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.     

30年来中国民航运输行业的大气污染物排放

民航是我国重要的交通运输方式之一,但我国民航运输行业的大气污染物排放问题报道较少.根据中国民航统计部门逐年统计数据,采用基于燃料消耗量的排放因子法,估算了1980～2009年中国民航飞机的大气污染物排放量,并分析了大气污染物排放强度及其变化.结果表明,30年来中国民航飞机SO2、CO、NOx和HC排放量逐年增多,分别由1980年的0.031、0.189、0.225和0.314万t增至2009年的1.183、7.298、8.705和12.159万t,排放量年均增加分别为0.039 7、0.245、0.292和0.408万t.SO2、CO、NOx和HC的排放强度呈降低趋势,其值分别由1980年的0.624、3.806、4.53和6.322 g.(t.km)-1降至2009年的0.275、1.697、2.025和2.828 g.(t.km)-1.中国民航运输行业所排放的SO2、CO、NOx占全国总排放量的比重很低,与其他行业排放量相比,中国民航运输行业所排放的大气污染物量也较小.     

Comprehensive and high-resolution emission inventory of atmospheric pollutants for the northernmost cities agglomeration of Harbin-Changchun, China: Implications for local atmospheric environment management

Using a bottom-up estimation method, a comprehensive, high-resolution emission inventory of gaseous and particulate atmospheric pollutants for multiple anthropogenic sectors with typical local sources has been developed for the Harbin-Changchun city agglomeration (HCA). The annual emissions for CO, NOx, SO₂, NH₃, VOC_S, PM_2.5, PM₁₀, BC and OC during 2017 in the HCA were estimated to be 5.82 Tg, 0.70 Tg, 0.34 Tg, 0.75 Tg, 0.81Tg, 0.67 Tg, 1.59 Tg, 0.12 Tg and 0.26 Tg, respectively. For PM₁₀ and SO₂, the emissions from industry processes were the dominant contributors representing 54.7% and 49.5%, respectively, of the total emissions, while 95.3% and 44.5% of the total NH₃ and NOx emissions, respectively, were from or associated with agricultural activities and transportation. Spatiotemporal distributions showed that most emissions (except NH₃) occurred in November to March and were concentrated in the central cities of Changchun and Harbin and the surrounding cities. Open burning of straw made an important contribution to PM_2.5 in the central regions of the northeastern plain during autumn and spring, while domestic coal combustion for heating purposes was significant with respect to SO₂ and PM_2.5 emissions during autumn and winter. Furthermore, based on Principal Component Analysis and Multivariable Linear Regression model, air temperature, relative humidity, electricity and energy consumption, and the urban and rural population were optimized to be representative indicators for rapidly assessing the magnitude of regional atmospheric pollutants in the HCA. Such indicators and equations were demonstrated to be useful for local atmospheric environment management.     

33年来中国铁路运输行业的大气污染物排放

铁路是中国重要的交通运输方式,但中国至今尚无铁路运输行业大气污染物排放的报道.根据中国铁路部门逐年统计数据,采用基于燃料消耗量的排放因子法,估算了1975～2007年中国铁路机车大气污染物排放量,并分析了大气污染物排放强度及其变化.结果表明,33年来中国铁路机车烟尘、SO2、CO和CnHm排放量逐年降低,分别由1975...     

木薯乙醇-汽油混合燃料生命周期排放多目标优化研究

建立了木薯乙醇-汽油混合燃料生命周期排放单目标和多目标优化模型.以生命周期CO,NO_x,PM,HC,SO_x,CO₂排放为优化目标,对木薯乙醇-汽油混合燃料生命周期排放进行了单目标及多目标优化,并进行了灵敏度分析.结果表明:多目标优化后木薯乙醇-汽油混合燃料的混合比例为63%.与原始值相比,多目标优化后生命周期CO排放略有升高,NO_x升高15%,PM升高19%;生命周期HC、SO_x和CO₂分别降低8%、50%和21%.     

The impact of changing regional emissions on precipitation chemistry in the eastern United States

From 1975 to 1987 a 19% change in SO₂ emissions a 16% change in NO_x emissions have occurred over the eastern and mid-western U.S. Six continental precipitation chemistry sites from the MAP3S network, plus the Hubbard Brook Experimental Forest, NH, show a direct relationship between emission levels and precipitation H⁺ and SO₄^2- concentrations, except for Penn State, PA. MAP3S sites at Illinois and Ohio, located closest to the major SO₂ source regions, demonstrates statiscally significant (P <0.05) linear regressions of SO₄^2- concentrations on SO₂ emissions. Whiteface Mt., NY, shows a weaker relationship (P <0.01), and Hubbard Brook shows the strongest relationship (P <0.01) between SO₂ emissions and SO₄^2- concentration in precipitation. No site shows a significant relationship (P <0.10) for NO_x emissions and NO₃⁻ concentrations in precipitation. Illinois, Ohio, Ithaca and Hubbard Brook show significant linear regressions of H⁺ concentrations on emissions of SO₂ + NO_x (P <0.10, 0.05, 0.01, and 0.01, respectively). Overall, for the entire region examined, decreasing SO₂ emissions levels appear to have decreased SO₄^2- concentrations with an efficiency of 74% ± 15% (s.e.). Decreasing SO₂ plus NO_x emissions (18%) have been accompanied by a decreasing H⁺ concentrations (18%) suggesting an efficiency of conversion of 100% ± 15% (s.e.) for the study region as a whole. While significant reductions in acid species have occured at Hubbard Brook, further reductions in excess of 50% of present deposition are necessary to protect acid-sensitive ecosystems.     

民航飞机起飞过程气态污染物排放特征分析

民航飞机在起飞过程中发动机推力高、耗油量大,并且飞行高度低,由其排放的污染物对局地空气质量和人体健康存在较大影响.选择B737-800作为典型机型,通过对飞机性能参数的模拟,精确计算了其在全推力和减推力等多种方式下起飞离场爬升至1 000 m高度过程中NO_x、CO、HC和SO_2的排放量,并与ICAO基准模型估算结果进行对比.结果表明,NO_x是排放量最大的污染物.其中,全推力起飞过程4种污染物的排放量分别为4.849、0.062、0.031和0.229 kg.减推力起飞方式下,选择更高的灵活温度后,NO_x和CO排放量分别降低和升高,HC和SO2排放量变化不大.经过对比发现,ICAO的基准排放模型,对4种污染物的估算结果存在较大偏差.与机动车相比,单次全推力起飞过程与一辆小客车行驶9 508 km的NO_x排放量相当.精确计算方法为准确估算机场区域飞机污染排放清单提供基础.     

长三角地区火电行业主要大气污染物排放估算

以2012年为基准年,利用排放因子法估算了长三角地区火电行业主要大气污染物(SO2、NOx、烟尘、PM10、PM2.5)排放.其中,SO2、NOx、烟尘、PM10、PM2.5的排放量分别为473 238、1 566 195、587 713、348 773、179 820 t.对于SO2和NOx,300 MW以上机组的贡献分别为85%和82%;烟尘、PM10和PM2.5方面,100 MW以下的机组贡献占比分别为81%、53%和40%.地区贡献方面,由大到小依次为江苏、浙江和上海.另通过对上海地区多家电厂不同等级机组污染排放数据进行统计计算,得出上海地区300 MW以上等级机组的污染物排放因子,对比分析可知,上海地区火电厂污染物排放因子水平总体较低.假设长三角地区火电行业同等级机组均与现在上海地区机组排放水平相当,则行业排放SO2可削减55.8%~65.3%,NOx可以削减50.5%~64.1%,烟尘可以削减3.4%~11.3%.若能提高较小等级机组的发电技术和污染控制水平,各污染物排放削减量可进一步提高.然而,根据长三角地区实际污染情况,应综合因素考虑火电行业削减排放,以促进区域空气质量不断改善.     

Simulation based life cycle assessment of airborne emissions of biomass-based ethanol products from different feedstock planting areas in China

Oil shortage and environmental deterioration urge people to pay more and more attention to Biomass-based Fuel Ethanol (BFE), because it is renewable and apparently environmentally friendly. This paper aims to assess and compare the air emissions of three BEF products from different feedstock planting areas in China. For the purpose of a “cradle to grave” study of biomass-based ethanol fuel as a substitute transportation fuel, the authors chose “vehicle fueled by biomass-based E10 (a blend of 10% ethanol and 90% gasoline, v/v)” as the subject. Then, life cycle emission models of Wheat-based E10 from central China, Corn-based E10 from northeast China, and Cassava-based E10 from southwest China were set up based on surveys; life cycle emission functions of CO₂, CO, N₂O, NO_x, SO₂, CH₄, VOC, and PM₁₀ were constructed and value of each emission category was calculated based on Monte Carlo simulation of the life cycle emission models. The calculation results showed that compared with gasoline-fueled vehicles, biomass-based E10-fueled vehicles release less CO₂ and VOC in their lifecycles, but wheat-based E10-fueled and cassava-based E10-fueled ones have more emissions of CO, CH₄, N₂O, NO_x, SO₂, PM₁₀ and corn-based E10-fueled ones have more emissions of CH₄, N₂O, NO_x, SO₂, PM₁₀. Suggestions on reducing the emissions have been proposed for future actions.     

The influence of ambient temperature on tailpipe emissions from 1985 to 1987 model year light-duty gasoline motor vehicles—II

Tailpipe emissions from gasoline fieled motor vehicles are sensitive to a number of factors including driving schedule (speed vs time), ambient temperature and fuel composition. The sensitivity of hydrocarbon (HC), aldehyde, CO, and oxides of nitrogen (NO_x) emissions to these variables was examined with 11 recent technology (1985–1987 model year) four- six- and eight-cylinder gasoline fueled motor vehicles. In excess of 200 individual HCs and 12 aldehydes were included in the detailed organic emission characterizations. Two fuels and driving schedules were used. Hydrocarbon and CO emissions increased significantly and NO_x emissions, in general, increased slightly as ambient temperature decreased. Formaldehyde also increased only slightly at test temperature decreased. Paraffin and aromatic emission fractions were dependent on fuel composition with olefin fraction being less fuel sensitive. When the low temperature cold start was preceded by a 5 min engine idle, CO and HC emissions were lowered, and NO_x emissions essentially unchanged.     

海峡西岸经济区大气污染物排放清单的初步估算

以2009年为基准年,结合污染源普查数据、统计年鉴及工业活动、居民生活等多个方面对海峡西岸经济区包括SO2、NOx、PM2.5、VOCs和NH3在内的大气污染物的排放量进行了估算,建立了海西区大气污染物排放清单.结果发现,上述5类污染物基准年的排放量分别为40.67×104、55.84×104、50.57×104、152.26×104和26.18×104t.其中,SO2、NOx及PM2.5的排放主要来自电厂,占排放总量的比例分别为25.58%、34.89%和38.75%;VOCs和NH3的主要排放源分别来自植被排放和养殖业,其贡献量分别为49.12%和47.07%.采用GIS对排放清单进行网格化处理,得出SO2、NOx及PM2.5的高排放强度区域与固定源的空间分布较为一致.此外,结合国家和地方"十二五"发展规划,采用情景分析方法估算了2015年海西区大气污染物的排放清单.与基准年相比,SO2、NOx和NH3的排放量呈下降趋势,PM2.5和VOCs的排放量呈大幅度增加.基准年排放清单的不确定性分析显示,VOCs排放估算的不确定度最大,为225%.     

辽宁省港口邻近区域海运废气排放测算

为准确测算沿海地区船舶废气排放量,基于试验数据确定了NO_x、CO、HC和CO₂排放因子;结合文献资料和海事局进出港船舶签证数据,采用基于船舶活动过程的方法测算了2014年辽宁省港口邻近区域〔距港口减速区外边界25 n mile(1 n mile=1 852 m)以外的边界线与港口陆地岸线所围成的区域〕海运废气排放清单. 结果表明:2014年辽宁省港口邻近区域海运NO_x、CO、HC、CO₂、SO₂和PM(颗粒物)的排放量分别为11 827.1、971.4、399.6、1 097 426.5、11 654.1和959.2 t;散货船、集装箱船和油船3种主要类型船舶的NO_x、CO、HC、CO₂、SO₂和PM的分担率之和分别为74.7%、77.8%、70.8%、68.0%、70.9%和70.6%;主机NO_x、CO、HC、CO₂、SO₂和PM的分担率最大,分别为63.7%、63.0%、46.0%、40.4%、46.4%和45.3%;停泊工况下的NO_x、CO、HC、CO₂、SO₂和PM排放量分别为3 318.3、281.7、168.3、520 194.9、4 894.0和411.5 t. 船舶降速运行、减少停港时间、燃用低硫油和向船舶供应岸电等措施能降低港口邻近区域海运废气排放. 基础数据缺乏或数据代表性不足给废气排放清单带来了一定的不确定性.      

NOx和VOC自然源排放及其对中国地区对流层光化学特性影响的数值模拟研究

利用Williams等和Guenther等的模型估计中国地区NO_x和VOC的自然源排放.所得清单显示土壤NO_x排放总量（以N计）为225.75 Gg;植被VOC年排放总量（以C计）为13.23 Tg,其中异戊二烯、单萜烯、其它VOC分别为7.77、1.86、3.60 Tg;排放有明显季节变化和空间变化.运用中尺度气象模式MM5以及光化学模式Calgrid研究这些排放在不同季节对对流层化学的影响.结果表明,O₃、NO_x、HNO₃和PAN的全国平均浓度在土壤NO_x排放影响下分别增加15.3%、15.7%、25.5%和6.5%;在植被VOC排放影响下改变5.6%、-4.9%、-19.3％和142.3％;在两者综合影响下增加26.1%、8.8%、4.3%和177.9%;浓度变化在夏季明显强于其它季节.自然源对中国地区光化学污染物空间分布有不同程度的影响,这种影响同区域气象条件、源排放和NMHC/NO_x比值等因素有关.NO_x和VOC的自然源排放对光化学特性影响显著,在光化学模拟过程中不容忽视.     

A review and evaluation of nonroad diesel mobile machinery emission control in China

China’s emission control for nonroad diesel mobile machinery (NDMM) must deal with a fast increase in stock as well as regulations that are two decades behind those for on-road vehicles.This study provides the first large-scale review and evaluation of China’s NDMM policies,along with emission measurements and an investigation on diesel fuel quality.The sulfur contents of the investigated diesel declined from 430 ppm (median value) in 2011 to6-8 ppm during the 2017-2018 period.The emission contr...     

SO2 and NOx emissions due to fossil ruel combustion in Saudi Arabia: A preliminary inventory

Phenomenal economic growth during the last two decades, as a result of oil wealth, has led to a dramatic increase in the demand for fossil fuel in the Kingdom of Saudi Arabia (KSA). In this paper a preliminary inventory for sulfur dioxide (SO₂) and nitrogen oxides (NO_x) emitted into the atmosphere as a result of fossil fuel combustion by various economic sectors in KSA in the year 1986 is presented. Emissions are discussed in relation to major source categories (major fuel consuming economic sectors) and on the basis of type of fuel combusted. The data are also geographically disaggregated according to major economic and population centers in KSA in order to show the spatial distribution of emissions. Also, SO₂ and NO_x emission trends (1971–1990) were estimated from 1986 data and historical and projected fuel consumption figures.     

兰州盆地人为源大气污染物网格化排放清单及其空间分布特征

基于所搜集的兰州盆地各类人为污染源排放大气污染物的活动水平数据及其排放因子,采用"自下而上"的方法建立了2009年兰州盆地(石油化工城市)1 km×1 km的7种(类)大气污染物网格化排放清单,并对其来源和空间分布特征进行了分析研究.结果显示:2009年兰州盆地NOx、SO_2、VOCs、CO、PM_(10)、PM_(2.5)和NH3的排放总量分别为1.2×10~5、8.8×10~4、4.3×10~4、4.1×10~5、9.6×10~4、4.2×10~4和1.4×10~4t;工业燃烧排放是兰州盆地NO_x和SO_2的主要贡献源,分别占其总排放量的85.70%和52.55%;工业非燃烧过程排放是VOCs的最大贡献源,占总排放量的81.25%;工业点源和工业非燃烧过程排放是CO的两大贡献源,分别占其总排放量的33.97%和28.32%;PM_(10)和PM_(2.5)主要来源于工业非燃烧过程,贡献分别为51.09%和55.12%;氮肥使用和禽畜养殖是NH_3排放最大的贡献源,分别占其总排放量的39.20%和30.70%.空间分布特征表现为:以工业源为主要排放源的NO_x、SO_2、VOCs、CO、PM_(10)、PM_(2.5)主要分布在工业和人口最为集中的兰州盆地市区一带,NH_3的排放则主要集中在榆中县和皋兰县交界的农村地区.同时,还对2014年工业燃烧源和道路移动源的7种(类)大气污染物排放量进行了估算,并与2009年进行了排放比较研究.结果表明,2014年工业污染源的7种(类)污染物排放量与2009年相比平均增幅不高,最高不超过30%,但移动源污染物排放量却大幅增加,增幅将近1倍.此外,基于排放因子及活动水平的不确定性,本研究对排放清单的结果进行了不确定性分析,并通过蒙特卡罗模拟对各污染物的排放量进行了评估.本排放清单的建立,不仅填补了兰州盆地大气污染物网格化排放清单的空白,还可为兰州盆地大气污染物排放清单更新、区域环境过程、大气复合污染成因及大气污染预警技术等相关研究提供基本方法手段及基础数据.     

超低改造下中国火电排放清单及分布特征

本研究基于2018年火电在线监测和环境统计等数据,自下而上编制了中国高分辨率火电行业排放清单,并核算了排放浓度、排放因子和排放量.结果表明超低排放政策效果显著：2018年火电SO₂、NO_x和烟尘平均排放浓度分别为37.57、56.71和7.41mg ·m^-3.比2015年分别下降58.71%、43.12%和60.79%;中国燃煤机组的SO₂、NO_x和烟尘平均排放因子分别为0.30、0.48和0.06 g ·kg^-1,比2015年分别下降55.2%、36.84%和62.5%;中国火电SO₂、NO_x、烟尘和PM_2.5总排放量分别为72.14、118.38、14.90和13.59万t ·a^-1,比2015年分别下降41.32%、19.29%、48.12%和40.39%.     

珠江三角洲非道路移动源排放清单开发

根据收集到的珠江三角洲非道路移动源活动水平数据,采用适合各类非道路移动源污染物排放量的估算方法和排放因子,建立了珠江三角洲地区2006年非道路移动源排放清单.结果表明,珠江三角洲地区2006年非道路移动源排放SO2为6.52×104t,NOx为1.24×105t,VOC为4.54×103t,CO为2.67×104t,PM10为4.51×103t.其中船舶为最大的SO2、NOx、CO和PM10排放贡献源,分别占非道路移动源排放总量的96.4%、73.8%、39.4%和50.5%.在船舶排放源中,SO2、NOx、VOC、CO和PM10排放量的89.8%、81.8%、77.3%、79.5%和81.7%来自货轮和散装干货船.非道路移动源已成为该地区第三大SO2和NOx排放贡献源,分别占珠江三角洲大气污染源SO2和NOx排放总量的8.6%和13.5%.     

南昌市固定燃烧点源大气污染物排放清单及特征

大气污染物排放清单是了解区域污染物排放特征、准确模拟空气质量的重要资料,而工业点源是大气污染的重点排放源.通过收集相关活动水平信息和合理的排放因子,采用"自下而上"的方法建立了南昌市2014年点源大气污染物排放清单.结果表明,SO_2、NO_x、CO、PM_(10)、PM_(2.5)和VOC排放总量分别为29576.2、17115.1、25946.6、4689.4、922.9和1190.4 t,其中,金属炼制行业对SO_2、CO和VOC的贡献最高,分别占37.75%、30.59%和38.45%;火电行业是NO_x的主要来源,其贡献率为47%;水泥等建材制造行业对PM_(10)和PM_(2.5)排放贡献最高,分别为26%和25%.根据排放源污染物排放量及地理坐标信息,建立了0.4 km×0.4 km的污染物排放量空间分布特征图,结果表明,南昌市大气污染物排放较为集中,青山湖区北部和新建区北部是SO_2、NO_x、CO和VOC的主要排放区,而PM_(10)和PM_(2.5)的排放量相对分散,并在安义县出现排放高值区.通过将计算结果与统计数据结果进行对比,了解所估算清单的准确程度.对SO_2和NO_x的计算值和统计值进行统计分析,结果显示,NMB(标准化平均偏差)和NME(标准化平均误差)值均小于50%,清单计算精度较高.同时,为了解清单数据质量,对清单的不确定性进行定量分析,结果显示,SO_2和VOC不确定性较低而PM_(10)和PM_(2.5)的不确定性相对较高,清单整体不确定性与其他研究结果相差不大.建议后期研究可以从提升基础数据质量和建立具有区域代表性的排放因子数据库着手,从而减小排放量的不确定性,获得精准可靠的大气污染物清单并应用于空气质量模型预报等更深入的研究.     

Multi-process and multi-pollutant control technology for ultra-low emissions in the iron and steel industry

The iron and steel industry is not only an important foundation of the national economy, but also the largest source of industrial air pollution. Due to the current status of emissions in the iron and steel industry, ultra-low pollutant emission control technology has been researched and developed. Liquid-phase proportion control technology has been developed for magnesian fluxed pellets, and a blast furnace smelting demonstration project has been established to use a high proportion of fluxed pellets (80%) for the first time in China to realize source emission reduction of SO₂ and NO_x. Based on the characteristics of high NO_x concentrations and the coexistence of multiple pollutants in coke oven flue gas, low-NO_x combustion coupled with multi-pollutant cooperative control technology with activated carbon was developed to achieve efficient removal of multiple pollutants and resource utilization of sulfur. Based on the characteristics of co-existing multiple pollutants in pellet flue gas, selective non-catalytic reduction (SNCR) coupled with ozone oxidation and spray drying adsorption (SDA) was developed, which significantly reduces the operating cost of the system. In the light of the high humidity and high alkalinity in flue gas, filter materials with high humidity resistance and corrosion resistance were manufactured, and an integrated pre-charged bag dust collector device was developed, which realized ultra-low emission of fine particles and reduced filtration resistance and energy consumption in the system. Through source emission reduction, process control and end-treatment technologies, five demonstration projects were built, providing a full set of technical solutions for ultra-low emissions of dust, SO₂, NO_x, SO₃, mercury and other pollutants, and offering technical support for the green development of the iron and steel industry.