我国和东亚地区硫化物跨边界输送态势研究

本文利用污染物三维欧拉长距离输送实用模式,较详细地模拟了我国和东亚地区硫化物跨地区、跨边界输送态势,分析了东亚地区硫化物输送通量随高度、季节变化的分布特点,讨论了不同地区边界上硫化物的跨边界输送通量及流的收支平衡,并给出了我国和周边国家和地区之间硫化物的相互输送量。结果表明,我国向外输送的硫化物占周边国家和地区总硫沉降的比例并不大,各地区硫沉降的主要来源是自身排放;硫化物长距离输送中硫酸根的输送占重要地位,各地区硫酸根沉降中的外来比例较大。我们初步总结出一个东亚地区硫化物输送的概念模式：在低层,夏季主要自西南向东北输送,冬季长江以北自北向南输送,长江以南由西南向北输送,并在长江中下游地区形成一个较强的硫化物辐合带,在高层,无论冬夏均由西向东输送,并随高空带变化,中层为二者的过渡,春秋季的情形界于冬夏之间,偏向冬季。     

用STEM—Ⅱ模式研究东亚地区春季沙尘气溶胶对硫化物输送和沉降的影响

利用ＳＴＥＭ－ＩＩ三维区域尺度大气化学模式,研究了１９９４年３月１日至１４日东亚地区春季沙尘气溶胶对硫化物输送和沉降的影响。结果表明,ＳＯ２和ＳＯ２４的大值区主要出现在我国东部地区。在模拟时段,日本地区火山源的排放对该地区大气中Ｓ分布的贡献达１０％～３０％。并与当时飞机的观测结果相吻合。模拟区域内ＳＯ２和ＳＯ２４的收支的分析研究表明,在硫的总排放量中,从东边界面流出去的输送通量最大,并出现在３０～４００Ｎ带的２～６ｋｍ高度上,这是与该地区最大的人为排放源所在地相一致的。最后,给出了模拟时段整个对流层大气ＳＯ２－４气溶胶含量的分布,还仨算了ＳＯ２－４气溶胶对地气系统的直接辐射强迫和温度变化的影响。     

污染源、气象条件变化对我国SO2浓度及硫沉降量分布的影响

用三维欧拉型污染物长距离输送模式,模拟了中国大陆SOx的分布,并采用不同时期(1975、1980、1987年)的污染源与气象场资料,分析了污染源与气象条件变化对SOx分布产生的影响.研究表明,在该期间中国SOx污染比较严重的地区,气象条件变化导致SO2浓度和硫沉降量的相对变化通常在20%左右;污染源对SO2浓度与硫沉降量的作用通常大于气象条件,污染源变化产生的SO2浓度与硫沉降量的相对变化率为气象条件变化的几倍,甚至1～2个量级,尤其SOx污染比较严重的地区更为明显;但对西北及青藏高原地区,在源排放量变化不大,而气象条件变化较显著时,气象条件的作用通常大于排放源的影响.     

利用次网格技术模拟华东地区大气硫氮沉降

采用数值模拟方法,在区域酸性沉降模式系统中引入次网格处理技术。通过4种次网格方案模拟结果的相互比较,选择最优方案,然后利用最优次网格方案,选取华东地区为例,进一步模拟研究大气硫氮沉降的空间分布。结果表明,就干沉积速率而言,以细网格方案(水平分辨率25 km)为参照,采用次网格方案比粗网格方案(水平分辨率75 km)有明显改进,其中“次网格风速与摩擦速度之积为常数”为最优次网格方案。华东地区硫的年总沉降量是1.92 mt(1 mt=106ton),氮的年总沉降量是0.65mt。华东地区硫化物(SO2、硫酸盐SO42-)干沉降量占总沉降量的49%,氮化物(NO、NO2、硝酸盐NO3-)干沉降量占总沉降量的80%,可见干沉降在大气沉降中具有重要地位。华东地区总的大气硫、氮沉降量中,70%以上到达有植被覆盖的土壤生态系统,这将对农田、草地和森林的硫素和氮素平衡有重要影响。此外,华东部分地区的硫沉降已经超过了临界负荷,而氮沉降尚未出现超临界负荷的现象。     

华东典型地区大气硫沉降通量的观测和模拟研究

本文使用中国科学院常熟和鹰潭生态实验站和气象站的观测资料，应用区域酸沉降模式系统（RegADMS）和大叶阻力相似模型来研究华东地区不同下垫面条件上的大气硫沉降问题，定量估计了农田下垫面上大气硫化物的沉降通量。SO2和硫酸盐的干沉降速率使用大叶阻力相似模型来估计，使用与降水量有关的参数化方案来确定湿沉降系数。结果表明，常熟地区农田下垫面的大气硫沉降通量为19．0gm^-2 a^-1，其中干沉降占42％；而位于江西红壤地区的鹰潭站的大气硫沉降通量为10．4gm^-2a^-1，其中干沉降占83％。比较发现，两地硫干沉降通量绝对值相差不大，但其在总沉降通量中所占的份额有较大差异；常熟站的硫湿沉降通量比鹰潭站要大9．23gm^-2a^-1，该差异是由两地污染状况和气象条件的不同造成。华东地区的年硫沉降总量为1．88Mt（1Mt=10^6t），其中72．8％沉降在农田下垫面上。硫沉降中43％是干沉降，57％是湿沉降。     

两广地区前、后汛期降水异常反位相现象及可能机理

利用1961—2018年中国地面气象台站2 400站中广东省和广西壮族自治区(两广地区)134站逐日降水资料、英国Hadley中心逐月海表温度资料、NCEP/NCAR逐月再分析资料,筛选了两广地区前汛期降水正(负)异常、后汛期降水负(正)异常的年份,即前、后汛期降水异常反位相年份。结果表明,近60 a来,两广地区前、后汛期降水反位相现象与热带西太平洋海温异常存在密切联系。前汛期期间,当热带西太平洋海温为负异常时,大气对该冷源的Rossby波响应引起西北太平洋反气旋环流异常,且水汽由热带西太平洋向两广地区输送并辐合,同时两广地区为水汽的湿平流区域、风场异常辐合区域,其上空受异常上升运动控制,这样的环流配置有利于两广前汛期期间降水正异常。热带西太平洋海温负异常可持续至后汛期期间,大气的Rossby波响应所致的西太平洋反气旋较前汛期偏西北,两广地区为水汽异常辐散区域,同时水汽干平流且风场异常辐散,受异常下沉运动控制,不利于两广地区降水的产生。反之亦然。     

两广地区夏季降水异常与澳大利亚东侧海温异常的联系及可能机制

广东省和广西壮族自治区(两广地区)夏季降水时空分布很不均匀,存在显著的年际变化。利用站点观测降水资料、海洋及大气再分析资料,研究了近40 a两广地区夏季降水年际异常与澳大利亚东侧海温异常的联系及机理。在年际时间尺度上,两广夏季降水异常与澳大利亚东侧的海温异常存在显著的负相关关系。当澳大利亚东侧海温异常偏高时,一方面,部分水汽由热带中太平洋向澳大利亚东侧海区辐合,部分沿西太平洋副热带高压边缘向东亚地区输送,两广地区为水汽辐散区域,另一方面,澳大利亚东侧海区的对流活动增强,该地区上空的上升运动异常增强,通过"大气桥"遥相关使得海洋性大陆地区的异常上升运动增强,从而加强了东亚地区的局地Hadley环流,使得两广地区下沉运动增强,二者共同作用致使两广地区夏季干旱少雨;反之亦然。     

关于我国和东亚酸性物质的输送研究：Ⅱ.硫化物浓度空间分布特征及 …

应用硫化物输送三维欧拉实用模式,计算和分析了我国和东亚地区二氧化硫和硫酸盐粒子的空间分布特点及季节变化,给出了年平均硫化物大气含量分布,还讨论了四种典型下垫面硫化物浓度的垂直分布廓线。结果表明,近地层硫化物浓度分布与排放源的分布类似,高值区主要在山东半岛及相邻的华北部分地区和四川盆地。在上海,台南,汉城和东京等地是小范围的高值区,地面浓度冬季大,夏季浓度小,高空分布形势与低层不同,由西南－东北走向     

关于我国和东亚酸性物质的输送研究II. 硫化物浓度空间分布特征及季节变化

应用硫化物输送三维欧拉实用模式,计算和分析了我国和东亚地区二氧化硫和硫酸盐粒子的空间分布特点及季节变化,给出了年平均硫化物大气含量分布,还讨论了四种典型下垫面硫化物浓度的垂直分布廓线。结果表明,近地层硫化物浓度分布与排放源的分布类似,高值区主要在山东半岛及相邻的华北部分地区和四川盆地,在上海、台南、汉城和东京等地是小范围的高值区。地面浓度冬季大,夏季浓度小。高空分布形势与低层不同,由西南-东北走向变为东西走向。硫酸盐粒子分布高值中心少且平滑。夏季分布更加均匀化。年平均硫酸盐大气含量高值区主要集中在江淮流域,向海上延伸距离较远。四类地区硫化物垂直廓线反映了不同季节外来输送贡献。     

我国雷暴的日变化特征

利用地面1980－2008年(缺2000年)517个常规气象站的观测资料分析了近30年来我国雷暴的日变化特征及其可能的原因.分析表明:雷暴主要发生在午后至傍晚.雷暴的日变化与地形有密切的关系:平原多峰型,山区单峰型,四川盆地夜间高发型,两广沿海地区白天多发.并利用风向的日变化解释了四川盆地地区和两广沿海地区雷暴的日变化...     

Modelled sulphur depositions over Croatia

Summary A Lagrangian receptor-oriented long-range transport model has been applied in order to estimate the relative contribution of domestic, Austrian, Hungarian, Italian and Slovenian emissions to the long-term deposition of airborne sulphur in Croatia. During the November 1, 1991 to April 30, 1992 period 163.31 thousands of tonnes of sulphur were deposited over Croatia., where 90.9% originated from transboundary emission sources. Relative contribution of domestic sources was the biggest (9.1%), while Austrian contribution was the smallest (0.4%).With 1 Figure     

Urban air pollution: process identification, impact analysis and evaluation of forecast potential

The daily variations in the atmospheric pollutants like suspended particulate matter (SPM), respirable suspended particulate matter (RSPM), sulphur dioxide (SO₂) and nitrogen dioxide (NO₂) depend on both local meteorological processes and various natural as well as anthropogenic sources and sinks. It was shown in an earlier work (Goswami and Baruah in Mon Wea Rev 136(9):3597?C3607, 2008) that the daily variations in SPM over a location could be simulated quite well by considering daily meteorological fields from NCEP Reanalysis in combination with a model for natural and anthropogenic sources over Delhi. In the present work, we extend the scope of the model to include three other pollutants: RSPM, SO₂ and NO₂. While the basic conservation equations and the meteorological fields are common to all the three (and SPM) pollutants, the sources and sinks for each is modeled in a species-specific manner to obtain maximum skill. As we do not consider active chemistry, the present model provides the minimal dynamics of pollution over an urban location in terms of annual load; the model error is about 10% on the average, with no significant bias for any of the species.     

Atmospheric chemistry of carbon disulphide

The oxidation of carbon disulphide has been studied under conditions which are likely to pertain in the atmosphere. The quantum yield for direct photo-oxidation of CS₂ in air at 1 atm pressure, using near UV radiation was 0.012, with OCS as a major product. The rate coefficient (k ₁) for the reaction of OH with CS₂, was determined from measurements of OCS formation in the near UV photolysis of HONO?CS₂?O₂?N₂ mixtures. k ₁ was dependent on oxygen concentration rising from ≤4×10^-14 cm³ molecule^-1 s^-1 at O₂≤15 Torr to (2.0±1.0)×10^-12 cm³ molecule^-1 s^-1 at 1 atm air and 300 K. Equimolar amounts of carbonyl sulphide and sulphur dioxide were the major reaction products. The concentration of carbon disulphide in the ambient atmosphere was measured and the concentration to be expected in the background atmosphere was estimated. Rate and concentration data were used to show that carbon disulphide oxidation represents a major source for atmospheric carbonyl sulphide. It can also serve as an alternate source for atmospheric sulphur dioxide in addition to that produced from hydrogen sulphide and dimethyl sulphide. A consideration of atmospheric concentrations and rate data for these trace sulphur gases suggests that the natural sulphur budget is much smaller than the yearly amounts of sulphur dioxide emitted from anthropogenic sources.     

On the application of the Gaussian model for multiple industrial sources for selected centers in South India

Effective environmental planning is essential for any developing urban region. In the present article, the Gaussian model is applied for multiple industrial sources for the months of January, April, July and October, for the cities Hyderabad, Mangalore and Nagpur, to study the spatial distribution of sulphur dioxide concentration. The validity of the model is tested with the actual observations for two stations.     

The importance of three centuries of land-use change for the global and regional terrestrial carbon cycle

Large amounts of carbon (C) have been released into the atmosphere over the past centuries. Less than half of this C stays in the atmosphere. The remainder is taken up by the oceans and terrestrial ecosystems. Where does the C come from and where and when does this uptake occur? We address these questions by providing new estimates of regional land-use emissions and natural carbon fluxes for the 1700–2000 period, simultaneously considering multiple anthropogenic (e.g. land and energy demand) and biochemical factors in a geographically explicit manner. The observed historical atmospheric CO₂ concentration profile for the 1700 to 2000 period has been reproduced well. The terrestrial natural biosphere has been a major carbon sink, due to changes in climate, atmospheric CO₂, nitrogen and management. Due to land-use change large amounts of carbon have been emitted into the atmosphere. The net effect was an emission of 35 Pg C into the atmosphere for the 1700 to 2000 period. If land use had remained constant at its distribution in 1700, then the terrestrial C uptake would have increased by 142 Pg C. This overall difference of including or excluding land-use changes (i.e. 177 Pg C) comes to more than half of the historical fossil-fuel related emissions of 308 Pg C. Historically, global land-use emissions were predominantly caused by the expansion of cropland and pasture, while wood harvesting (for timber and fuel wood) only played a minor role. These findings are robust even when changing some of the important drivers like the extent of historical land-use changes. Under varying assumptions, land-use emissions over the past three centuries could have increased up to 20%, but remained significantly lower than from other sources. Combining the regional land-use and natural C fluxes, North America and Europe were net C sources before 1900, but turned into sinks during the twentieth century. Nowadays, these fluxes are a magnitude smaller than energy- and industry-related emissions. Tropical regions were C neutral prior to 1950, but then accelerated deforestation turned these regions into major C sources. The energy- and industry-related emissions are currently increasing in many tropical regions, but are still less than the land-use emissions. Based on the presented relevance of the land-use and natural fluxes for the historical C cycle and the significance of fossil-fuel emissions nowadays, there is a need for an integrated approach for energy, nature and land use in evaluating possible climate change mitigation policies.     

Dimethylsulphide production in the subantarctic southern ocean under enhanced greenhouse conditions

Dimethylsulphide (DMS) is an important sulphur‐containing trace gas produced by enzymatic cleavage of its precursor compound, dimethylsulphoniopropionate (DMSP), which is released by marine phytoplankton in the upper ocean. After ventilation to the atmosphere, DMS is oxidised to form sulphate aerosols which in the unpolluted marine atmosphere are a major source of cloud condensation nuclei (CCN). Because the micro‐physical properties of clouds relevant to climate change are sensitive to CCN concentration in air, it has been postulated that marine sulphur emissions may play a rôle in climate regulation. The Subantarctic Southern Ocean (41–53°S) is relatively free of anthropogenic sulphur emissions, thus sulphate aerosols will be mainly derived from the biogenic source of DMS, making it an ideal region in which to evaluate the DMS‐climate regulation hypothesis. We have extended a previous modelling analysis of the DMS cycle in this region by employing a coupled general circulation model (CGCM) which has been run in transient mode to provide a more realistic climate scenario. The CGCM output provided meteorological data under the IPCC/IS92a radiative forcing scenario. A DMS production model has been forced with the CGCM climate data to simulate the trend in the sea‐to‐air DMS flux for the period 1960 to 2080, corresponding to equivalent CO₂ tripling relative to pre‐industrial levels. The results confirm a minor but non‐negligible increase in DMS flux in this region, in the range +1% to +6% predicted over the period simulated. Uncertainty analysis of the DMS model predictions have confirmed the positive sign for the change in DMS flux, that is a negative DMS feedback on warming.     

Analysis of VOC emissions using PCA/APCS receptor model at city of Shanghai,China

Qualification of the sources of volatile organic compounds (VOCs) and their effects on city air pollution are crucial issues to develop an effective air pollution control strategy in many polluted large cities of China. In this study, the VOC concentrations measured in Shanghai, China from 2006 to 2008 are analyzed. A receptor model (PCA/APCS; Principal Component Analysis/Absolute Principal Component Scores) is applied for identifying the contributions of individual VOC sources to VOC concentrations. Using the PCA/APCS technique, five and four surrogated VOC sources are classified in the center of Shanghai city in summer and in winter. In summer, the five VOC sources include PCs1 (liquefied petroleum gas/natural gas leakage and gasoline evaporation), PCs2 (vehicle related emissions), PCs3 (solvent usages), PCs4 (industrial productions), and PCs5 (biomass/biofuel/coal burning and other natural sources). In winter, the four VOC sources include PCw1 (liquefied petroleum gas/natural gas leakage and gasoline evaporation), PCw2 (solvent usages and industrial productions), PCw3 (vehicle related emissions), and PCw4 (biomass/biofuel/coal burning). The result suggests that during summer, 24, 28, 17, 18, and 13% of the measured VOC concentrations were estimated due to the PCs1, PCs2, PCs3, PCs4, and PCs5 VOC sources, respectively. During winter, 17, 48, 23, and 12% of the measured VOC concentrations were attributed to the PCw1, PCw2, PCw3, and PCw4 VOC sources, respectively. For aromatic concentrations, 35% of the concentrations were resulted from solvent usage (PCs3), following by industrial productions (PCs4) of 27%, and vehicle emissions (PCs2) of 19%. For alkene concentrations, the two largest contributors were due to gasoline industrial and vehicle emissions in both summer and winter. For alkane concentrations, the largest sources were due to gasoline industrial emissions (PCs1) and vehicle emissions (PCs2) in summer. In winter, vehicle emissions (PCw3), solvent usages/industrial productions (PCw2), and gasoline industrial emissions (PCw1) were the major sources. For halo-hydrocarbon concentrations, biomass/biofuel/coal burning and other natural sources were the major sources in both summer and winter.     

福建省硫沉降量变化的分析与比较

应用中国科学院大气物理研究所建立的三维欧拉污染物输送模式模拟了1995、2000、2002年福建省本省排放源造成的和邻近省份排放源向其输送的硫沉降量,结果表明,福建省接收的硫沉降量有一半以上是由周围省份的远距离输送造成的。进而分析了每年4个季节硫沉降的变化特点,并结合福建省气象条件给出理论解释。最后,把这3年福建省SO2及SO42-年沉降量和各季节沉降量分别作了比较,结果显示,造成福建省SO2沉降的主要来源是本省的排放源,而SO42-沉降中外来源占很大比例,超过了50%。     

Application of Lead Isotopic Ratios in Atmospheric Pollution Studies in the Valley of Mexico

Lead isotopic studies of airborne particulate matter, gasoline and other environmental samples have been carried out to determine possible sources of lead pollution in the Metropolitan Zone of the Valley of Mexico. ²⁰⁶Pb/²⁰⁷Pb ratio in gasoline was 1.1395 ± 0.0165 and 1.071 ± 0.008 for industrially-derived lead as a mean. Natural lead is more radiogenic with values from 1.2082 ± 0.022 to 1.211 ± 0.108. The measured Pb isotopic signature of airborne particulate matter reflects the relative importance of each of these sources. The ²⁰⁶Pb/²⁰⁷Pb ratio was 1.179 ± 0.105 as a mean. The relative importance of gasoline has decreased, and, therefore, other sources (natural and industrial) can be identified by means of isotopic studies. This is a consequence of the introduction of unleaded gasoline as mandaped by strictest environmental regulation.     

A comparison between natural and anthropogenic emissions of the reduced sulfur compounds H2S, COS, and CS2 in a tropical industrialized region

Extensive ambient concentration and flux measurements have been performed in the heavily polluted region of Cubatão/Brazil. Substantial contribution of anthropogenic sources to the local reduced sulfur burden has been observed. As a result of this atmospheric sulfur burden average gas exchange between vegetated soils and the atmosphere shows net deposition. Based mainly on own field measurements a local budget for H₂S, COS, and CS₂ has been made up in order to calculate anthropogenic emissions. All major sources and sinks in the chosen atmospheric reservoir (24×20×1 km) have been taken into account. Due to the small reservoir size fluxes across its boundaries are dominant sources and sinks. The differences between outflux and influx therefore account for the unknown anthropogenic emissions which have been determined to be 80±10 (H₂S), 66±15 (COS), and 29±6 Mmol year^-1 (CS₂). Other sources and sinks like natural emissions, chemical conversion, and dry deposition turned out to be of minor importance on a local scale. In fact, inside the investigated reservoir natural emissions were below 0.5% of anthropogenic emissions. Anthropogenic emissions of H₂S, COS, and CS₂ quantified in this work have been compared with global emission estimates for these compounds made by other authors. We conclude that global anthropogenic emissions of reduced sulfur compounds especially of COS and CS₂ are currently under-estimated.