污染源、干沉降和气相化学影响硫沉降的数值研究

利用欧拉型区域硫沉降模式对污染源、干沉降和气相化学等物理化学过程在酸沉降中的作用进行了数值分析。结果表明:排放源的强度和高度影响着污染物的分布和输送,其影响是非线性的。在区域酸沉降模式中,干沉降速度和气相化学转化率简单地取为常数对SO#-[2]及SO#+[2-]#-[4]浓度分布引起的误差是不可忽视的。     

区域酸沉降模式

本文提出一个区域的欧拉酸雨模式,包括了大气中污染物质的输送、扩散、非线性化学转化和干湿沉降等物理和化学过程.气相化学反应有18种化学物质,包含了二氧化硫气相氧化的主要化学方程.液相氧化反应包含了H_2O_2,O_3及催化剂对二氧化硫的氧化过程.水平方向有35×35个网格点,垂直方向分15层.选用了四川、贵州地区1988年的8次降水过程对模式作了检验,结果证明模式能较好地模拟这个地区的二氧化硫、硫酸根及降水pH的分布状况.     

区域酸性沉降的数值研究 II. 个例模拟和试验

利用建立的区域酸性污染物沉降模式，配合中尺度模式MM4预报的气象场，以1991年6月12～14日淮河流域的一次降雨过程作为实例，对我国东半部及其相邻地区的酸沉降进行了数值模拟和试验研究。结果表明，模式基本上能够模拟出区域酸性沉降的特征，具有良好的综合模拟性能和广阔的应用前景。     

区域酸性沉降的数值研究：Ⅱ.个例模拟和试验

利用建立的区域酸性污染物沉降模式，配合中尺度模式ＭＭ４预报的气象场，以１９９１年６月１２￣１４日淮河流域的一次降雨过程作为实例，对我国东半部及其相邻地区的酸沉降进行了数值模拟和试验研究。结果表明，模式基本上能够模拟出区域酸性沉降的特征，具有良好的综合模拟性能和广阔的应用前景。     

欧拉型区域硫沉降模式研究

建立了一个三维硫沉降欧拉模式，模式中比较全面地考虑了硫沉降过程中的物理、化学机制。包括平流、扩散、干湿沉降和积云的垂直输送作用等物理过程，气相化学、液相化学和气溶胶表面的非均相化学等化学过程。其中非均相化学和积云的垂直输送参数化在国内外同类模式中尚不多见。模式结果与实测及其他模式结果的对比表明，该模式能够较好地模拟出SO2的水平和垂直分布及SO2-4在降水中的浓度。     

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。     

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。     

东亚酸沉降模式不确定性分析

酸沉降会对生态环境造成危害。要控制和减少酸沉降,就要了解酸沉降的幅度和不确定性,而模式研究是获得这些因子的重要工具。用东亚酸沉降模式比较计划（MICS-AsiaⅡ）中7个模式模拟的2001年7月和12月东亚地区酸沉降数据及东亚酸沉降监测网络（EANET）的观测数据,通过相关分析发现多模式模拟的平均值可表现东亚地区酸沉降的分布特征。采用各个模式与模拟结果平均值的离散程度来表征这些模式在东亚地区的不确定性,简要分析了目前模式模拟东亚酸沉降的不确定及其产生原因,可为制定酸沉降的控制措施提供依据。     

农田生态系统大气硫沉降通量的观测研究

1998年 11月～ 1999年 10月间在中国科学院红壤站 (江西鹰潭 )农田小气候站进行了大气二氧化硫 (SO2 )、硫酸盐粒子 (SO2 -4)浓度采样和雨水样本收集 ,利用阻力模式和全年逐时气象资料计算 SO2 和 SO2 -4的干沉降速度 ,估算干沉降通量 ,利用降水资料和雨水中硫酸根离子浓度估计大气硫的湿沉降 ,从而定量研究大气硫沉降输入农田生态系统的通量 ,结果表明 :农田下垫面上 SO2 和 SO2 -4干沉降速度的年平均值分别是 0 .373± 0 .170 cm· s-1(月均值 0 .16 1～ 0 .5 45 cm·s-1)、0 .198± 0 .12 3cm· s-1(月均值 0 .15 2～ 0 .2 6 9cm· s-1)。农田下垫面硫年总沉降量为 10 .3g· m-2 ,其中干沉降占总沉降的 83.3%。硫的干沉降又以 SO2 的干沉降为主 ,占年干沉降总量的 92 .2 %。大气硫沉降输入占农田生态系统输入总量的 90 %以上 ,是农田生态系统获取硫素的一个重要途径     

南京郊区大气氮化物浓度和氮沉降通量的研究

为研究南京郊区的大气氮化物污染状况,进而估算其大气氮沉降通量,2005年6月-2006年5月在南京大学浦口校区气象园进行了大气、气溶胶和雨水样本的收集,同步进行近地面气象观测.在实验室分析大气氮化物NOx、NH3和有机氮浓度、总悬浮颗粒物(TSP)中硝酸盐、亚硝酸盐、铵盐和有机氮的质量浓度、雨水中NO-3、NO-2、NH+4离子和有机氮的质量浓度,利用气象资料和大叶阻力相似模型计算大气氮化物的干沉降速度,进而定量估算大气氮沉降通量.研究结果表明:南京郊区大气中有机氮浓度水平较高,无机氮(氨态氮和硝态氮)浓度水平较低.大气氮沉降量较大,且湿沉降和有机沉降贡献率占主导地位,这取决于本地区的下垫面和污染状况,同时也与气象条件有密切关系.     

Numerical Investigation of Gas Scavenging by Weak Precipitation

A one-dimensional cloud model with size-resolved microphysics and size-resolved aqueous-phase chemistry, driven by prescribed dynamics, has been used to study gas scavenging by weak precipitation developed from low-level, warm stratiform clouds. The dependence of the gas removal rate on the physical and chemical properties of precipitation has been explored under controlled initial conditions. It is found that the removal of four gaseous species (SO₂, NH₃, H₂O₂ and HNO₃) strongly depends on the total droplet surface area, regardless the mean size of droplets. The removal rates also correlate positively with the precipitation rate, especially for precipitation having a mean radius larger than 20 μm. The dependence of the scavenging coefficients on the total droplet surface area is stronger than on the precipitation rate. The removal rates of SO₂, NH₃ and H₂O₂ by precipitation strongly depend on the others' initial concentrations. When NH₃ (or H₂O₂) concentration is much lower than that of SO₂, the removal rate of SO₂ is then controlled by the concentration of H₂O₂ (or NH₃). The removal of NH₃ (or H₂O₂) also directly depends on the concentration of SO₂. NH₃ and H₂O₂ can also indirectly affect each other's removal rate through interaction with SO₂. The scavenging coefficient of SO₂ increases with the concentration ratio of NH₃ to SO₂ if the ratio is larger than 0.5, while the scavenging coefficient of NH₃ increases with the concentration ratio of SO₂ to NH₃ when the ratio is smaller than 1. The scavenging coefficient of H₂O₂ generally increases with the concentration ratio of SO₂ to H₂O₂. Although the Henry's law equilibrium approach seems to be able to simulate gas scavenging by cloud droplets, it causes large errors when used for simulating the scavenging of soluble gas species by droplets of precipitating sizes.     

Determination of Sulfur Balance Between the Atmosphere and a Norway Spruce Forest Ecosystem: Comparison of Gradient Dry + Wet and Throughfall Deposition Measurements

Total sulfur deposition was determined above a Norway spruce forest, in Hungary. Two methods were applied, on one hand dry + wet deposition measurements and on the other, throughfall and stemflow deposition estimations have been carried out. Results show: total depositions are 3.3 and 3.2 g S m^–2 yr^–1 determined by dry + wet and throughfall deposition methods, respectively. The share of the dry deposition in the total S-load is 73%. The agreement between the results of the two different methods is good and suggests the needlessness of complicated dry + wet flux measurements, i.e. the total and dry deposition of sulfur compounds to forests can be determined by simple throughfall and wet deposition measurements.     

Precipitation Chemistry and Wet Deposition in Kruger National Park, South Africa

The chemical composition, as well as the sources contributing to rainwater chemistry have been determined at Skukuza, in the Kruger National Park, South Africa. Major inorganic and organic ions were determined in 93 rainwater samples collected using an automated wet-only sampler from July 1999 to June 2002. The results indicate that the rain is acidic and the averaged precipitation pH was 4.72. This acidity results from a mixture of mineral acids (82%, of which 50% is H₂SO₄) and organic acids (18%). Most of the H₂SO₄ component can be attributed to the emissions of sulphur dioxide from the industrial region on the Highveld. The wet deposition of S and N is 5.9 kgS⋅ha⁻¹⋅yr⁻¹ and 2.8 kgN⋅ha⁻¹⋅yr⁻¹, respectively. The N deposition was mainly in the form of NH₄ ⁺. Terrigenous, sea salt component, nitrogenous and anthropogenic pollutants have been identified as potential sources of chemical components in rainwater. The results are compared to observations from other African regions.     

积云的清除作用与其酸化的数值模拟

一维时变参数化积云模式与污染物浓度连续方程相结合，根据积云内外SO2和HNO3浓度、云水S(VI)浓度、H2O2和O3的氧化速率以及地面雨水S(VI)浓度的时空变化，分别讨论核化清除、液相氧化、云下气溶胶清除、碱性气溶胶、云外污染物的夹卷以及SO2初始分布等因子的重要性。     

适用于大中尺度污染物输送模式的粒子干沉降参数化方案

用“二层”模式给出一个适用于污染物输送模式的粒子干沉降参数化方案,它比较详细地考虑了近地面层的气象条件,地表特性和气溶胶粒子的物理、化学特性等。从计算值与观测值的比较来看,计算值的离散范围能涵盖所有的观测结果,因而从总体上看此参数化方案是合理的,能够描述粒子总污染物干沉降的主要物理过程及机制。       

Absorption and desorption of dichloromethane vapor by water drops in air. An experimental test of scavenging theory

An experimental study of the scavenging of dichloromethane vapor by water drops falling at terminal velocity, has been carried out in the UCLA precipitation shaft, in order to test the predictions of theoretical washout models. Whereas good agreement between theory and experiment was found for drops of radius 0.332 mm, computed gas uptake rates for 1.253 and 2.21 mm radius drops were much slower than those measured, just as reported previously for the washout of both sulfur dioxide and acetaldehyde. An analysis shows that theory can be reconciled with all of the experimental data by replacing the compound specific aqueous phase Fickian molecular diffusion coefficient used in the theory, by an effective diffusivity, having a constant value, (3×10^-4 cm² s^-1), independent of the physical and chemical nature of the absorbed species, for all drops of equivalent radii greater than 0.9 mm.