Modelling the role of nitrogen oxides,hydrocarbons and carbon monoxide in the global formation of tropospheric oxidants

A new zonally averaged two-dimensional chemical and transport model of the lower atmosphere has been used to study the budgets of photochemical oxidants on a global scale in the troposphere. The sensitivities of these budgets to controls on the emissions of NO_x, CO and hydrocarbons from a variety of sources have also been considered. The species studied include O₃, PAN, H₂O₂ and organic peroxides, as well as the global budget of the hydroxyl radical. The results show the relative impacts of emissions from natural and from man-made sources. Overall, some 75% of the turnover of tropospheric ozone results from in situ chemical production, with only 25% having its origins in the stratosphere. The respective fractions for chemical loss and dry deposition are similar. Of the ozone formed in situ, approximately one-third is formed from natural emissions, and two-thirds from man-made emissions. Over half of this man-made contribution is due to industrial society, with much of the rest being caused by biomass burning and methane emitted from paddy fields. Although reducing emissions of NO_x is the most effective way of controlling tropospheric O₃, this also increases the inventories of peroxides and the rate of increase in the concentration of methane, due to a reduction in the inventory of the OH radical. It is, therefore, necessary to control the emissions of a wide range of species in order to reduce the budget of all photochemical oxidants without adversely perturbing the budget of CH₄.     

四川省大气固定污染源排放清单及特征

根据收集到的四川省电厂、工业及民用部门的活动水平数据,采用合理的估算方法和排放因子,建立了四川省2010年大气固定污染源排放清单.结果表明:12010年四川省固定源共排放SO₂ 84.1万t、NO_x 44.9万t、CO 318.8万t、PM₁₀ 44.1万t、PM_2.5 25.5万t、VOC 17.9万t;2电厂和工业过程是固定源排放的主要贡献源;3燃煤是固定燃烧排放的主要贡献源,煤矸石、焦炭、天然气对污染物的贡献也不容忽视,水泥、钢铁、轻工业制造是本地区主要的工业过程排放源;4宜宾、成都及攀枝花是固定源污染物的主要贡献城市,约占四川省总排放量的20%~40%;5电厂、能源工业燃烧清单的不确定性主要来自排放因子,而工业过程涉及排放源种类繁多且复杂,排放测试研究较少,不确定性较高.     

Development of a new cleaner production process for producing chromic oxide from chromite ore

Chromic oxide (Cr₂O₃) is an important chemical with numerous industrial applications. The traditional process used for manufacturing chromic oxide from chromite ore has low resources and energy efficiency. Moreover, large quantities of chromium-containing toxic solid wastes are discharged, posing serious pollution concerns. To reduce the environmental impact of this procedure, a new cleaner process was developed by the Institute of Process Engineering, Chinese Academy of Sciences in Beijing, PR China, based upon the 3Rs (Reduce, Recycle, Reuse) principles of cleaner production and industrial ecology; this new cleaner process utilizes resources more efficiently, and does not discharge emissions of chromium-containing waste residue. A demonstration plant featuring this process, as well as an Eco-Industrial Park (EIP) has been built in He'nan Province, PR China. The new cleaner process is a promising advancement for the industrial production of chromic oxide (Cr₂O₃) as well as other chromium compounds such as potassium chromate (K₂CrO₄) and potassium dichromate (K₂Cr₂O₇).     

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.     

典型城市臭氧污染源贡献及控制策略费效评估

东莞是珠三角O_3污染最严重的城市,使用RSM/CMAQ(曲面响应模型)法分析了珠三角区域人为排放的NO_x和VOCs对东莞市O_3浓度变化源贡献.2014基准年分析结果表明,扣除模型域外区域传输及天然源排放对O_3本底浓度贡献(41.00%)后,东莞本地VOCs排放对O_3贡献最大(18.50%),珠三角区域NO_x减排率13%时可持续降低东莞市O_3浓度.进一步使用ABa CAS-SE(空气污染控制成本效益与达标评估系统)对2017、2020、2025东莞市3个未来年O_3污染控制情景进行了费效评估.评估结果显示,NO_x和VOCs控制比例相对较低的2017年控制情景人体健康效益/区域控制成本比约为1.1;而控制比例相对较高的2025年东莞O_3达标情景效益成本比仅为0.1.这说明,在高减排率情景下,以末端治理为主的控制措施经济可行性较差,需综合采取产业/能源结构调整、清洁生产等措施实现NO_x和VOCs的大比例减排,实现东莞O_3的稳定达标.今后将进一步研究NO_x和VOCs减排对PM_(2.5)环境浓度及健康效益影响,开展多目标污染物协同控制费效评估.     

Influence of power plant emissions and industrial emissions on the leeward ozone levels

In this paper a multibox model is applied to investigate how power plant emissions and industrial emissions affect the O₃ levels in a leeward urban area and a farther downwind rural area. Apart from a detailed consideration of one specific situation, the effect of advection is described and the influence of emission reductions on ozone formation is analyzed. The results prove that the characteristics of upstream emissions is of great significance for the O₃ levels. In particular, a reduction of hydrocarbon emissions was proved to be beneficial in all considered cases, while a reduction of primarily NO_x emissions may lead to an enhanced O₃ formation.     

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.     

火电行业清洁生产与末端治理技术对二氧化硫减排效果评估

为探明清洁生产技术在我国大气污染物削减中所起的作用,本文以火电行业为例,以SO_2作为特征污染物,对“清洁生产”和“末端治理”技术进行了筛选,建立了削污和减排效果分析模型,并收集火电行业的权威统计数据,计算了火电行业“清洁生产”技术削污量与“末端治理”技术减排量及两类技术各自削减量占比情况,研究了建国以来(1949—2013年)我国火电行业清洁生产技术削污效果和末端治理技术减排效果及其演变规律,并在此基础上提出政策建议.研究结果显示,以火电行业发电效率最低的低温低压发电技术为基准线,1949—2013年65年期间电力行业通过清洁生产技术累计实现SO_2削污量为4.94亿t,节约4940亿元的环保资金投入,削污率达到58.5%;2002—2013年12年期间电力行业末端治理技术累计实现SO_2减排量为1.10亿t,减排率为13.0%.     

长江三角洲地区人为源大气污染物排放特征研究

在收集整理长江三角洲地区（简称＂长三角＂）各城市人为大气污染源资料的基础上,采用以＂自下而上＂为主的方法建立了2007年长三角地区人为源大气污染物排放清单.清单结果显示,2007年长三角地区的SO2、NOx、CO、PM10、PM2.5、VOCs和NH3等大气污染物排放总量分别达到2391.8、2292.9、6697.1...     

Global warming contributions from wheat,sheep meat and wool production in Victoria,Australia – a life cycle assessment

This paper compares the life cycle global warming potential of three of Australia’s important agricultural production activities – the production of wheat, meat and wool in grazed subterranean clover (sub-clover) dominant pasture and mixed pasture (perennial ryegrass/phalaris/sub-clover/grass and cape weed) systems. Two major stages are presented in this life cycle assessment (LCA) analysis: pre-farm, and on-farm. The pre-farm stage includes greenhouse gas (GHG) emissions from agricultural machinery, fertilizer, and pesticide production and the emissions from the transportation of these inputs to paddock. The on-farm stage includes GHG emissions due to diesel use in on-farm transport and processing (e.g. seeding, spraying, harvesting, topdressing, sheep shearing), and non-CO₂ (nitrous oxide (N₂O), and methane (CH₄)) emissions from pastures and crop grazing of lambs.The functional unit of this life cycle analysis is the GHG emissions (carbon dioxide equivalents – CO₂ -e) from 1 kg of wheat, sheep meat and wool produced from sub-clover, wheat and mixed pasture plots. The GHG emissions (e.g. CO₂, N₂O and CH₄ emission) from the production, transportation and use of inputs (e.g. fertilizer, pesticide, farm machinery operation) during pre-farm and on-farm stages are also included. The life cycle GHG emissions of 1 kg of wool is significantly higher than that of wheat and sheep meat. The LCA analysis identified that the on-farm stage contributed the most significant portion of total GHG emissions from the production of wheat, sheep meat and wool. This LCA analysis also identified that CH₄ emissions from enteric methane production and from the decomposition of manure accounted for a significant portion of the total emissions from sub-clover and mixed pasture production, whilst N₂O emissions from the soil have been found to be the major source of GHG emissions from wheat production.     

Inventory of Strategies for Reducing Anthropogenic Emissions of N2O and Potential Reduction of Emissions in The Netherlands

The purpose of this study is to give a general overview of strategies to reduce N₂O emissions and to investigate their potential effects in the Netherlands. For all major sources of N₂O, technologies to reduce emissions are available or could become available in the near future. Their potential to reduce emissions has been estimated for conventional power plants (>10%), fluidized bed combustion (>80%), industrial production of adipic acid (>98%) and nitric acid (>80%), municipal solid waste incineration (>10%) and sewage treatment plants (50%). In addition, it is estimated that fertilizer-induced emissions in intensive agriculture can be reduced by at least 65%. In the Netherlands, these strategies could reduce emissions of N₂O by at least 40% in 1990 (i.e. if the technologies were fully implemented and nothing else would change) and by at least 30% in 2010 (relative to business as usual). Taking trends in activities into account, the mix of options considered could, in the period 2000–2010, reduce the annual Dutch emission to about 75% of the 1990 level. Most of this potential reduction is achieved by a catalytic reduction step in nitric acid production. Development of a catalytic converter seems feasible within a few years. The reduction options considered do not include additional reductions in the volumes of activities. Thus emissions could be further reduced by reductions in fossil fuel use, vehicle use, nitrogen fertilizer use, manure production, and waste production. Conceivable technologies that may not be implementable before 2000 include a number of promising options, such as low NO _x engines in vehicles, electric vehicles, NO _x reduction with low N₂O formation in stationary combustion and the development of modified combustors.     

基于本地污染源调查的杭州市大气污染物排放清单研究

基于实地调查数据并辅以统计数据,采用物料衡算法和排放因子法,估算了杭州市2015年大气污染物排放清单,并选取经纬度坐标、路网、航道、土地类型和人口等数据作为权重因子,研究了该地区各类排放源污染物排放空间分布特征.结果表明,杭州市2015年SO_2、NO_x、CO、VOCs、PM_(10)、PM_(2.5)和NH_3年排放总量分别为22.20×10~3、108.17×10~3、192.10×10~3、134.94×10~3、78.12×10~3、27.65×10~3和59.75×10~3t.工业源是杭州市SO_2排放的主要来源,移动源对NO_x和CO的排放贡献最为显著,扬尘源是杭州市PM_(10)和PM_(2.5)排放的最主要来源,其次为工业源;VOCs排放的主要来源依次为工业源、天然源和移动源;NH_3排放主要来自农业源.从空间分布来看,排放主要集中在中心城区及其周边的萧山、下沙、大江东、余杭和富阳等工业企业相对密集的区域.本研究建立的排放清单在污染源覆盖范围和排放因子方面仍然存在一定的不确定性,建议在后续研究中重点开展低、小、散企业及本地化排放因子调查研究工作,进一步提升大气污染物排放清单的准确度.     

天然气-汽油双燃料车实际道路排放特性研究

为研究使用天然气对轻型汽车排放的影响,利用便携式排放测试系统（PEMS）,对25辆压缩天然气-汽油双燃料出租车在实际道路上分别使用汽油和天然气时的CO2、CO、NOx和THC排放进行了对比测试.研究结果表明：实际道路上,原装车使用天然气相比汽油时,CO2、CO的排放平均分别降低22%和24%,NOx和THC的排放平均分...     

2010~2015年我国水泥工业NOx排放清单及排放特征

基于我国2011~2015年水泥企业逐条生产线基础信息、活动水平及控制技术等数据,建立了水泥工业NO_x排放量计算方法和动态排放数据库.利用该方法,计算了2011~2015年逐条水泥生产线NO_x排放量,分析了2010~2015年我国水泥工业NO_x排放特征.结果表明,我国水泥工业NO_x排放量变化范围为168~199万t,自2010年的169万t增加到2012年的199万t,达到排放峰值,随后逐年下降,到2015年与2010年基本持平.水泥工业NO_x排放的地区分布不均衡,2015年安徽、四川、河南、湖南、云南、山东是排放量最大的省份,占全国排放总量的40%,上海、内蒙、山西、新疆、湖南、云南、四川是单位熟料NO_x排放强度最大的省份.从生产线规模来看,规模≥ 4000 t·d^-1的熟料生产线产量占比和NO_x排放量占比均最大,分别为68.5%和66.5%,单位熟料NO_x平均排放强度最低.水泥生产工艺结构的转变及水泥工业降氮脱硝工作的开展是影响水泥工业大气NO_x排放特征的主要因素.     

High NO2/NOx emissions downstream of the catalytic diesel particulate filter: An influencing factor study

Diesel vehicles are responsible for most of the traffic-related nitrogen oxide (NO_x) emissions, including nitric oxide (NO) and nitrogen dioxide (NO₂). The use of after-treatment devices increases the risk of high NO₂/NO_x emissions from diesel engines. In order to investigate the factors influencing NO₂/NO_x emissions, an emission experiment was carried out on a high pressure common-rail, turbocharged diesel engine with a catalytic diesel particulate filter (CDPF). NO₂ was measured by a non-dispersive ultraviolet analyzer with raw exhaust sampling. The experimental results show that the NO₂/NO_x ratios downstream of the CDPF range around 20%–83%, which are significantly higher than those upstream of the CDPF. The exhaust temperature is a decisive factor influencing the NO₂/NO_x emissions. The maximum NO₂/NO_x emission appears at the exhaust temperature of 350°C. The space velocity, engine-out PM/NO_x ratio (mass based) and CO conversion ratio are secondary factors. At a constant exhaust temperature, the NO₂/NO_x emissions decreased with increasing space velocity and engine-out PM/NO_x ratio. When the CO conversion ratios range from 80% to 90%, the NO₂/NO_x emissions remain at a high level.     

Vehicle emissions of primary air pollutants from 2009 to 2019 and projection for the 14th Five-Year Plan period in Beijing, China

Over the past decade, the emission standards and fuel standards in Beijing have been upgraded twice, and the vehicle structure has been improved by accelerating the elimination of 2.95 million old vehicles. Through the formulation and implementation of these policies, the emissions of carbon monoxide (CO), volatile organic compounds (VOCs), nitrogen oxides (NO_x), and fine particulate matter (PM_2.5) in 2019 were 147.9, 25.3, 43.4, and 0.91 kton in Beijing, respectively. The emission factor method was adopted to better understand the emissions characteristics of primary air pollutants from combustion engine vehicles and to improve pollution control. In combination with the air quality improvement goals and the status of social and economic development during the 14th Five-Year Plan period in Beijing, different vehicle pollution control scenarios were established, and emissions reductions were projected. The results show that the emissions of four air pollutants (CO, VOCs, NO_x, and PM_2.5) from vehicles in Beijing decreased by an average of 68% in 2019, compared to their levels in 2009. The contribution of NO_x emissions from diesel vehicles increased from 35% in 2009 to 56% in 2019, which indicated that clean and energy-saving diesel vehicle fleets should be further improved. Electric vehicle adoption could be an important measure to reduce pollutant emissions. With the further upgrading of vehicle structure and the adoption of electric vehicles, it is expected that the total emissions of the four vehicle pollutants can be reduced by 20%-41% by the end of the 14th Five-Year Plan period.     

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.     

海南省淘汰落后产能政策的污染物协同减排效应评价

结构减排是我国污染物减排的主要措施,是海南省推进产业结构升级、实现建成"全国生态文明建设示范区"的必然选择.为评价该政策产生的环境效应,采用海南省2006~2013年"十一五"和"十二五"期间淘汰落后产能数据,运用排放因子法,估算各年份由于淘汰水泥、炼铁、炼钢、造纸和实心黏土砖落后产能带来的多种污染物协同减排效应.结果表明,研究期间氮氧化物(NO_x)、二噁英类污染物、大气汞累计削减量分别达到2 826.0 t·a~(-1)、10 462.5 mg·a~(-1)和280.8 kg·a~(-1).淘汰落后产能对海南省NO_x减排的影响不是很显著,但对降低新型污染物二噁英类和大气汞的排放起到有效的源头控制作用,累计效应显著.该研究为评估淘汰落后产能政策对常规污染物和新型污染物协同控制效应提供了方法和思路.     

海峡西岸地区人为源大气污染物排放特征研究

采用以"自下而上"为主的方法建立了2007年海峡西岸地区的人为源大气污染物排放清单.计算结果显示,海西地区人为源SO2、NOx、CO、PM10、PM2.5、VOCs和NH3排放总量分别为69.5×104、96.1×104、413.1×104、93.9×104、40.6×104、85.0×104和28.5×104t.电厂和工业燃烧设施分别占SO2排放的48%和39%,以及NOx排放的51%和25%.水泥、砖瓦等制造过程贡献了约51%的PM10排放和36%的PM2.5排放.秸秆燃烧、加油站和涂料等VOCs面源分别占到其排放总量的27%、15%和4%.NH3的主要排放源为畜禽养殖和氮肥施用等农业部门,占到总排放量的89%.海西地区的单位面积大气污染物排放量仅相当于长三角地区的25%左右,略高于全国平均水平.该地区人为源和天然源VOCs排放比重分别占56%和44%,人为源VOCs排放比重低于全国大部分地区.海西大气污染高排放地区主要集中在沿海一带,以泉州、潮汕、福州和温州等地区为主,建议"十二五"发展过程中,重点关注上述高排放地区,限制重点排放源的发展,开发低耗能、低污染的发展模式.