The removal of sulphur dioxide in a long-lived line echo system: A numerical study

The removal of SO₂ in precipitation systems is not only a major sink of SO₂ but is also directly related to the acidity of precipitation. However the physical and chemical processes are not well understood due to their complicated characteristics. The lack of measurements also hinders us from studying those processes. In order to investigate what mechanisms are important about the removal of SO₂ in precipitation systems, an alternative approach is to examine the simulation result from a numerical cloud model.A two-dimensional version of the Klemp-Wilhelmson numerical model (1978, J. atmos. Sci.35, 1070–1096) is used to simulate a fast-moving long-lived line echo precipitation system that occurred in the Taiwan area during Mei-Yu season. The simulation model was assumed to be perpendicular to the north-south orientated line echo. In this simulation an artificial source of SO₂ is placed in front of the line echo system in the low level. As the line echo system approaches the region of SO₂, some SO₂ is brought into the line echo system through advection and diffusion effects. A simple parameterization scheme similar to Fisher's (1982, Atmospheric Environment16, 775–783) is used to represent the removal of SO₂ by cloud and rain. The model results show that the major sink of SO₂ is removed by rain below the cloud base although some is removed by cloud and rain inside the precipitation system itself.     

Chemical composition of rain in Thessaloniki,Greece, in relation to meteorological conditions

Wet precipitation was collected in Thessaloniki, Greece, during the period March 1989–December 1990 by using an automatic wet-only precipitation sampler.Rainwater samples were analysed for major cations (H⁺, NH₄⁺, Na⁺, K⁺, Ca²⁺, Mg²⁺) and anions (Cl⁻, NO₃⁻, SO₄²⁻), in addition to acidity and conductivity measurements. The majority of rain had a neutral or alkaline character as a result of neutralization, primarily caused by calcareous soil dust and secondarily by atmospheric ammonia. In all rain, SO₄²⁻ concentration exceeded NO₃⁻ concentration. The contribution of maritime sources to the total SO₄²⁻ concentration was very low (<2%).The chemical composition of precipitation was analysed in conjunction with meteorological variables (season of the year, precipitation type, airflow patterns) to evaluate temporal variations and chemical source influence. Rain caused by weak, localized flows showed the highest acidity and the minimum influence of neutralization processes.     

酸雨对两广地区农作物的经济损失研究

本研究通过模拟试验和现场调查,确立两广地区主要农作物对酸性降水、SO₂单一污染,酸性降水与SO₂复合污染的产量反应生态基准值。根据酸性降水年均pH和SO₂年日均浓度等值线,农作物的空间分布,采用市场价格法,估算了酸雨引起两广地区农作物经济损失值。      

SO2排放造成的森林损失计算:以湖南省为例

SO₂排放对我国的森林生态系统造成了严重的损害,因而损失计算对于SO₂控制具有重要意义,但是目前仍缺乏有效的方法计算不同排放水平下的森林损失.本研究以硫沉降超临界负荷作为计算森林损失的参数,推导了适用于我国硫沉降导致森林损失的剂量-响应函数,并以湖南省为例,以1995为基准年,计算了2000年～2020年高中低3种SO₂排放方案下的森林损失.研究结果表明,随着今后湖南省经济和能源消费的增长,森林损失将继续增加.高排放方案下2020年SO₂排放将增长1.2倍,但森林损失增长4.3倍,边际损失高于6000元/t.在当前排放水平下对SO₂排放进行削减,边际效益达到1500元/t,因此控制SO₂具有显著的经济效益.对湖南案例的不确定性分析显示,计算方法有较高的可靠性.研究结果为区域SO₂控制策略的优化提供了支持.     

成渝经济区火电发展的大气环境影响

基于CALPUFF模型,以2007年为基准年,根据成渝经济区基准年火电SO₂排放量、2008—2009年国家核定的火电SO₂减排量(20.9×104 t)、“十二五”年地方计划火电SO₂减排量(18.5×104 t)以及地方愿景下的“十二五”期间新增火电SO₂排放量,设计3种不同排放情景,并且对不同情景下的ρ(SO₂)分布特征进行了模拟. 结果表明:2008年和2009年成渝经济区的火电SO₂减排使成渝经济区的ρ(SO₂)年均值比2007年平均降低了18.9%;“十二五”新增火电装机将会使成渝经济区的ρ(SO₂)年均值比2007年平均升高20.7%. 虽然通过工程减排及“上大压小”的方式减缓了新增火电机组带来的影响,但从空间分布来看,ρ(SO₂)增加的局部地区与酸雨严重的地区高度重合,导致该区域酸雨污染风险依然存在.      

桂林市酸雨污染特征及防治对策研究

为促进桂林市酸雨污染防控,利用2013—2017年桂林市3个监测站点采集的共1 147个降雨样品,分析了降雨pH、电导率和水溶性离子成分,结合气态污染物的变化特征和气象因素影响分析,探讨了桂林市酸雨污染成因,并提出了桂林市酸雨污染防治对策建议.结果表明:①2013—2017年桂林市降雨的pH年均值范围为4.85~5.23.酸雨频率范围为42.5%~74.9%,2017年酸雨频率达74.9%.虽然近年来桂林市环境空气质量明显改善,但是酸雨污染却没有明显减轻,反而在2015年后出现恶化.降雨的离子组成中,SO₄2-和NO₃-是主要的阴离子成分,分别占总离子当量浓度的28.19%和10.82%;Ca2+和NH₄+是主要的阳离子成分,分别占总离子当量浓度的23.46%和17.64%.酸中和效应分析显示,Ca2+和NH₄+为降雨中主要的中和物质.②降雨中碱性离子当量浓度的降幅比酸性离子当量浓度的降幅大,这是导致桂林市近年酸雨恶化的重要因素;此外,来自西部和东南部方向的气流对应了较高的降雨酸度和总离子当量浓度,因此污染物的远距离传输对降雨酸度和离子当量浓度也有一定影响.研究显示,桂林市SO₂和NO_x排放的持续管控将有利于酸雨污染防治,但桂林市目前实施的削减大气粗颗粒物和NH₃排放的大气污染控制策略对于降雨酸度的影响还需要开展进一步评估.      

酸沉降对非金属建筑材料腐蚀机理的探讨

将酸雨对非金属建筑材料的整个腐蚀过程分为腐蚀初期、中期和末期3个腐蚀阶段,进而提出腐蚀机理。对整个腐蚀过程探讨表明:酸雨对材料的腐蚀是酸雨中H+和SO2₄-共同侵蚀作用的结果;H+将溶解硬化水泥石中的Ca(OH)₂,SO2₄-将与硬化水泥石作用生成膨胀性的物质CaSO₄·2H₂O。因此,酸雨对非金属建筑材料的腐蚀,主要是H+引起溶解腐蚀和SO2₄-引起的膨胀腐蚀。      

浙江宁波天童地区酸性降水化学特征研究

为了解浙江宁波天童地区降水的化学特征、离子来源及酸性降水的成因,于2010年3月—2011年2月在该地区采集了90个降水样品,并运用离子色谱法分析其化学组分.结果显示,天童地区降水的酸化频率和酸化程度非常高,酸雨频率为97%,雨量加权pH平均值为4.37,离子浓度的大小顺序为SO24->NH4+>NO3->Ca2+>Cl->Na+>Mg2+>K+>F-,降水较清洁;降水pH值和各离子含量存在明显的季节变化,总体表现为冬、春季污染程度高于夏、秋季;SO24-/NO3-的浓度比值为1.9,表明该地区酸雨类型为硫酸和硝酸复合型;SO24-、NO3-、NH4+和部分Ca2+主要来自人为污染源,Na+、Cl-和大部分Mg2+主要来自海洋源,K+和大部分Ca2+则主要来自地壳源,海洋对天童地区降水离子组分影响较大,但对降水酸度影响并不显著;NH4+与SO42-(r=0.90)、NO3-(r=0.88)的相关性分别大于Ca2+与SO24-(r=0.67)、NO3-(r=0.73)的相关性,且NH4+/Ca2+的浓度比值为1.47,说明NH4+对降水酸性的中和作用大于Ca2+,与我国其他城市降水相比,天童地区降水中的碱性离子,尤其是Ca2+浓度较低,从而导致降水酸度高于北方地区和西南其他地区.     

广州地区雨水化学组成与雨水酸度主控因子研究

采集了广州地区2003-10～2004-09的雨水样品,通过对雨水样品的pH值、主要阴阳离子组成和可溶性有机碳(DOC)的测定,分析了广州地区酸雨的现状以及影响雨水酸度的主要因素等.结果表明,在观测期间,广州地区酸雨频率高达85%;雨水的主要离子组成为NH₄⁺、SO₄^2-、NO₃^-、Ca²⁺、Cl^-和Na⁺,而DOC约占总化学组成的24.0%;雨水酸度的主要控制离子还是SO₄^2-,但NO₃^-对雨水酸度的影响越来越大;同时,水溶性有机酸对雨水酸度的贡献也很明显.另外,来自扬尘中高浓度的碱性含钙化合物也对雨水酸度有明显的中和作用.     

北京市典型区域夏季降水及其对大气污染物的影响

通过采集北京市典型区域2015年夏季大气降水样品,分析研究了大气降水的理化特性,典型降水过程化学组分的变化特征、成因以及对大气污染物的影响.结果表明,北京市典型区域夏季降水pH值范围为5.15~7.34,雨量加权平均值为6.21,酸雨率极低.降水中污染元素Cd、Ca和Mn呈现中度富集,Cu、Zn、Pb和S呈现严重富集;Ca和S是降水中主要污染元素,分别占总污染元素浓度的45.43%和43.93%,Zn、Mn、Cu、Pb和Cd是降水中主要重金属污染元素,占总污染元素浓度的1.32%.降水速率不同的降水对大气污染物的影响作用也有所不同.降水速率较大的降水对PM_(2.5)的清除作用较小,对SO_2、NO_2和O_3的清除作用较大,且影响机制表现为4个重要过程:大气污染物的清除、累积、累积和清除、清除.降水速率较小的降水主要以云内雨除为主,对PM_(2.5)、SO_2、NO_2和O_3的云下清除作用较小,且影响机制表现为:污染物的清除、清除和累积、累积、以及清除为特征的4个重要过程.降水速率较大的降水对大气污染物的清除作用大于降水速率较小的降水.     

V2O5/AC催化剂脱除烟气中SO2的微观动力学研究

利用热重分析仪对V2O3/AC脱除SO2的微观动力学进行了研究,考察了催化剂V2O5的含量[w(V2O5)]、反应物SO2和H2O的浓度[ψ(SO2)和ψ(H2O)]及反应温度对催化剂增重分率的影响,并采用微孔填充模型描述V2O5/AC的脱硫行为.模型研究表明:V2O5/AC脱除SO2反应速率由吸附-催化剂表面化学反应控制,SO2和H2O的吸附可用Langmuir-Hinshelwood模型分析.将活性组分表面分率和V2O5/AC的微孔孔容随反应的变化用参数n表示,n类似于反应级数,以表示二者对反应的影响程度.     

近3年太原市夏季降水的化学特征研究

本研究采集了2011~2013年太原市夏季66场降水样品,分析了p H值、电导率和水溶性阴阳离子,探讨了太原市夏季降水的化学组成及来源.结果表明,近3年太原市夏季降水p H值范围为4.63~8.02,加权平均值为5.19;2011~2013年酸雨频率分别为37.0%、31.2%和17.4%.太原夏季降水的化学组成以SO2-4、NO-3、Ca2+和NH+4为主,阴离子SO2-4和NO-3加权平均浓度分别占阴离子总浓度的67.2%和22.0%,阳离子Ca2+和NH+4加权平均浓度分别占阳离子总浓度的55.1%和29.0%;降水中SO2-4、NO-3、Ca2+和NH+4浓度水平随年度有明显的下降趋势.近3年SO2-4/NO-3的当量浓度比分别为2.97、3.06和3.08,平均值为3.02,说明太原市夏季酸性降雨类型为硫酸和硝酸复合型,且硝酸盐的贡献逐年增强.通过中和因子分析,表明太原市夏季降水中Ca2+和NH+4对酸性中和起主导作用,但Mg2+的作用不可忽略.太原市夏季降水中水溶性化学组分主要与燃煤排放有关;结合气团的后向轨迹分析表明太原市夏季降水主要受山西省内南部低空运行的短距离输送气团的控制;西南和东南气团是太原市夏季降水中水溶性化学组分的主要来源.为了有效改善太原市的空气质量,太原南部及本地焦化企业和燃煤电厂污染物的排放应给予关注.     

Numerical modeling of long-range transport of acidic species in association with mesoβ-convective-clouds across the Japan sea resulting in acid snow over coastal Japan—II. Results and discussion

The acid snow/rain model [describedin Part I, Kitada et al., Atmospheric Environment27A, 1061–1076, 1993] was applied to investigate transport/transformation/deposition of acidic species in association with snow-precipitating cloud over the Japan Sea in winter. The model results showed: (1) The snow-precipitating clouds generated by relatively weak convective motions tend to trap aerosols of sulfate and nitrate and soluble gases such as SO₂ and HNO₃ below cloud levels, thus keeping their concentrations at higher levels than those for no-cloud situations. The mechanisms involved are: transfer of gas- and aerosol-phase species to cloud-phase through absorption and nucleation scavenging, then their transfer from cloud to snow through riming, and subsequent release from sublimating snow back to gas- and aerosol-phases below cloud base. (2) In-cloud oxidation enhanced the overall conversion of SO₂ to SO₄²⁻ by some 25% with respect to no-cloud situation after 12 h. Furthermore, contributions to the oxidation were 77.4%, 21.1% and 1.5% for S(IV)H₂O₂, S(IV)O₂ with catalysts of Fe³⁺ + Mn²⁺ and S(IV)O₃ reactions, respectively. (3) The sulfate wet deposited by precipitating snow for 12 h was due mostly to in-cloud scavenging and in-cloud oxidation, i.e. 66% by nucleation scavenging and the remaining by in-cloud oxidation of S(IV), while the contribution of below-cloud scavenging was negligible. (4) The adsorption process of HNO₃ onto the surface of falling snow was found to account for major below-cloud scavenging of snow, and thus in contrast to SO₄²⁻, the below-cloud scavenging contributed very significantly to the nitrate wet deposition. Throughout the stimulation, below-cloud scavenging was responsible for 75% of the snow-NO₃⁻ formation. Therefore, taking account of this process in acid snow models is important.     

马莲河流域河水化学特征和化学风化过程分析

采用Gibbs图解和端元分析方法研究了马莲河水化学特征、离子来源和化学风化作用,利用质量平衡正演模型评价了各风化作用对水化学组分的贡献率。结果表明,马莲河水为高TDS咸水,阳离子以Na~+、Mg~(2+)为主,阴离子以Cl~-、SO_4~(2-)为主;沿河水流向TDS降低,水化学类型由Cl-Na型演变为HCO_3·SO_4-Na·Mg型;河水化学组分的主要形成作用为化学风化,蒸发盐主导了流域风化过程,对离子组分平均贡献率高达76.5%,硅酸盐和碳酸盐风化较弱;化学风化具空间变异,从上游到下游,硫酸盐和碳酸盐贡献率增加,岩盐贡献率降低。岩性是控制流域化学风化作用的首要因素,降雨量和径流量可能也有一定影响。     

Numerical simulation of wet scavenging of air pollutants—II. Modeling of rain composition at the ground

The modeling of rain composition for a convective shower (Tucson, AZ, 10 September 1977) and a frontal precipitation event (Den Helder, Holland, 12 December 1978) is performed in this paper by including the pollutant species and wet scavenging mechanisms into the mass transport equation of the sequential sampling model described in Part I of this series. The results indicate that: (1) the major scavenging mechanisms of most pollutants in convective showers appear to be similar to those in frontal precipitations; (2) the major scavenging mechanisms of NH₄ and NO₃ are gas absorption, whereas the absorption of SO₂ by aqueous drops and oxidation of S(IV) by H₂O₂ and O₃ in the aqueous phase are the major formation and scavenging mechanisms for SO₄; (3) the scavenging by raindrops in the below-cloud region is the dominant removal mechanism for coarse particles, whereas nucleation is the major scavenging mechanism for submicrometer particles; (4) H₂O₂ is the most important oxidant responsible for the oxidation of S(IV) and the formation of sulfate in precipitation; (5) the contributions of both (SO₂ + H₂O₂) and (SO₂ + O₃) reactions to sulfate concentration in precipitation are larger for convective precipitation than for frontal precipitation.     

Parameterization of episodical cloud and rainout events in large-scale atmospheric chemistry models

A parameterization scheme taking into account the episodical nature of rainout and incloud chemical transformation has been tested in a 2-D channel model. In the liquid phase many soluble gases are observed in concentrations never experienced in the gas phase. The effects on the trace gases SO₂ and hydrogen peroxide, when they are modified by clouds and precipitation, are studied. When incloud interaction of SO₂ and hydrogen peroxide is taken into consideration, calculated hydrogen peroxide profiles are brought closer to observed distributions. The effect of varying the time periods between cloud and rain events is tested. The impact on the formation and destruction of tropospheric ozone is also discussed.     

钠盐对高负荷餐厨垃圾和剩余污泥中温厌氧混合发酵过程的抑制作用

针对高负荷餐厨垃圾和剩余污泥混合发酵系统在实际应用过程中存在的盐度抑制问题,通过批次试验探究了不同钠盐（CH₃COONa、NaCl和Na₂SO₄）对中温混合发酵体系的影响,考察了添加不同浓度钠盐时混合发酵体系的甲烷累积产量、有机物去除率、挥发性脂肪酸（VFAs）累积量及水解、酸化、乙酸化和产甲烷速率的抑制作用.结果表明,随着CH₃COONa浓度的增加,相应的甲烷产量逐渐增加,但在高浓度时理论甲烷产量降低,当Na⁺浓度为8 g·L^-1时,对产甲烷抑制率为21%.此外,NaCl和Na₂SO₄对甲烷累积产量具有抑制作用,相同Na⁺浓度下,Na₂SO₄对混合发酵体系甲烷产量的抑制作用更大;当SO₄^2-浓度为8.3 g·L^-1时,相应甲烷抑制率为23%.相反,Cl^-浓度为3.1~6.2 g·L^-1时,对混合发酵过程中甲烷抑制率为4.6%~7.7%;但随着Cl^-浓度增至9.3~12.3 g·L^-1时,甲烷产量提升了14.5%~37.6%.分析认为,NaCl对混合发酵过程有机物去除率的抑制作用主要是Na⁺的影响,而Na₂SO₄的抑制作用主要来源于SO₄^2-和Na⁺的协同作用.NaCl和Na₂SO₄对水解速率和产甲烷速率的抑制作用较大,而对酸化速率和乙酸化速率抑制作用较小.