Sensitivity analysis of surface ozone to emission controls in Beijing and its neighboring area during the 2008 Olympic Games

The regional air quality modeling system RAMS (Regional Atmospheric Modeling System)-CMAQ (Community Multi-scale Air Quality modeling system) is applied to analyze temporal and spatial variations in surface ozone concentration over Beijing and its surrounding region from July to October 2008. Comparison of simulated and observed meteorological elements and concentration of nitrogen oxides (NOx) and ozone at one urban site and three rural sites during Olympic Games show that model can generally reproduce the main observed feature of wind, temperature and ozone, but NOx concentration is overestimated. Although ozone concentration decreased during Olympics, high ozone episodes occurred on 24 July and 24 August with concentration of 360 and 245 μg/m³ at Aoyuncun site, respectively. The analysis of sensitive test, with and without emission controls, shows that emission controls could reduce ozone concentration in the afternoon when ozone concentration was highest but increase it at night and in the morning. The evolution of the weather system during the ozone episodes (24 July and 24 August) indicates that hot and dry air and a stable weak pressure field intensified the production of ozone and allowed it to accumulate. Process analysis at the urban site and rural site shows that under favorable weather condition on 24 August, horizontal transport was the main contributor of the rural place and the pollution from the higher layer would be transported to the surface layer. On 24 July, as the wind velocity was smaller, the impact of transport on the rural place was not obvious.     

High-resolution modeling and evaluation of ozone air quality of Osaka using an MM5-CMAQ system

High-resolution modeling approach is increasingly being considered as a necessary step for improving the monitoring and predictions of regional air quality.This is especially true for highly urbanized region with complex terrain and land-use.This study uses Community Multiscale Air Quality (CMAQ) model coupled with MM5 mesoscale model for a comprehensive analysis to assess the suitability of such high-resolution modeling system in predicting ozone air quality in the complex terrains of Osaka,Japan.The 1-km and 3-km grid domains were nested inside a 9-km domain and the domain with 1-km grid covered the Osaka region.High-resolution Grid Point Value-Mesoscale Model μgPV-MSM) data were used after suitable validation.The simulated ozone concentrations were validated and evaluated using statistical metrics using performance criteria set for ozone.Daily maxima of ozone were found better simulated by the 1-km grid domain than the coarser 9-km and 3-km domains,with the maximum improvement in the mean absolute gross error about 3 ppbv.In addition,1-km grid results fared better than other grids at most of the observation stations that showed noticeable differences in gross error as well as correlation.These results amply justify the use of the integrated high-resolution MM5-CMAQ modeling system in the highly urbanized region,such as the Osaka region,which has complex terrain and land-use.     

High-resolution modeling and evaluation of ozone air quality of Osaka using MM5-CMAQ system

High-resolution modeling approach is increasingly being considered as a necessary step for improving the monitoring and predictions of regional air quality. This is especially true for highly urbanized region with complex terrain and land-use. This study uses Community Multiscale Air Quality (CMAQ) model coupled with MM5 mesoscale model for a comprehensive analysis to assess the suitability of such high-resolution modeling system in predicting ozone air quality in the complex terrains of Osaka, Japan. The 1-km and 3-km grid domains were nested inside a 9-km domain and the domain with 1-km grid covered the Osaka region. High-resolution Grid Point Value-Mesoscale Model (GPV-MSM) data were used after suitable validation. The simulated ozone concentrations were validated and evaluated using statistical metrics using performance criteria set for ozone. Daily maxima of ozone were found better simulated by the 1-km grid domain than the coarser 9-km and 3-km domains, with the maximum improvement in the mean absolute gross error about 3 ppbv. In addition, 1-km grid results fared better than other grids at most of the observation stations that showed noticeable di erences in gross error as well as correlation. These results amply justify the use of the integrated high-resolution MM5-CMAQ modeling system in the highly urbanized region, such as the Osaka region, which has complex terrain and land-use.     

夏季长三角地区臭氧非线性响应曲面模型的建立及应用

2013年8月上旬,长三角地区发生了一次大范围高浓度臭氧污染事件.本研究基于WRF-CMAQ空气质量模型系统,结合长三角地区大气污染物排放清单,构建了臭氧与其前体物之间的非线性响应曲面模型(Response surface modeling,RSM).基于RSM探讨了长三角地区O_3化学的敏感性特征,分析了上海市O_3的来源并预测不同情景下O_3的变化,提出O_3污染的最优控制方案.研究结果表明,长三角地区夏季O3主控因素区域差别较大,上海环科院、杭州卧龙桥、南京玄武湖等城区点位属于VOC控制型;徐州铜山、合肥肥西、丽水青田等郊区属于NOx控制型.O_3的敏感性特征在不同浓度水平下也呈现较大差异,随着O_3浓度水平的升高,各地区NOx敏感性均有所增加.从区域来源来看,远距离传输对平日上海O_3贡献较大,占50%以上;而在O_3污染日,本地及区域贡献为72.1%,而远距离传输贡献下降至27.9%.快速预测了110组减排情景,表明在本地及区域前体物均减排70%的情况下,2013年8月上海O_3浓度能完全达标.     

Strong ozone production at a rural site in theNorth China Plain: Mixed effects of urban plumesand biogenic emissions

Regional ozone (O₃) pollution has drawn increasing attention in China over the recent decade, but the contributions from urban pollution and biogenic emissions have not been clearly elucidated. To better understand the formation of the regional O₃ problem in the North China Plain (NCP), intensive field measurements of O₃ and related parameters were conducted at a rural site downwind of Ji'nan, the capital city of Shandong province, in the summer of 2013. Markedly severe O₃ pollution was recorded, with the O₃ mixing ratios exceeding the Chinese national ambient air quality standard on 28?days (a frequency of 78%) and with a maximum hourly value of 198 ppbv. Extensive regional transport of well-processed urban plumes to the site was identified. An observation-constrained chemical box model was deployed to evaluate in situ photochemical O₃ production on two episodes. The results show that the in situ formation accounted for approximately 46% of the observed O₃ accumulation, while the remainder (~ 54%) was contributed by regional transport of the O₃-laden urban plumes. The in situ ozone production was in a mixed controlled regime that reducing either NOx or VOCs would lead to a reduction of ozone formation. Biogenic VOCs played an important role in the local ozone formation. This study demonstrates the significant mixed effects of both anthropogenic pollution from urban zones and biogenic emission in rural areas on the regional O₃ pollution in the NCP region, and may have general applicability in facilitating the understanding of the formation of secondary pollution over China.     

生态NMHC对臭氧和PAN影响的数值模拟研究

利用数值模拟方法结合GEIA生态源排放清单，研究了夏季我国东部生态系统排放非甲烷烃（NMHC）对臭氧和过氧乙酰硝酸脂（PAN）的影响，阐明了生态NMHC在大气化学系统中的重要作用。研究结果表明，生态NMHC使我国东部大部分地区臭氧和PAN增加，最大平均增量分别为9ppb和0．6ppb；白天最大平均增量分别达到21ppb和1．2ppb，最大增量地区位于长江三角洲的浙江、上海附近地区。模拟结果与实测值有好的一致性，研究结果表明对于区域和城市臭氧的模拟及其控制应该充分考虑生态源的作用。     

上海市近地面臭氧污染的健康影响评价

根据2008年上海市环境保护部门的每日24h近地面臭氧监测数据,以每日最大8h(11:00～18:59)的臭氧浓度均值作为上海市居民的平均暴露水平,以该年上海市的全部常住人口作为臭氧暴露人口,计算近地面臭氧污染对上海市居民的健康影响和相关的健康经济损失.2008年上海市近地面臭氧每日最大8h的年平均水平为88μg/m3,其中市区为78μg/m3,市郊区为96μg/m3.结果表明,近地面臭氧污染可以导致上海市居民1892(95%CI:589～3540)例早逝和26049(95%CI:13371～38499)例住院,全年的归因健康经济损失为32.42(95%CI:10.80～59.23)亿元,其中由早逝引起的损失占总健康经济损失的88.12%.提示近地面臭氧污染已对上海市居民产生了较大的健康损失和经济损失.     

我国典型钢铁工业城市夏季臭氧污染来源解析研究

邯郸与其周边城市相比,臭氧(O3)污染最为严重.基于观测数据分析夏季邯郸O3浓度的时空特征,结果显示:观测期间邯郸O3超标天数比率为86.7％,各区县O3浓度分布存在差异,高温、低湿和偏南贴地气团传输是此次O3连续污染的主要成因.继而,以CAMx-OSAT模型模拟方法进行O3来源解析,溯源分析显示:邯郸O3污染具有明显...     

夏季局地环流对北京下风向地区O3输送的影响

于2007年6~9月,北京地区环流背景属于局地“山谷风”环流期间,在沿主导风向路径分布的4个代表性测点开展了地面O3浓度观测,并采用Models-3/CMAQ模式对典型个例进行模拟,以研究城市对下风向地区O3输送的影响.结果表明,城市下风向测点上甸子本底站O3平均浓度、超标率最高,上风向测点超标率最低,O3小时极大值出现在城区站,为271.56×10-9;不同测点O3浓度日变化规律一致,但浓度日峰值出现时间呈现自城市至下风向地区逐渐滞后的规律;各测点主导风向下O3浓度分布具有沿输送路径逐渐升高的趋势,且两主导风向下的浓度差值也具有沿西南输送路径逐渐升高的趋势;本底地区O3的浓度受来自清洁地区和城市污染地区不同气流影响,观测资料估算得出城市对区域背景地区的输送贡献为36.7×10-9;模拟结果验证了北京地区城市对下风向地区O3的输送影响.     

对环境空气质量预测中不利气象条件的研究

评价区域内的气象条件是影响大气环境影响预测结果的重要因子.为寻找可能的最大影响,须设置可能发生的不利于污染物传输与扩散的气象条件.分别以城市和郊区的高、中和低架源为例,计算其在各种风速和稳定度组合情况下的最大地面浓度,利用Screen3模式,寻找各类污染源对环境影响最大时的不利气象条件,以及需关注的环境空气敏感点(区).结果表明:小风速和强不稳定度是城市和郊区2类源的不利气象条件;而城市源的不利气象条件还可能出现在小风速和稳定类的情况下. 由于城市高架源影响范围广,评价时更应关注整个评价区域的环境空气敏感点;虽然城市高架源的影响程度比郊区高架源小,但城市低架源的影响程度却大于郊区低架源.      

上海市大气挥发性有机物化学消耗与臭氧生成的关系

本研究基于夏季上海3个不同功能站点臭氧(O3)及其前体物的观测结果,分析了上海不同地区O3及其前体物的污染特征及空间差异;采用参数化的方法估算了VOCs的大气化学消耗水平.结果表明,观测期间上海市区VOCs浓度约为20×10-9,高于西部郊区的17×10-9;两个地区VOCs最大增量反应活性(以O3/VOCs计)的平均值比较接近,约为5.0mol·mol-1.但是,市区VOCs的大气消耗水平(4.0×10-9)不足西部郊区VOCs消耗水平(8.3×10-9)的一半,这是西部郊区O3污染更重的重要原因;东部沿海郊区O3浓度的变化主要是由于区域输送.不同地区VOCs消耗水平与O3生成浓度的比值接近,说明不同地区VOCs消耗生成O3的效率接近;烯烃和芳香烃是最主要的VOCs消耗物种,二者对VOCs消耗量的总贡献高达90%.VOCs的消耗水平在正午达到最大,夜间消耗水平最低,日分布曲线与O3生成的日变化曲线相似,但O3峰值出现时间略晚于VOCs消耗水平峰值出现的时间.     

上海市光化学污染期间挥发性有机物的组成特征及其对臭氧生成的影响研究

光化学污染导致的高浓度臭氧(O3)是上海面临的重要大气污染问题.本研究分别选取了市区(徐汇)、城郊(青浦)和郊区(南汇)3个典型地区在夏季光化学污染易发季节开展了O3及其前体物挥发性有机物(VOCs)和氮氧化物(NOx)的观测,结合光化学箱模型研究探讨了O3生成的主控污染物.研究表明,不同地区O3污染呈现较强的同步性,日最大浓度也比较接近;但南汇郊区由于受机动车排放影响较小,NOx浓度显著低于其他两个地区,导致该地区O3浓度日变化曲线相对平缓,夜间O3浓度也维持在较高水平.大气VOCs浓度较高时,往往伴随高浓度的O3;3个地区VOCs浓度和组成差异明显,就VOCs浓度而言,徐汇青浦南汇;浓度贡献最主要的物种为甲苯、C2~C3的烷烃和烯烃、丙酮以及辛烷;而C7~C10芳香烃、C3~C4的烯烃、异戊二烯以及乙醛是上海大气臭氧生成潜势贡献最大的VOCs类物质.3个地区O3的生成主要受人为排放的二甲苯类和C3~C4烯烃类物质控制;对于徐汇,只控制NOx会导致O3浓度升高,而南汇郊区O3的生成对NOx排放不敏感.     

北京地区SO2、NOx、O3和PM2.5变化特征的城郊对比分析

2006-01-01～2006-12-31在北京上甸子区域大气本底站和城区宝联环境观测站连续观测了SO2、NOx、O3和PM2.5的浓度,分析了北京城区和郊区的季节变化及日变化的差异,并结合风向讨论了城区污染对于大气本底的影响.结果表明,①NOx、SO2浓度在采暖季城郊差异最大,城区是本底的4～6倍,城郊O3有一致的浓度变化.本底站PM2.5在4、5月达到100μg/m3以上,是年平均的2～3倍;②NOx和SO2的日变化在城区表现为双峰型,在09:00前后和22:00前后形成高值,郊区表现为单峰型,在22:00前后出现高值.郊区O3的日变化峰值滞后于城区大约2 h.PM2.5日变化规律表现得较不规则;③西南风条件下本底各污染物浓度明显受城区输送影响而升高,东北风条件下干洁气团的影响比较明显.     

北京市郊区夏季臭氧重污染特征及生成效率

为研究北京郊区夏季O₃(臭氧)重污染过程特征及O₃生成的光化学敏感性,基于2016年夏季在北京郊区开展的针对O₃及其相关污染物的强化观测试验(7月23日—8月31日,共计40 d),分析了观测期间O₃浓度[以φ(O₃)计]变化特征、O₃重污染过程主控因素与O₃敏感性化学特征.结果表明:观测期间φ(O₃)超标时有发生,最大小时φ(O₃)为151.1×10-9,其中有15 d的φ(O₃)最大8 h滑动平均值(O₃-max-8h)超过了GB 3095—2012《环境空气质量标准》二级标准限值,占观测天数的37.5%;不同O₃重污染过程成因有所不同,城市烟羽传输的污染物对郊区O₃重污染过程影响显著(观测期间臭氧重污染过程:过程1,7月27—29日;过程3,8月9—11日;过程4,8月16日;过程5,8月21—24日),区域光化学污染对郊区O₃重污染过程也有贡献(观测期间O₃重污染过程2:8月4—6日);结合后向气流轨迹进一步辅助说明了不同重污染过程中O₃的来源不同.研究还发现,观测区域存在反“周末效应”现象,说明观测区域周末受人为影响较为明显;基于观测数据计算的OPE(O₃生成效率)分析了O₃光化学敏感性表明,在有OPE值的22 d内NO_x控制区和VOCs控制区出现的概率(41%)相等,即观测区域O₃对NO_x和VOCs均敏感;此外还发现,在O₃重污染过程中光化学敏感性会随其反应进程发生改变,由NO_x控制区逐渐转变为VOCs控制区.      

A numerical study of summer ozone concentration over the Kanto area of Japan using the MM5/CMAQ model

We assessed the ability of the MM5/CMAQ model to predict ozone (O3) air quality over the Kanto area and to investigate the factors that a ect simulation of O3. We find that the coupled MM5/CMAQ model is a useful tool for the analysis of urban environmental problems. The simulation results were compared with observational data and were found to accurately replicate most of the important observed characteristics. The initial and boundary conditions were found to have a significant e ect on simulated O3 concentrations. The results show that on hot and dry days with high O3 concentration, the CMAQ model provides a poor simulation of O3 maxima when using initial and boundary conditions derived from the CMAQ default data. The simulation of peak O3 concentrations is improved with the JCAP initial and boundary conditions. On mild days, the default CMAQ initial and boundary conditions provide a more realistic simulation. Meteorological conditions also have a strong impact on the simulated distribution and accumulation of O3 concentrations in this area. Low O3 concentrations are simulated during mild weather conditions, and high concentrations are predicted during hot and dry weather. By investigating the e ects of di erent meteorological conditions on each model process, we find that advection and di usion di er the most between the two meteorological regimes. Thus, di erences in the winds that govern the transport of O3 and its precursors are likely the most important meteorological drivers of ozone concentration over the central Kanto area.     

Urban and rural transport of semivolatile organic compounds at regional scale: A multimedia model approach

Urban areas are generally regarded as major sources of some semivolatile organic compounds and other persistent organic pollutants(POPs) to the surrounding regions. Huge differences in contaminant emissions between urban and rural areas directly affect their fate in environmental media. Little is known about POPs behavior between urban and rural areas at a regional scale. A spatially resolved Berkeley-Trent-Urban-Rural Fate Model(BETR-UR) was designed by coupling land cover information to simulate the transport of POPs between urban and rural areas, and the Bohai Rim was used as a case study to estimate Polycyclic Aromatic Hydrocarbon(PAH) fate. The processes of contaminant fate including emission, inter-compartmental transfer, advection and degradation in urban and rural areas were simulated in the model. Simulated PAH concentrations in environmental media of urban and rural areas were very close to measured values. The model accuracy was highly improved, with the average absolute relative error for PAH concentrations reduced from 37% to 3% compared with unimproved model results. PAH concentrations in urban soil and air were considerably higher than those in rural areas. Sensitivity analysis showed temperature was the most influential parameter for Phen rather than for Bap, whose fate was more influenced by emission rate, compartment dimension, transport velocity and chemical persistence. Uncertainty analysis indicated modeled results in urban media had higher uncertainty than those in rural areas due to larger variations of emissions in urban areas. The differences in urban and rural areas provided us with valuable guidance on policy setting for urban–rural POP control.     

长江三角洲地区大气O3和PM10的区域污染特征模拟

以TRACE-P污染源资料及上海市地方排放清单为基础,采用Models-3/CMAQ环境空气质量模型和中尺度气象模式MM5,模拟研究了2001-01和2001-07长三角近地面二次污染物O₃及PM₁₀的浓度分布及输送状况,并以上海市国控点2001年冬、夏季各10 d的小时监测数据对模型进行了验证.验证结果显示,Models-3/CMAQ对O₃和PM₁₀的模拟结果与监测值的相关系数分别为0.77和0.52;一致性指数分别达到0.81和0.99.模型对O₃小时最高浓度的估算偏低27%,标准偏差为-3.1%;对PM₁₀小时平均浓度的估算偏低10%,标准偏差为46%.模型已具备再现和模拟长三角大气污染输送过程的能力,且误差落在可接受的范围之内.模拟结果显示,2001-07长三角区域16个主要城市中,有14个城市O₃小时最大浓度超过国家二级标准,高浓度O₃可覆盖苏南和浙北广大区域.2001-01泰州、扬州、南京、镇江、常州等城市受本地排放源和北部大气污染输送的影响显著,大气PM₁₀日均浓度超过PM₁₀国家二级标准.长三角地区环境空气质量与污染类型受大气污染传输与化学转化的影响十分明显.夏季太阳辐射较强时,南部城市排放的污染物常以二次污染物的形式影响下风向城市;太阳辐射较弱的情况下,则以一次污染物输送为主的形式影响周边地区.冬季长三角区域颗粒物污染总体水平较高,这与我国北方地区排放的颗粒物在西北风作用下向长三角输送造成的影响密切相关.长三角地区的大气污染已逐渐从局地转为区域问题.     

被动采样监测珠江三角洲NOx、SO2和O3的空间分布特征

为获得珠江三角洲区域污染特征,采用被动扩散采样技术,在珠江三角洲200 km×200 km网格区域内测量11月两周暴露的NO2、SO2和O3浓度水平,采用克里格空间插值法(Kriging)获取NOx、SO2和O3的空间分布特征,并与源清单和已有模型结果比对.采用反向轨迹方法模拟了O3的输送途径.结果表明,采样期间珠江三...     

长江三角洲地区对流层臭氧的数值模拟研究

将NCAR的中尺度天气预报模式MM5和作者开发的化学模式相耦合,建立了一个中尺度区域空气质量模式.利用该模式选取了2个典型个例研究了长江三角洲地区的区域臭氧化学问题.本研究的目的是利用模式再现并描述长江三角洲地区的大气物理化学过程,结合地面观测资料进一步定量分析控制该地区臭氧浓度的物理和化学因子.通过个例模拟和分析表明,模式基本反应了长江三角洲地区的大气物理化学过程,进一步的因子分析解释了模拟区域内1999 06 18(个例2)臭氧浓度普遍比1999 08 07(个例1)的臭氧浓度高的原因.模拟结果表明天气条件决定的大气动力过程对区域空气质量起着至关重要的作用,这也是个例2区域臭氧浓度普遍偏高的最主要因素之一.分析表明,物理因子(平流输送,垂直湍流输送)的作用和化学因子的作用同样重要.同时还做了模式参数的敏感性实验研究,并对中尺度云雨化学模拟及其对臭氧化学的影响做了初步研究.     

上海地区臭氧数值预报

基于WRF-Chem在线区域化学/传输模式构建了区域化学天气数值预报业务系统,评估了2013年5月1日至9月30日期间的1h和8h臭氧业务数值预报效果.结果表明:臭氧预报没有明显的系统偏差,预报偏差在0两侧基本呈对称分布;数值预报具有较高的准确性,其中8h臭氧的效果略好,不同时效预报的相关系数均在0.8上下,浓度平均偏差和偏差中值都只有1′10-9~2′10-9,臭氧达标日和污染日预报都有很高准确率和CSI/TS评分,首要污染物也较准确;不同时效的预报效果接近,48h时效略好,24h和72h相当;数值预报也存在一定不足,存在极个别显著偏高或显著偏低的情况,同时由于等级划分阈值的存在,等级预报的准确性明显低于浓度和分指数预报.综合地看,数值预报可以提供较为准确的臭氧预报,为空气质量预报预警业务提供有力的支撑,但分指数等级预报上仍需要进一步提高.