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1.
在过去的20多年里,中外对硫酸盐气溶胶做了大量的研究,对它在大气中的排放、含量、光学特征和辐射强迫有了深入的认识;由于硝酸盐气溶胶在大气中平均含量比硫酸盐低很多,因此过去人们对硝酸盐的研究没有给予重视。然而,近年来的研究表明,硝酸盐气溶胶的散射性质在某些波段甚至强于硫酸盐;同时,由于未来对人为硫酸盐前体物的减排,硫酸盐气溶胶排放会大幅度减少,而硝酸盐气溶胶的排放却增长迅速,其在人为气溶胶中所占的比重越来越高,将会导致其在未来造成的辐射强迫有可能超过硫酸盐,使得其在地区范围内和季节尺度上成为重要的辐射强迫和气候影响因子。中国是硝酸盐气溶胶排放量较大的地区,硝酸盐对未来中国气候和气候变化的影响显得越来越重要。因此,就近年来有关硝酸盐气溶胶的排放和在大气中的浓度变化、光学厚度分布特征及其辐射强迫的研究进展做了回顾和介绍,并对其未来的研究做了展望。  相似文献   

2.
Organic aerosol formation resulting from the ozonolysis of α-pinene, myrcene and sabinene was investigated in a large aerosol chamber in the presence of aqueous seed aerosols. The chemical composition of the particles was monitored by an aerosol mass spectrometer (Aerodyne Research Inc.) as a function of time and the particle size. Smaller particles were found to contain more organics relative to sulfate than the larger ones. In contrast, the water to sulfate mass ratio was not dependent on the particle size. These experimental findings indicate the formation of organic layers on the particles. With the aid of an aerosol dynamic model we demonstrate that the observations are consistent with the formation of multilayered organic films having thicknesses of approximately 10 nm. The results also suggest that the films were formed through condensation of low-volatile oxidation products that did not take up water considerably. Even though dissolution of oxidation products into the particle aqueous phase cannot be conclusively ruled out, the most plausible interpretation of the results is that the monoterpene ozonolysis lead to the formation of organic coatings on aqueous aerosols. Such films are likely to form in regions with monoterpene emissions.  相似文献   

3.
We intercompare a series of multi-year simulations with a coupled regionalchemistry-climate model for east Asia to assess the relative importance ofdirect and indirect (Type I) effects of anthropogenic sulfate on the climateof the region. Both direct and indirect aerosol effects induce a negativeradiative forcing that results in a cooling of the surface and in a decrease of precipitation. Under present day sulfur emissions,the direct aerosol effects prevail during the cold season, while the indirecteffects dominate in the warm season (when cloudiness is maximum over the region). When both the direct and indirect effects are included, the surface cooling varies in the range of –0.1 to over –1 K throughout the region and extended areas ofstatistically significant cooling are found in all seasons except winter.The indirect effects largely dominate in inhibiting precipitation, especiallyduring the summer. When doubling the sulfur emissions, the direct effects aresubstantially strengthened, while the indirect effects are only marginally affected. This indicates that the indirect effects over the region might be asymptotically approaching their maximum efficiency. Overall, the indirect effects appear necessary to explain theobserved temperature record over some regions of China, at least in the warm season.A number of uncertainties need to be addressed, such as due to Type IIindirect effects, modeling of the relationship between aerosol concentration and cloud optical properties, and contribution of aerosols other than anthropogenic sulfate.  相似文献   

4.
夏季硫酸盐和黑碳气溶胶对中国云特性的影响   总被引:1,自引:2,他引:1  
利用WRF-Chem(Weather Research and Forecasting model coupled with Chemistry)模式研究2006年8月1日—9月1日中国区域硫酸盐和黑碳气溶胶对云特性的影响。模式验证利用了卫星和地面观测的气象要素、化学物质浓度、气溶胶光学特性和云微物理特性。模式性能评估表明该模式能较好地抓住气象要素(温度、降水、相对湿度和风速)的量级和空间分布特征。通过与地面观测和MODIS卫星数据对比发现,尽管模式模拟还存在偏差,但还是能较好模拟出气溶胶物种的地表浓度、气溶胶光学厚度(AOD)、云光学厚度(COD)、云量(CLDF)、云顶云滴有效半径(CER)和云水路径(LWP)。通过两个敏感性试验(分别增加二氧化硫和黑碳排放量至控制试验排放的3倍)与控制试验的对比发现硫酸盐比黑碳更易成为云凝结核,在中国东部云顶云滴数浓度和其它云特性参数对二氧化硫排放增加的响应均从北向南呈递增,这与地面湿度分布有关。云滴有效半径对硫酸盐气溶胶的响应符合气溶胶第一间接效应的定义,即硫酸盐气溶胶增多,云滴数浓度增加,云滴有效半径减少,但是对黑碳气溶胶的响应在各区域不尽相同。还发现黑碳对云量的影响远大于硫酸盐,主要原因是由于黑碳气溶胶直接辐射效应(对太阳光的吸收)导致的云的“燃烧”作用。   相似文献   

5.
We used an online aerosol–climate model to study the equilibrium climate response of the East Asian summer monsoon (EASM) to increases in anthropogenic emissions of sulfate, organic carbon, and black carbon aerosols from 1850 to 2000. Our results show that each of these aerosol species has a different effect on the EASM as a result of changes in the local sea–land thermal contrast and atmospheric circulation. The increased emission of sulfate aerosol leads to a decrease in the thermal contrast between the land and ocean, a southward shift of the East Asian subtropical jet, and significant northerly wind anomalies at 850 hPa over eastern China and the ambient oceans, markedly dampening the EASM. An increase in organic carbon aerosol results in pronounced surface cooling and the formation of an anomalous anticyclone over the oceans north of 30°N. These effects cause a slight increase in the sea–land thermal contrast and southerly flow anomalies to the west of the anticyclonic center, strengthening the northern EASM. An increase in organic carbon emission decreases the sea–land thermal contrast over southern China, which weakens the southern EASM. The response of the summer 850-hPa winds and rainfall over the East Asian monsoon region to an increase in black carbon emission is generally consistent with the response to an increase in organic carbon. The increase in black carbon emission leads to a strengthening of the northern EASM north of 35°N and a slight weakening of the southern EASM south of 35°N. The simulated response of the EASM to the increase in black carbon emission is unchanged when the emission of black carbon is scaled up by five times its year 2000 levels, although the intensities of the response is enhanced. The increase in sulfate emission primarily weakens the EASM, whereas the increases in black carbon and organic carbon emissions mitigate weakening of the northern EASM.  相似文献   

6.
春季中国东部气溶胶化学组成及其分布的模拟研究   总被引:2,自引:0,他引:2  
本文利用区域空气质量模式RAQMS(Regional Air Quality Model System),对2009年春季中国东部气溶胶主要化学成分及其分布进行了模拟研究。与泰山站观测资料的对比结果显示,模式能比较合理地反映气溶胶浓度的逐日变化特征。整体上,模式对无机盐气溶胶的模拟好,分别高估和低估黑碳和有机碳气溶胶浓度,其原因与排放源、二次有机气溶胶化学机制和模式分辨率的不确定性有关。模拟结果显示,春季气溶胶浓度高值主要集中于华北、四川东部、长江中下游等地区。受东南亚生物质燃烧和大气输送的影响,中国的云南和广西等地区有机碳浓度高于中国其他地区。中国西北部沙尘浓度较高,而且向东输送并影响到中国东部和南方部分地区。中国东部的华北、四川东部、长江中下游等地PM2.5(空气动力学直径在2.5微米以下的颗粒物)污染严重,4月平均PM2.5浓度超过了我国日平均PM2.5浓度限值。中国东部泰山站的观测和模拟结果都显示近地面硝酸盐浓度超过硫酸盐,中国北部对流层中硝酸盐的柱含量也大于硫酸盐,而在中国南部则相反,这一方面与春季中国云量 南多北少的分布特征以及云内液相化学反应有关,另一方面也与南北温差对气溶胶形成的影响有关。就整个中国东部而言,虽然硫酸盐的柱含量(46 Gg)仍大于硝酸盐(42 Gg),但比较接近,反映出我国氮氧化物排放迅速增加的趋势。春季中国地区对流层中PM10(空气动力学直径在10微米以下的颗粒物)及其化学成分柱含量分别为:990.8 Gg(PM10),52.6 Gg(硫酸盐),48.2 Gg(硝酸盐),32.1 Gg(铵盐),22.9 Gg(黑碳)和74.1 Gg(有机碳),有机碳(OC)中一次有机碳(POC)和二次有机碳(SOC)分别占60%和40%,中国东部PM10中人为气溶胶和沙尘分别占30%和70%,反映了春季沙尘对我国大气气溶胶的重要贡献。  相似文献   

7.
In this study, a combination of satellite observations and reanalysis datasets is used to analyze the spatiotemporal distribution, classification and source of pollutants over the eastern slope of the Tibetan Plateau(ESTP). The aerosol optical depth(AOD) over the ESTP is extremely large and even larger than some important industrialized regions and deserts. The main aerosol component over the ESTP is sulfate, followed by carbonaceous and dust aerosols. Local emissions related to human activity directly contribute to the accumulation of sulfate and carbonaceous aerosols over the Sichuan Basin. In addition, in spring, abundant carbonaceous aerosols emitted from forest, grassland and savanna fires in Southeast Asia can be transported by the prevailing southwesterly wind to southern China and the ESTP. The dust AOD over the ESTP peaks in spring because of the transport from the Taklimakan and Gobi deserts. Additionally, the high aerosol loading over the ESTP is also directly related to the meteorological background. Due to the special topography, the terrain-driven circulation can trap aerosols in the Sichuan Basin and these aerosols can climb along the ESTP due to the perennial updraft. The aerosol loading is lowest in summer because of effective wet deposition induced by the strong precipitation and better dispersion conditions due to the larger vertical temperature gradients and ascending air movement enhanced by the plateau heat pump effect. In contrast,the aerosol loading is greatest in winter. Abundant anthropogenic aerosols over the ESTP may generate some climatic and environmental risks and consequently greatly influence the downstream regions.  相似文献   

8.
基于新耦合气溶胶气候模式FGOALS-f3-L模拟分析了2002-2011年青藏高原地区气溶胶时空分布特征.结果表明:青藏高原地区,沙尘,硫酸盐,碳质气溶胶(包括黑碳,有机碳和混合碳)地表质量浓度分别占比为53.6%,32.2%,14.2%;在拉萨站点,模拟的气溶胶地表质量浓度被低估,尤其是黑碳和有机碳气溶胶;模拟的气...  相似文献   

9.
The concentrations of selected trace elements and non-sea salt sulfate were determined for aerosol particle samples collected over the open North Atlantic Ocean as part of the Atmosphere/Ocean Chemistry Experiment (AEROCE). The concentrations of atmospheric sea salt and mineral aerosol, which together dominate the mass of particulate material in the atmosphere, were higher at Barbados than at Bermuda. In contrast, the impact of pollution sources on trace element concentrations was more evident at Bermuda than at Barbados. At both sites Sb and Se were enriched significantly over the concentrations expected from mineral dust or from atmospheric sea salt. Moreover, the concentrations of Sb and Se were correlated, and the observed Sb/Se ratios often were similar to those resulting from anthropogenic emissions. At Bermuda, the concentrations of Sb and Se co-varied with non-sea salt sulfate, suggesting that a significant fraction of the non-sea salt sulfate is anthropogenic. In a broader context, the synthesis of results demonstrates that trace element data are useful for evaluating the relative contributions of anthropogenic vs. natural sources to the budgets of non-sea salt sulfate in acrosol particles.  相似文献   

10.
Temporal variations in atmospheric hydrogen sulphide concentrations and its biosphere-atmosphere exchanges were studied in the World’s largest mangrove ecosystem, Sundarbans, India. The results were used to understand the possible contribution of H2S fluxes in the formation of atmospheric aerosol of different size classes (e.g. accumulation, nucleation and coarse mode). The mixing ratio of hydrogen sulphide (H2S) over the Sundarban mangrove atmosphere was found maximum during the post-monsoon season (October to January) with a mean value of 0.59?±?0.02 ppb and the minimum during pre-monsoon (February to May) with a mean value of 0.26?±?0.01 ppb. This forest acted as a perennial source of H2S and the sediment-air emission flux ranged between 1213?±?276 μg S m?2 d?1(December) and 457?±?114 μg S m?2 d?1 (August) with an annual mean of 768?±?240 μg S m?2d?1. The total annual emissions of H2S from the Indian Sundarban were estimated to be 1.2?±?0.6 Tg S. The accumulation mode of aerosols was found to be more enriched with non-sea salt sulfate with an average loading of 5.74 μg m?3 followed by the coarse mode (5.18 μg m?3) and nucleation mode (1.18 μg m?3). However, the relative contribution of Non-sea salt sulfate aerosol to total sulfate aerosol was highest in the nucleation mode (83%) followed by the accumulation (73%) and coarse mode (58%). Significant positive relations between H2S flux and different modes of NSS indicated the likely link between H2S, a dominant precursor for the non-sea salt sulfate, and non-sea sulfate aerosol particles. An increase in H2S emissions from the mangrove could result in an increase in enhanced NSS in aerosol and associated cloud albedo, and a decrease in the amount of incoming solar radiation reaching the Sundarban mangrove forest.  相似文献   

11.
The paper discusses the potential effects on the ozone layer of gases released by the engines of proposed high altitude supersonic aircraft. The major problem arises from the emissions of nitrogen oxides which have the potential to destroy significant quantities of ozone in the stratosphere. The magnitude of the perturbation is highly dependent on the cruise altitude of the aircraft. Furthermore, the depletion of ozone is substantially reduced when heterogeneous conversion of nitrogen oxides into nitric acid on sulfate aerosol particles is taken into account in the calculation. The sensitivity of the aerosol load on stratospheric ozone is investigated. First, the model indicates that the aerosol load induced by the SO2 released by aircraft is increased by about 10–20% above the background aerosols at mid-high latitude of the Northern Hemisphere at 15 km for the NASA emission scenario A (the NASA emission scenarios are explained in Tables I to III). This increase in aerosol has small effects on stratospheric ozone. Second, when the aerosol load is increased following a volcanic eruption similar to the eruption of El Chichon (Mexico, April 1982), the ozone column in spring increases by as much as 9% in response to the injection of NO x from the aircraft with the NASA emission scenario A. Finally, the modeled suggests that significant ozone depletion could result from the formation of additional polar stratospheric clouds produced by the injection of H2O and HNO3 by the aircraft engines.  相似文献   

12.
温室气体和硫酸盐气溶胶的辐射强迫作用   总被引:9,自引:4,他引:5  
对GOALS4 .0海 陆 气耦合模式的相关部分进行了改进 ,主要改进包括温室气体的扩充和硫酸盐气溶胶“显式”方案的引入 ,并引入 2 0世纪温室气体的实际浓度变化以及硫循环模式模拟的硫酸盐气溶胶的三维全球浓度分布 ,模拟了温室气体和硫酸盐气溶胶造成的辐射强迫的空间分布和时间变化。全球平均的温室气体和硫酸盐气溶胶的辐射强迫分别为 2 .17W /m2 和 - 0 .2 9W /m2 ;温室气体造成的辐射强迫在空间上呈现明显的纬向结构 ,最大值 (大于 2 .5W/m2 )和最小值 (小于 1W /m2 )分别位于副热带和两极地区 ,在北半球主要工业区硫酸盐气溶胶的辐射强迫绝对值接近温室气体的辐射强迫值 (大于 - 2 .0W /m2 )。  相似文献   

13.
Future global emissions of aerosols will play an important role in governing the nature and magnitude of future anthropogenic climate change. We present in this paper a number of future scenarios of emissions of black carbon (BC) and organic carbon (OC) by world region, which we combine with sulfate (SO4) assessed in terms of the emissions of its precursor, SO2. We find that aerosol emissions from the household and industrial sectors are likely to decline along almost all future pathways. Transportation emissions, however, are subject to complex interacting forces that can lead to either increases or decreases. Biomass burning declines in many scenarios, but the Amazon rainforests remain vulnerable if unsustainable economic growth persists. East Asia is the key region for primary aerosols, and trends in China will have a major bearing on the direction and magnitude of releases of BC (expected reductions in the range of 640–1290 Gg), OC (reductions of 520–1900 Gg), and SO2 (ranging from an increase of 21 Tg to a reduction of 30 Tg). Analysis of joint BC, OC, and SO2 emission changes identifies a number of key world regions and economic sectors that could be effectively targeted for aerosol reductions.  相似文献   

14.
《Atmospheric Research》2007,83(3-4):688-697
Intensive measurements of gas and aerosol for 2 weeks were carried out at Qingdao (gas and aerosol in 2000, 2001 and 2002), Fenghuangshan (gas and aerosol in 2000 and 2001), and Dalian (aerosol in 2002) in the winter–spring period. High SO2 episodes were observed on 18 January 2000 at both Qingdao and Fenghuangshan. According to back trajectory calculations and analysis of gaseous species, high SO2 episodes were caused by local pollution and transport.Nitrate, sulfate and ammonium were the major species in PM2.5. Mass fractions of NO3, nss-SO42− and NH4+ at Qingdao in 2002 were 10%, 12% and 5.5% for PM2.5, respectively, which were higher than that of nss-Ca2+ (1%). Chemical compositions observed at Dalian and Fenghuangshan were similar to those at Qingdao. The mass ratio of nss-SO42−/SO2 at Qingdao in winter was low (< 1.2), indicating that sulfate was probably produced by the slow oxidation of SO2 in the gas phase and/or was transported from outside of Qingdao in winter. The equivalent ratio of NH4+ to nss-SO42− was 1.39, suggesting that ammonium sulfate was one of the major chemical compositions in PM2.5. The NO3/SO42− ratio at Qingdao was higher than that at remote places in East Asia. Gas and aerosol data obtained at Fenghuangshan were similar to data at Qingdao, suggesting that emissions from small cities may have a great influence on pollution in northern China.  相似文献   

15.
A modelling platform for studying photochemical gaseous and aerosol phase processes from localized (e.g., point) sources has been presented. The current approach employs a reactive plume model which extends the regulatory model RPM‐IV by incorporating aerosol processes and heterogeneous chemistry. The physics and chemistry of elemental carbon, organic carbon, sulfate, nitrate, ammonium material of aerosols are treated and attributed to the PM size distribution. A modified version of the carbon bond IV chemical mechanism is included to model the formation of organic aerosol. Aerosol dynamics modeled include mechanisms of nucleation, condensation, dry deposition and gas/particle partitioning of organic matter. The model is first applied to a number of case studies involving emissions from point sources and sulfate particle formation in plumes. Model calculations show that homogeneous nucleation is an efficient process for new particle formation in plumes, in agreement with previous field studies and theoretical predictions. In addition, the model is compared with field data from power plant plumes with satisfactory predictions against gaseous species and total sulphate mass measurements. Finally, the plume model is applied to study secondary organic matter formation due to various emission categories such as vehicles and the oil production sector.  相似文献   

16.
Concentrations of aerosol methanesulfonic acid (MSA) and non-sea-salt (nss) sulfate were measured at six island stations in the Pacific Ocean to investigate regional and seasonal patterns of organosulfur emissions and the origin of nss sulfate over the Pacific. The mean MSA concentrations, in g/m3, at the stations were: Shemya, 0.097±0.098; Midway, 0.029±0.021; Fanning, 0.044±0.012; American Samoa, 0.026±0.012; New Caledonia, 0.021±0.009; Norfolk, 0.024±0.019. The extremely high MSA levels found at Shemya indicate a major source of organosulfur emissions in the western North Pacific. Significant seasonal trends in MSA were observed, with higher MSA occurring during warm months. The amplitude of the seasonal variation was greatest at higher latitude stations. At Fanning and American Samoa, which have minimal input of continental material, there is a significant positive correlation between MSA and nss sulfate. MSA/nss sulfate ratios at other Pacific stations exhibit greater variability, which may be related to variations in: the input of continentally derived sulfate, the composition of oceanic organosulfur emissions, and atmospheric reaction pathways.  相似文献   

17.
The effect of anthropogenic emissions from China on global burdens of ozone, sulphate, organic carbon (OC) and black carbon (BC) aerosols is examined, using the three-dimensional chemistry transport model Oslo CTM2. Two model simulations were performed, the first with global present-day emissions and the second with the anthropogenic emissions from China set to their pre-industrial levels. The global radiative forcing for these species is then calculated. Industrial emissions from China are found to account for a 4–5% increase in the global burden of OC aerosol, the change in secondary organic aerosol being slightly less than that of primary organic aerosol. A 10% increase in the global sulphate aerosol burden is calculated, and the increase in BC is 23%. The global radiative forcing of aerosols from China was calculated to be −62, −3.7, −13 and 89 mW m−2, for sulphate, secondary organic, primary organic and BC aerosols, respectively. The increase in ozone causes a forcing of 77 mW m−2.  相似文献   

18.
Intensive measurements of gas and aerosol for 2 weeks were carried out at Qingdao (gas and aerosol in 2000, 2001 and 2002), Fenghuangshan (gas and aerosol in 2000 and 2001), and Dalian (aerosol in 2002) in the winter–spring period. High SO2 episodes were observed on 18 January 2000 at both Qingdao and Fenghuangshan. According to back trajectory calculations and analysis of gaseous species, high SO2 episodes were caused by local pollution and transport.Nitrate, sulfate and ammonium were the major species in PM2.5. Mass fractions of NO3, nss-SO42− and NH4+ at Qingdao in 2002 were 10%, 12% and 5.5% for PM2.5, respectively, which were higher than that of nss-Ca2+ (1%). Chemical compositions observed at Dalian and Fenghuangshan were similar to those at Qingdao. The mass ratio of nss-SO42−/SO2 at Qingdao in winter was low (< 1.2), indicating that sulfate was probably produced by the slow oxidation of SO2 in the gas phase and/or was transported from outside of Qingdao in winter. The equivalent ratio of NH4+ to nss-SO42− was 1.39, suggesting that ammonium sulfate was one of the major chemical compositions in PM2.5. The NO3/SO42− ratio at Qingdao was higher than that at remote places in East Asia. Gas and aerosol data obtained at Fenghuangshan were similar to data at Qingdao, suggesting that emissions from small cities may have a great influence on pollution in northern China.  相似文献   

19.
 The atmospheric general circulation model ECHAM-4 is coupled to a chemistry model to calculate sulfate mass distribution and the radiative forcing due to sulfate aerosol particles. The model simulates the main components of the hydrological cycle and, hence, it allows an explicit treatment of cloud transformation processes and precipitation scavenging. Two experiments are performed, one with pre-industrial and one with present-day sulfur emissions. In the pre-industrial emission scenario SO2 is oxidized faster to sulfate and the in-cloud oxidation via the reaction with ozone is more important than in the present-day scenario. The atmospheric sulfate mass due to anthropogenic emissions is estimated as 0.38 Tg sulfur. The radiative forcing due to anthropogenic sulfate aerosols is calculated diagnostically. The backscattering of shortwave radiation (direct effect) as well as the impact of sulfate aerosols on the cloud albedo (indirect effect) is estimated. The model predicts a direct forcing of −0.35 W m-2 and an indirect forcing of −0.76 W m-2. Over the continents of the Northern Hemisphere the direct forcing amounts to −0.64 W m-2. The geographical distribution of the direct and indirect effect is very different. Whereas the direct forcing is strongest over highly polluted continental regions, the indirect forcing over sea exceeds that over land. It is shown that forcing estimates based on monthly averages rather than on instantaneous sulfate pattern overestimate the indirect effect but have little effect on the direct forcing. Received: 16 October 1996/Accepted: 24 October 1996  相似文献   

20.
Field data on the ion composition and mass concentration of aerosol in the rural (Wingene) and urban (Antwerp) regions of Belgium and the results of their thermodynamic analysis are presented. Ammonium nitrate and ammonium sulfate are found to be the major water-soluble components of aerosol particles. The seasonal variability of mass concentration, phase state, and ion composition of aerosol particles is largely determined by variations in temperature and relative humidity. It is shown that the content of ammonium nitrate and ammonium sulfate in PM2.5 is close to their thermodynamic equilibrium concentrations.  相似文献   

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