珠江三角洲地区冬季硫、氮干沉降的来源解析

采用WRF-CMAQ模式对珠江三角洲地区2015年1月进行数值模拟,结合CMAQ的集成源解析方法ISAM对S、N及其干沉降的来源贡献进行分析.结果表明：珠江三角洲地区S、N干沉降量高值主要分布在广佛交界处以及珠江口附近,其逐日变化趋势主要受质量浓度变化影响,但在部分时间段受干沉降速率的影响亦相当显著.珠江三角洲区域内排放源对于S干沉降的平均贡献占比为36.2%,与其质量浓度区域内贡献占比相当,SO₂干沉降速率增加以及背景风场变弱会使区域内贡献占比增加;区域内源对于N干沉降的平均贡献占比为32.4%,远小于其质量浓度区域内贡献占比,当NO₂质量浓度减少,使得HNO₃的质量浓度和干沉降量减少时,区域内贡献占比增加.对于珠江三角洲典型城市,广州S干沉降的本地贡献为27.7%,N为14.2%;江门S干沉降的本地贡献为9.6%,N为8.8%.2个城市对比而言,广州受本地的影响较江门显著,江门受其上风方向广州和佛山两市输送的影响显著,但当背景风场减弱时,江门本地贡献会有明显增加.     

珠江三角洲地区冬季硫、氮干沉降的来源解析

采用WRF-CMAQ模式对珠江三角洲地区2015年1月进行数值模拟,结合CMAQ的集成源解析方法ISAM对S、N及其干沉降的来源贡献进行分析.结果表明：珠江三角洲地区S、N干沉降量高值主要分布在广佛交界处以及珠江口附近,其逐日变化趋势主要受质量浓度变化影响,但在部分时间段受干沉降速率的影响亦相当显著.珠江三角洲区域内排放源对于S干沉降的平均贡献占比为36.2%,与其质量浓度区域内贡献占比相当,SO₂干沉降速率增加以及背景风场变弱会使区域内贡献占比增加;区域内源对于N干沉降的平均贡献占比为32.4%,远小于其质量浓度区域内贡献占比,当NO₂质量浓度减少,使得HNO₃的质量浓度和干沉降量减少时,区域内贡献占比增加.对于珠江三角洲典型城市,广州S干沉降的本地贡献为27.7%,N为14.2%;江门S干沉降的本地贡献为9.6%,N为8.8%.2个城市对比而言,广州受本地的影响较江门显著,江门受其上风方向广州和佛山两市输送的影响显著,但当背景风场减弱时,江门本地贡献会有明显增加.     

An overview of emissions of SO2 and NOx and the long-range transport of oxidized sulfur and nitrogen pollutants in East Asia

The long-range transport of oxidized sulfur(sulfur dioxide(SO_2) and sulfate) and oxidized nitrogen(nitrogen oxides(NO_x ) and nitrate) in East Asia is an area of increasing scientific interest and political concern. This paper reviews various published papers, including ground- and satellite-based observations and numerical simulations. The aim is to assess the status of the anthropogenic emissions of SO_2 and NO_x and the long-range transport of oxidized S and N pollutants over source and downwind region. China has dominated the emissions of SO_2 and NO_x in East Asia and urgently needs to strengthen the control of their emissions, especially NO_x emissions. Oxidized S and N pollutants emitted from China are transported to Korea and Japan, due to persistent westerly winds, in winter and spring.However, the total contributions of China to S and N pollutants across Korea and Japan were not found to be dominant over longer time scales(e.g., a year). The source–receptor relationships for oxidized S and N pollutants in East Asia varied widely among the different studies. This is because:(1) the nonlinear effects of atmospheric chemistry and deposition processes were not well considered, when calculating the source–receptor relationships;(2) different meteorological and emission data inputs and solution schemes for key physical and chemical processes were used; and(3) different temporal and spatial scales were employed. Therefore, simulations using the same input fields and similar model configurations would be of benefit, to further evaluate the source–receptor relationships of the oxidized S and N pollutants.     

被动采样法表征降水离子浓度和通量的局限性

降水(湿沉降)是大气污染物进入地表环境的主要途径,由于传统的被动采样法易受到颗粒物和气体干沉降的干扰,而采集到的混合沉降样品不能科学表征降水化学组成,也不能准确量化湿沉降通量,因此目前正逐步被主动采样法所取代. 采用主动和被动2种采样法同步采集了降水样品,以考察被动采样法表征降水离子浓度和通量的适用性. 结果表明:被动采样法采集的降水样品中离子浓度明显偏高,其中ρ(NO₃-)、ρ(Mg2+)、ρ(Ca2+)、ρ(K+)、ρ(Cl-)、ρ(SO₄2-)、ρ(Na+)和ρ(NH₄+)分别比主动采样法高65%、58%、43%、41%、35%、26%、10%和9%. 受大气污染物干沉降影响,被动采样法获得的NO₃-、NH₄+和SO₄2-混合沉降通量分别比主动采样法获得的湿沉降通量高79%、18%和35%,差异最显著的是NO₃-. 被动采样法可以收集氮和硫的湿沉降,但不能有效捕获二者以颗粒物和气体形式发生的干沉降,对二者沉降总通量(干沉降通量+湿沉降通量)低估达39%〔23 kg/(hm2·a)〕和40%〔20 kg/(hm2·a)〕. 因此,鉴于大气污染形势日趋严重,污染物的干沉降作用凸显,被动采样法已难以准确测算污染物从大气向地表的沉降总通量,需要全面考虑细颗粒物(粒径≤2.5 μm)和气态物种(如HNO₃)的贡献.      

The influence of long term trends in pollutant emissions on deposition of sulphur and nitrogen and exceedance of critical loads in the United Kingdom

In the United Kingdom, as with other European countries, land-based emissions of NO_x and SO₂ have fallen significantly over the last few decades. SO₂ emissions fell from a peak of 3185 Gg S in 1970 to 344 Gg S in 2005 and are forecast by business-as-usual emissions scenarios to fall to 172 Gg by 2020. NO_x emissions were at a maximum of 951 Gg N in 1970 and fell to 378 by 2005 with a further decrease to 243 Gg N forecast by 2020. These large changes in emissions have not been matched by emissions changes for NH₃ which decreased from 315 Gg N in 1990 to 259 in 2005 and are forecast to fall to 222 by 2020. The Fine Resolution Atmospheric Multi-pollutant Exchange model (FRAME) has been applied to model the spatial distribution of sulphur and nitrogen deposition over the United Kingdom during a 15-year time period (1990–2005) and compared with measured deposition of sulphate, nitrate and ammonium from the national monitoring network. Wet deposition of nitrogen and sulphur was found to decrease more slowly than the emissions reductions rate. This is attributed to a number of factors including increases in emissions from international shipping and changing rates of atmospheric oxidation. The modelled time series was extended to a 50-year period from 1970 to 2020. The modelled deposition of SO_x, NO_y and NH_x to the UK was found to fall by 87%, 52% and 25% during this period. The percentage area of sensitive habitats in the United Kingdom for which critical loads are exceeded is estimated to fall from 85% in 1970 to 37% in 2020 for acidic deposition and from 73% to 49% for nutrient nitrogen deposition. The significant reduction in land emissions of SO₂ and NO_x focuses further attention in controlling emissions from international shipping. Future policies to control emissions of ammonia from agriculture will be required to effect further significant reductions in nitrogen deposition.     

Optimising the environmental benefits of emission reductions from UK coal- and oil-fired power stations: a critical loads approach

This paper describes a method for determining reductions of SO₂ emissions from coal- and oil-fired power stations, oil refineries and large industrial units in the UK taking into account their pollution potential. The method is based on the use of two gridded data sets: critical loads, which represent the sensitivity of the environment to acid deposition and modelled estimates of total (wet + dry) sulphur deposition for 646 point sources within the UK. An iterative method is used to identify and subsequently reduce emissions from point sources that contribute most to areas of critical loads exceedance. This paper demonstrates how the method may be used to determine an optimal allocation of emissions across the UK which yields the maximum amount of environmental protection per unit of emission.The paper then goes on to consider the changes that will have to take place within the UK power generation industry in order to meet the revised EC Large Combustion Plant Directive which comes into force on 1 January 2008. Particular emphasis is placed upon proposed emissions trading schemes and the environmental implications of allowing trading between stations with high and low pollution potentials. The paper concludes by suggesting that the emissions trading process should take into account the pollution potential of each source, irrespective of whether the proposed emission is within the plant's agreed emission limit. An approach based entirely on minimizing environmental damage rather than one which takes cost into account, as in current integrated assessment modelling, could provide an interesting approach across the rest of Europe.     

2010年中国大气氮沉降特征分析

利用区域空气质量模式Models-3/CMAQ对我国2010年的氮沉降特征进行了模拟分析.结果表明,2010年我国氮沉降总量约为7.6′ 103Gg,化学组成上以NHx-N(包括NH3、NH4+中的氮)沉降为主,平均占到2/3以上.夏季氮沉降量最高,冬季最低.干沉降为氮沉降的主要途径(约占62%),主要为气态含氮污染物的贡献,湿沉降的氮则主要来自颗粒态的铵盐和硝酸盐.我国氮沉降的空间分布具有东高西低、地区间差异显著的特征,高沉降通量区域主要集中在华北平原、四川盆地、华中的中南部、两广以及东北部分地区.加强对氨排放的管理和控制,同时重视东部沿海的发达地区的氮氧化物排放,对减少氮沉降具有重要意义.     

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...     

大气中硫污染物的干沉降模式

建立了计算ＳＯ２和硫酸盐气溶胶干沉降速度的数值模拟,模式中考虑了气象条件,下垫面特征等因素对不同污染物干沉降速度的影响。并利用该模式计算了垫面上ＳＯ２和ＳＯ４＾２－的干沉降速度,其变化范围分别为０．２－１．０ｃｍ／ｓ和０．１－０．８ｃｍ／ｓ,与文献给出的结果对比表明,该模式散于计算硫污染物的干沉速度是可行的,最后给出了包括我国大部分地区白天和夜晚的硫污染物干沉降速度的区域分布。     

Atmospheric sulfur and nitrogen budgets for southeast Europe

This paper presents atmospheric sulfur and nitrogen budgets for the region of southeast Europe, including Albania, Bulgaria, Greece, Italy, Romania, the western part of th Anthropogenic and natural emission fluxes are estimated from information in the literature; wet and dry deposition fluxes are determined from both EMEP measurements and modelling results and the input and output terms are based on EMEP modelling results. For sulfur, the total inputs and outputs for the region range from 3.8 to 4.4 and 4.0 to 7.2 Tg Sy⁻¹, respectively; for nitrogen, the inputs and outputs are 2.1 to 3.8 and 2.0 to 6.6 TgNy⁻¹, respectively. On average, the nitrogen fluxes consist of approximately equal parts of oxidized and reduced forms. Despite the presence of strong upwind sources, anthropogenic emission within the region dominate the inputs, accounting for approximately 70% of the total inputs for both S and N. The three output terms, outflow, wet and dry de'position, are of similar magnitude for both species, but all have considerable uncertainties (ca 50%). The cycling of S and N in the atmosphere of southeast Europe has common features with that in eastern North America and west-central Europe, in that anthropogenic S and N dominate the natural cycles of these substances, anthropogenic emissions within the region significantly exceed inflows to the region, and the region is a net exporter of S and N species.     

Atmospheric concentrations and deposition of nitrogen and major ions in conifer forests in the United States and Federal Republic of Germany

Emission densities of air pollutants are higher in Europe than in the U.S. as a whole, suggesting similar differences in atmospheric deposition. We determined air concentrations and deposition during the warm season at conifer forests in Tennessee and northern Germany. Our results confirmed major differences in both chemistry and fluxes. Atmospheric and precipitation concentrations of all ions except H⁺ were higher at the German site, most significantly for the nitrogen species. The much higher levels of NH₄⁺ at this site reflect higher emissions of NH₃, which was the species largely responsible for the lower levels of H⁺. Total airborne nitrate was dominated by HNO₃ in Tennessee. In Germany we found comparable amounts of HNO₃ and aerosol NO₃⁻, the concentration of which varied seasonally, apparently in response to agricultural emissions of NH₃ that reacted to form NH₄NO₃. Total deposition of all major ions was much higher at the German site, particularly for the nitrogen species, which exhibited a marked edge effect in throughfall. Dry deposition was determined from air concentrations by using a canopy resistance model and from a statistical model of throughfall fluxes, each of which yielded comparable fluxes for several ions. Dry deposition contributed 10–70% of the ion input and was most important at the German site. Both forest canopies absorbed 40–50% of total deposited nitrogen, primarily from dry deposition.     

Nitrogen budget for eastern Canada

A Lagrangian model incorporating S and N chemistry has been developed by the Atmospheric Environment Service. It was used to produce an annual nitrogen budget including annual nitrogen transboundary flux estimates for 1980 for eastern Canada.The model used trajectories computed from the analyzed winds produced at the Canadian Meteorological Centre (CMC) in addition to the temperature and precipitation analyses. The model parameterized the dry and wet deposition and chemical transformation of NO₂, nitrate (including HNO₃) and PAN using monthly, time-dependent dry deposition velocities, scavenging ratios and transformation rates. The model was integrated throughout eastern Canada on a 6-h basis for 1980. The boundary point concentrations were used to compute input and output fluxes which were summed over several boundary segments to give annual transboundary flux estimates.The total annual N deposition was about 0.6 TgN with high deposition in August and December and the lowest in February. Wet NO₃⁻ deposition (0.2 TgN) was higher than the dry deposition of any single N species (NO₂, nitrate or PAN) but lower than all dry N deposition combined. The annual N input (output) flux was about 1.0 (0.5) TgN. The highest input and output fluxes occurred in December and the lowest input and output fluxes occurred in May.     

Emissions of SOχ, NOχ, VOC and CO from East European countries

For the purpose of model calculations of long-term ozone levels over Europe a database, resembling that of the PHOXA project (PHotochemical OXidant and Acid deposition model application) and an inventory of SO_χ, NO_χ, VOC and CO emissions from main source types has been prepared for the reference year 1985 for all European Countries. The U.S.S.R. was included to 60° east longitude. Emissions from OECD and CEC member countries could be taken and updated where necessary, from recently compiled inventories. Emissions from East European countries, however, were only available in a form too aggregated to be applicable for the project. In this paper, the estimation of emissions from these countries is described and possibilities for improvement are discussed. This emission inventory is the first one for Eastern Europe with a rather complete structure including composition profiles of pollutants, temporal allocation procedures and temperature relations.     

基于CMAQ模式的中国大气BaP迁移转化模拟研究

在空气质量模式CMAQ中增加了对大气中苯并[a]芘(BaP)传输、转化和沉降过程的模拟,新增了BaP气相/颗粒相间分配模式(K_OA吸收模式)以及BaP化学转换,并采用该模型模拟了2014年1、4、7、10月四个季节代表月中国大气中BaP的浓度以及干湿沉降通量的空间分布特征.模拟结果与部分地区的实测数据进行了初步对比验证,结果显示BaP浓度的模拟值和测量值的量级基本一致,其比值基本在1~2个量级范围内,表明模拟结果处于可接受的范围.基于模型结果,还探讨了BaP浓度与沉降季节变化特征与人为源排放的紧密联系,说明湿沉降是BaP最主要的沉降途径.BaP沉降的空间分布与其排放源和浓度具有密切的联系,并且具有长距离输送的特征等.     

The stem-II regional scale acid deposition and photochemical oxidant model—IV. The impact of emission reductions on mesoscale acid deposition in the lower ohio river valley

Assessment of the effect of reduction in emissions of primary sources on eventual levels of pollutants, pH of precipitation and total wet deposition is crucial in designing acid-rain control strategies. The STEM-II/ASM model is used to investigate the effect of reduction in emissions on the ultimate deposition patterns and amounts of major acidic pollutants in a mesoscale region. This work also investigates the effect of background levels of primary pollutant species on the eventual levels and deposition amounts of SO₄⁼ and NO₃⁻. A series of mesoscale simulations were conducted in which emissions of primary sources of NO_x and SO₂ were reduced and/or background concentrations of certain key species were changed. The results indicate that the dominant effect on the eventual deposition amounts of SO₄⁼ and NO₃⁻ is due to background concentrations of key precursor species such as SO_x and NO_x. With relatively high background concentrations, reducing SO₂ emissions by 50% and NO_x emissions by 40% resulted in reductions of 2–3% for SO₄⁼ wet deposition aand about 15% for NO₃⁻ wet deposition. However, reducing the background concentrations of SO₂ and SO₄⁼ by 50% and NO, NO₂ and HNO₃ by 40% resulted in substantial reductions in wet deposition; SO₄⁼ deposition was reduced by 40–50% and NO₃⁻ deposition was reduced by approximately 35%.     

新型干法水泥生产中二恶英减排的环境技术经济研究

分析了水泥生产过程中多氯二苯并对二恶英和多氯二苯并呋喃(以下简称“二恶英”)的产生机理和国内外排放情况,针对我国部分新型干法水泥窑生产工艺二恶英排放偏高和窑炉能效偏低的问题,选择典型的新型干法水泥窑,开展了二恶英、常规污染物排放情况监测和能效检测及诊断,提出了二恶英协同减排措施,实施了有针对性的技术改造,并对改造后的排放和能效改进情况、环境和经济效益进行了系统评估. 结果表明:采用提高能效、充分燃烧、快速冷却废气及确保进入除尘器的废气温度低于200 ℃等二恶英减排最佳可行技术,烟气中二恶英的量降低了91.8%,单位熟料的能耗水平降低了2.08%;同时,颗粒物等常规污染物和二氧化碳等温室气体也实现了协同减排. 企业通过节能和余热利用获取了经济效益.      

AERMOD与估算模式在环境影响评价中的应用与比较研究

简单描述了大气环境影响评价中的AERMOD模型及估算模式,采用这两种预测模式对同一生活垃圾填埋场无组织排放的NH3、H2S进行了预测。比较两种模式的预测结果可以看出,估算模式仅能预测小时值,AERMOD模式可同时预测小时值、日平均值、年平均值。在污染源、预测范围、运行周期相同的情况下,不论哪种预测模式,污染物的最大落地浓度均与排放源强呈正比,敏感点处的落地浓度均与污染物源强呈正比、与距离呈反比。预测结果同时说明,估算模式是一种保守的预测模式,其预测结果比AERMOD模式大,可作为进一步预测模式的有效补充。     

长期土壤酸化模型(LTSAM)

以碱总量守恒为基础，以Ｕｌｒｉｃｈ缓冲范围为模型主要框架建立了兼能描述酸性与石灰性土壤长期酸化反应过程的动态模型．经与ＳＭＡＲＴ模型在理论设计和模拟结果两方面作对比之后，又利用新建模型以北京地区典型褐土为例进行了硫沉降与酸（Ｈ＋）沉降的对比计算．结果表明：（１）ＬＴＳＡＭ模型能够很好地反映土壤缓冲酸的主要机制．（２）模式运行即稳定又省时．（３）大气硫沉降不同于酸沉降．也就是说，硫沉降改变时，阳离子（尤其是主要离子）沉降量的变化应当加以考虑．     

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.