我国低纬度、亚热带地区的降水化学及其雨水酸化趋势分析

在世界上酸沉降研究尚为空白的低纬度、亚热带地区建立了酸沉降监测网。通过两年的监测，结果表明降水中酸度和离子总浓度季节变化明显，Ｃａ￣（２＋）和ＮＨ在降水离子构成中占百分率较高，阳离子总和略大于阴离子总和。两广地区降水酸度是雨水中多种阴、阳离子综合作用的结果，降水中ＳＯ浓度高的地区是ＳＯ＿２排放量高的地区，控制雨水逐年酸化趋势的唯一途径是限制ＳＯ＿２排放。     

青岛地区酸沉降现状的研究

青岛地区的降水酸化问题在我国北方具有一定的代表性。该研究在对青岛地区降水酸度的时空分布、酸性降水与气象条件的关系进行长期常规观测及集中综合观测,取得大量数据的基础上,重点分析了青岛地区酸沉降的现状及发展趋势。结果表明:青岛地区降水酸度和频率与SO₂环境浓度有关,SO₂浓度较高的市区降水酸度和频率亦高,市郊较低,远郊最低;降水酸度季节变化明显,冬、春季高,夏、秋季低;酸雨的发展趋势受SO₂排放量控制      

中国降水酸度和离子浓度的时空分布

1991～1995年在全国进行了酸雨观测,建立了覆盖全国的具有区域代表性的酸沉降监测网,含271个测站?降水的pH值和电导率在现场采样后立即测量,降水样品的化学分析则在实验室里进行?主要离子SO2-₄,NO-₃,NH+₄,Ca2+浓度的加权均值分别为125.86,19.96,67.89和80.41μeq/L?由离子浓度地理分布图看出,这些离子浓度地理分布状况因离子而异?值得注意的是降水中SO2-₄和NO-₃浓度,北方非酸雨区甚高于南方酸雨区,这说明降水的酸度并不简单地决定于降水中SO2-₄和NO-₃的绝对浓度,而决定于这些离子对于Ca2+和NH+₄的相对浓度?发现了降水年均pH值低至4的一些地区,此值可能是目前世界年降水酸性最强的地区?文中还对代表性地区1986～1993年降水化学特征进行了分析,结果表明降水的酸度仍在升高?      

广州市东郊的降水监测及其理化特征

本文采用1982年至1987年广州市东郊的降水监测资料,初步探讨了该区酸雨污染特征。结果表明:广州市东郊酸雨污染严重,降水酸度逐年上升,雨水中阴阳离子浓度以SO₄2-和NH₄+最高。不同天气系统酸雨频率不同。      

南昌市新城区大气降水化学特征与主要成分来源解析

为了解南昌新城区大气降水化学特性和来源,于2013年5月15日—2014年1月24日采集当地有效降水样品39个,分析其降水化学特性,包括pH、电导率和主要离子(Na+、NH₄+、K+、Mg2+、Ca2+、F-、Cl-、NO₃-和SO₄2-)的浓度.结果表明:南昌市新城区降水pH介于3.67～5.86之间,降水量加权平均值为4.63;电导率在6.13～73.01 μS/cm之间,降水量加权平均值为29.02 μS/cm;降水中总离子浓度为154.1～474.3 μeq/L,降水量加权平均值为300.1 μeq/L.SO₄2-、Ca2+、NH₄+和NO₃-是降水中的主要离子,合计占总离子浓度的82.6%.SO₄2-/NO₃-(当量离子浓度比)在1.82～3.61之间,平均值为2.66.南昌市新城区降水相对酸度为0.43,57.0%的致酸物质被大气中碱性物质中和,主要的酸度中和因子为Ca2+和NH₄+,分别贡献50.0%和36.6%的中和量.阴阳离子三角图分析表明,阴离子主要来自人为源;阳离子来源包括地壳源和人为源.富集系数分析表明,99.5%的Ca2+、88.4%的K+、63.0%的Mg2+来自地壳源;Mg2+、K+、Ca2+的海洋源输入分别为30.7%、4.6%和0.5%;1.2%的Cl-来自地壳源,55.8%来自海洋源,43.0%来自人为源;96.8%的SO₄2-和99.5%的NO₃-来自人为源.研究显示,南昌市新城区的降水为混合型降水,人为源对大气环境产生了重要影响.      

广州地区SO2转化规律及其形成气溶胶特征的研究

为探明广州地区的酸沉降和细粒子气溶胶污染来源,在该地区用室外烟雾箱进行了环境空气中SO₂反应实验研究,其结果表明:影响SO₂转化速率的主要因素是SO₂起始浓度、太阳光强度、相对湿度和空气中颗粒物。SO₂转化速率与箱内凝结核(简称CNC)气溶胶最大浓度密切相关。气态污染物转化是该地区的细粒子空气污染的一个重要来源。      

西安市大气降水污染和沉降特征及其来源解析

基于东亚酸沉降监测网(Acid Deposition Monitoring Network in East Asia,EANET)的湿沉降观测数据,分析了2000～2017年西安市大气降水化学特征、沉降特征以及潜在来源.结果表明,2000～2017年西安市降水pH和电导率的变化分别呈上升和下降趋势;大气降水中离子平均浓度大小依次为SO₄^2-> Ca²⁺> NH₄⁺> NO₃^-> Na+> Cl-> Mg²⁺> K+,其中SO₄^2-浓度占总离子的比值由2000年的38. 6%降低到2017年的27. 9%.近年来的SO₄^2-和NO₃^-的比值表明,西安市大气污染物排放类型有由燃煤型向混合型转变的趋势.近十几年来SO₄     

大气污染物源—接受体关系的数值试验

设计了一个三维欧拉型大气污染物远距离输送的酸沉降模式。利用该模式进行数值试验,讨论污染源排放量的不同减少和背景浓度的不同变化对大气污染物酸沉降的影响。结果表明:污染源排放量和背景浓度对地面SO₂气相浓度和硫酸物湿沉降的影响是非线性的,当污染源中SO₂减少50%,NOx减少40%时,地面SO₂气相浓度最大减少率大于50%;仅仅减少大气污染物的背景浓度,地面SO₂气相浓度和硫酸物湿沉降略有减少,进一步减少污染源排放量,地面SO₂气相浓度和硫酸物湿沉降明显减少。      

珠海市降水化学与沉降特征

为探究珠海市降水及湿沉降的长期变化趋势,基于东亚酸沉降监测网（EANET）的湿沉降监测数据,针对2008—2018年珠海市大气降水量、降水电导率、pH、水溶性离子浓度与湿沉降量进行了降水酸化、降水组分及湿沉降分析.结果表明:①珠海市1—12月降水pH均低于5.6,强酸雨及特强酸雨频率较高,降水酸化问题普遍;2008—2018年pH由4.9增至5.2,总体呈改善趋势;降水电导率小于3 mS/m的月份占61.68%.②珠海市降水中Cl-浓度和Na+浓度较高,二者的区域性特征表明海洋源和人为源共同影响珠海市降水;SO₄2-/NO₃-（浓度比）总体呈逐年递减趋势,降水类型为硫酸-硝酸混合型;较低的ΔpH（酸中和能力评估参数）说明缺乏中和能力可能是珠海降水酸化问题严重的主要原因.③珠海市湿沉降量范围为71.98~200.77 kg/（hm2·a）,其中SO₄2-湿沉降量最高;2008—2018年DIN-N（可溶性无机氮湿沉降量）在11 kg/（hm2·a）上下波动,而SO₄2--S（硫湿沉降量）降幅接近40%;大气氮、硫湿沉降量在春季达到最高.四季NH₄+-N/NO₃--N（铵态氮湿沉降量与硝态氮湿沉降量的比值）均大于1,说明珠海市活性氮主要来源于农业活动.研究显示,珠海市大气降水酸化问题普遍但总体呈改善趋势,严重的降水酸化问题与缺乏中和能力存在一定关系.      

雨季玉龙雪山白水1号冰川表层雪中无机离子特征及环境意义

分析了玉龙雪山白水1号冰川雨季(5-10月)表层雪中无机离子的组成和特征,并与其他高海拔地区湿沉降进行对比。结果表明:白水1号冰川表层雪一定程度上受到了人类活动的影响;由于雨季强烈的淋溶作用,表层雪SO₄^2-含量较低,酸度的主要贡献离子是NO₃^-;pH值较高的原因是碱性金属离子的中和作用;海盐示踪结果显示雨季表层雪中离子来源主要以海源为主。在6-9月之间由于降水的淋洗作用,表层雪中离子浓度较低。表层雪中NO₃^-、SO₄^2-、Ca²⁺高于大多数其他高海拔区域降水,是表层雪中无机离子浓度的主要贡献者,Ca²⁺浓度较高说明该地区高空水汽也受到了局地岩石岩性的强烈影响。     

中国硫沉降数值模拟

采用致酸污染物长距离传输模型ATMOS,对我国2002年排放的SO₂所产生的S沉降分布进行了数值模拟研究.分别将模式输出的ρ(SO₂),SO₄2-湿沉降量与实际监测地面层的ρ(SO₂),降水中SO₄2-湿沉降量进行相关性分析;对我国总S沉降、地面层ρ(SO₂)分布,以及S干、湿沉降分布特点等模拟结果进行详细分析.在此基础上,得到模拟各网格的总S沉降数值,将其与相应的S沉降临界负荷值进行比较,获得95%保证率(RAINS-Asia)下我国1°×1°S沉降超临界负荷分布图.为控制我国的S沉降,对各省SO₂减排的形势进行分析,并提出具体要求.      

中国北方二氧化硫发生源向南方输送模拟研究

酸雨问题是中国的一个环球问题,本研究利用HYSPLIT_4模型模拟了中国北方地区二氧化硫放出后其迁移、扩散、和沉积过程。二氧化硫放出后向周边地区扩散,到达南方长江三角洲的上海市后产生浓度分布和沉积。2001年9月、10月、11月和12月北方放出的二氧化硫对南方影响较大,二氧化硫气团以华北地区为浓度中心向南方迁移,在上海市9月份出现各月垂直层中浓度和地表沉积的最大值,且地表沉积量与0m-500m层的二氧化硫浓度密切相关。     

中国对流层二氧化硫光化学氧化过程的数值研究

利用一个三维非静力区域大气化学输送模式与中尺度气象模式MM5相连接构成一个数值模拟系统，模拟了中国地区对流层臭氧与其前体物的分布以及二氧化硫转化为硫酸盐的过程，模式扬地面源排放、大气输送和扩散、干沉积、气相化学反应和云雨过程。结果表明：日间，O3浓度主要由NOx和NMHC的源排放和光化学反应过程支配，大气辐射是光化学反应强弱的决定因子，其强度可使SO2、O3和SO4^2-的生成浓度呈现不同的日变化和季节变化，结果表明高浓度的O3对二氧化硫转化为硫酸盐的化学过程有很大的促进作用，然而，这种作用受NMHC浓度的影响很大，较高浓度的NMHC使O3浓度上升，但同时增加了对OH等自由基的消耗，使SO2的转化率降低。     

中国酸沉降:来源、影响与控制

总结我国酸沉降观测与模拟、来源与影响以及控制与成效,不仅能为未来我国大气污染治理提供科学依据,也能为国际酸沉降控制提供参考.本文回顾了40年来我国酸沉降研究的发展历程,对有关酸雨时空分布特征、致酸气体排放、土壤和地表水酸化、酸化缓冲机制、临界负荷区划以及酸雨控制对策等研究进展进行综述.我国酸雨污染经历了快速发展、污染缓...     

Measurement and prediction of ozone levels around a heavily industrialized area: a neural network approach

This paper presents an artificial neural network model that is able to predict ozone concentrations as a function of meteorological conditions and precursor concentrations. The network was trained using data collected during a period of 60 days near an industrial area in Kuwait. A mobile monitoring station was used for data collection. The data were collected at the same site as the ozone measurements. The data fed to the neural network were divided into two sets: a training set and a testing set. Various architectures were tried during the training process. A network of one hidden layer of 25 neurons was found to give good predictions for both the training and testing data set. In addition, the predictions of the network were compared to measurements taken during other times of the year. The inputs to the neural network were meteorological conditions (wind speed and direction, relative humidity, temperature, and solar intensity) and the concentration of primary pollutants (methane, carbon monoxide, carbon dioxide, nitrogen oxide, nitrogen dioxide, sulfur dioxide, non-methane hydrocarbons, and dust). A backpropagation algorithm with momentum was used to prepare the neural network. A partitioning method of the connection weights of the network was used to study the relative % contribution of each of the input variables. It was found that the precursors carbon monoxide, carbon dioxide, nitrogen oxide, nitrogen dioxide, and sulfur dioxide had the most effect on the predicted ozone concentration. In addition, temperature played an important role. The performance of the neural network model was compared against linear and non-linear regression models that were prepared based on the present collected data. It was found that the neural network model consistently gives superior predictions. Based on the results of this study, artificial neural network modeling appears to be a promising technique for the prediction of pollutant concentrations.     

Effects of acidic deposition on the erosion of carbonate stone — experimental results from the U.S. National Acid Precipitation Assessment Program (NAPAP)

One of the goals of NAPAP-sponsored research on the effects of acidic deposition on carbonate stone has been to quantify the incremental effects of wet and dry deposition of hydrogen ion, sulfur dioxide and nitrogen oxides on stone erosion. Test briquettes and slabs of freshly quarried Indiana limestone and Vermont marble have been exposed to ambient environmental conditions in a long-term exposure program. Physical measurements of the recession of test stones exposed to ambient conditions at an angle of 30° to horizontal at the five NAPAP materials exposure sites range from ∼ 15 to ∼ 30 μm yr⁻¹ for marble, and from ∼ 25 to ∼ 45 μm yr⁻¹ for limestone, and are approximately double the recession estimates based on the observed calcium content of run-off solutions from test slabs. The difference between the physical and chemical recession measurements is attributed to the loss of mineral grains from the stone surfaces that are not measured in the run-off experiments. The erosion due to grain loss does not appear to be influenced by rainfall acidity, however, preliminary evidence suggests that grain loss may be influenced by dry deposition of sulfur dioxide between rainfall events. Chemical analyses of the run-off solutions and associated rainfall blanks suggest that ∼ 30% of erosion by dissolution can be attributed to the wet deposition of hydrogen ion and the dry deposition of sulfur dioxide and nitric acid between rain events. The remaining ∼ 70% of erosion by dissolution is accounted for by the solubility of carbonate stone in rain that is in equilibrium with atmospheric carbon dioxide (“clean rain”). These results are for marble and limestone slabs exposed at an angle of 30° from horizontal. The relative contribution of sulfur dioxide to chemical erosion is significantly enhanced for stone slabs having an inclination of 60° or 85°. The dry deposition of alkaline particulate material has a mitigating effect at the two urban field exposure sites at Washington, DC, and Steubenville, OH.     

安阳市区二氧化硫污染总量控制研究

在充分调查的基础上,结合市区经济、社会发展远景目标纲要和城市总体发展规划,预测了近期、中期、远期SO₂排放量和控制总量,确定了SO₂排放总量与环境空气质量之间的相应关系,并以改善市区环境空气质量为目标,提出了不同阶段的综合防治方案,为实现国务院提出的对“两控区”的控制目标奠定了基础。SO2防治方案已经安阳市人民政府批准实施。      

西安市二氧化硫减排与环境空气质量相关性分析

历年环境统计数据和环境监测数据表明,2006年以来西安市二氧化硫排放量大幅下降,空气中二氧化硫浓度也呈下降趋势,空气质量有所改善,但由于减排措施实施的区域和力度的差异,不同典型监测点位二氧化硫浓度变化情况不尽相同,与我国北方其他省会城市相比,二氧化硫排放量虽然降幅较大,但城市空气中二氧化硫浓度降幅偏小,且工业减排量占总减排量的比例相对较小,因此,今后应高度关注二氧化硫减排工作中存在的问题,不断完善环境管理,多渠道多途径全面提升城市环境空气质量。     

广东、广西地区酸沉降统计模式的研究

介绍了两广地区酸沉降模式,该模式的基础是定常欧拉型酸沉降模式,其中包括硫污染物的人工排放源,扩散输送,化学转化和干湿沉降,对全年120天气象资料进行计算和平均以后,得到广东、广西地区硫沉降的基本图象.从模式计算的结果可以看出,在目前低空排放(排放源在300m以下)的条件下,城市污染源排放的硫污染物的输送范围约10~2km量级、污染物的浓度及干湿沉降量都有显著的非均匀分布.     

Acid deposition and its effects in China: an overview

Acid rain is an increasing environmental problem in China. At present SO₂ emission is about 20–22 million tons. However with a growing number of large power plants the long-range transport of air pollutants is expected to increase. The highest acid deposition is near the emission sources. Wind-blown, alkaline soil dust is important in neutralizing the acidity of the emissions, especially in large parts of northern China. In the south, where alkaline soil dust contributes less to acid neutralization, the annual pH in precipitation was below 4.5 at monitoring stations in several provinces and as low as 4.1 in some urban areas. Total sulfur deposition has been estimated to be about 10 g S m−² year⁻¹ in heavily exposed areas. Negative effects on forests, including die-back, have been reported for relatively small areas near large cities. Since large, regional surveys have not been carried out, there are large uncertainties about effects on a regional level. The high concentrations of gaseous pollutants, especially within and near the cities, are likely to have severe effects on human health as well as on materials and vegetation. Several field and laboratory studies, as well as computer simulations, indicate that acidification of soil and soil water has occurred in the past few decades. This has probably caused elevated concentrations of toxic aluminum in soil water. At present, the toxic effect of Al is likely to be counteracted by high concentrations of calcium at many places. The Chinese authorities have recognized air pollution and acid rain as serious environmental problems, however, there are difficulties in implementing effective measures to reduce the problems. With respect to ecological effects we lack a comprehensive regional overview of the extent of the acid deposition problem in China. Such information is necessary before effective countermeasures can be developed.