CO, CH4 and light NMHCs were made at eight different rural sites in the central part of India during February, 2004. The online analyzer was used for in-situ measurement of O3 while air samples were collected for the analyses of CO, CH4 and NMHCs using the gas chromatography techniques. The average mixing ratios of O3, which were in the range of 60–90 ppbv, are significantly higher compared to the typical values reported for urban sites of India. The increase rates of O3 in the forenoon hours were estimated to be in the range of about 8.8–10 ppbv h−1. The slopes of ∆O3/∆CO, which is an indicator of the efficiency of photochemical production, were in the range of 0.24–0.33 ppbv ppbv−1. However, levels of primary pollutants e.g., NMHCs, CO, etc. at these sites were much lower than urban sites, but higher compared to previously observed values surrounding marine region of India. The estimated ratios of NMHCs and CO indicate fossil fuel combustion process as the dominant source of primary pollutants in this corridor.  相似文献   

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