我国典型城市群O_3污染成因和关键VOCs活性解析

京津冀、长三角、珠三角和成渝地区四大城市群在夏秋季大气臭氧(O_3)污染问题严重.为了深入认识O_3的区域污染特征及其成因,在上述4个城市群于2014~2016年夏秋季节,开展了大气O_3及其前体物(氮氧化物(NOx)、挥发性有机物(VOCs))等的综合观测研究.观测发现,臭氧污染区域性明显,臭氧最大8h值在59~146(10^(-9)V/V),整体上城市站点臭氧浓度水平较郊区站点低,臭氧前体物NO2平均浓度水平在4~22(10^(-9)V/V),VOCs浓度为11~53(10^(-9)V/V),VOCs活性水平在1.6~10.5s^(-1).使用基于观测的盒子模型(OBM)分析臭氧生成控制区,发现四大城市群的O_3生成多数处于人为源VOCs控制区或者过渡区,且对烯烃和芳香烃的敏感性最强.运用PMF受体模型对城市站点VOCs来源进行解析,结果表明机动车尾气排放和汽油挥发是城市VOCs主要来源,占比30%~50%;溶剂涂料使用其次,占比为10%~20%.综合而言,我国现阶段臭氧污染防控应以VOCs控制为主,其中应着重控制机动车尾气排放和溶剂涂料使用.

Long-term trends of fine particulate matter and chemical composition in the Pearl River Delta Economic Zone （PRDEZ）, China

Understanding essential for formulating the trends in PM2.5 levels is clean air plans. This paper analyzes PM2.5 data from various published sources for the years 2000 to 2010 in the Pearl River Delta Economic Zone （PRDEZ）. The long-term variation in PM2.5 mass concentration is analyzed. Results show that PM2.5, organic carbon （OC）, elemental carbon （EC）, and SO24 show a similar trend, increasing before 2005 and then decreasing slightly. The annual average PM2.5 concentra- tion ranges from 49.1 μg·m-3 in 2000 to 64.3 μg·m-3 in 2010, with a peak of 84.1 μg· m3 in 2004. None of these 11 years meets the new National Ambient Air Quality standard （NAAQS） for PM2.5 （35 μg· m-3）. Overall average concentrations of OC, EC, and SO2/4 are 13.0, 6.5, and 11.8μg·m-3, respectively. NO3 and NH＋ respectively have concentrations of 1.5 μg·m-3 and 2.9 μg·m-3 in 2000 and 6.4 μg·m 3 and 5.3μg·m-3 in 2010, with a statistically significant average annual trend of＋ 0.2 μg·m-3 ·yr-1 and ＋ 0.1 μg· m-3. yr-1. In certain geographic regions, OC and EC contribute most of the PM2.5, while in other regions secondary water-soluble ions are more important. In general, OC and SO2/4- are the dominant components of PM2.5, contributing 20.6% and 18.6%, respectively. These results provide, for the first time, a better understanding of the long-term PM2.5 characteristics and trends, on a species-by-species basis, in the PRDEZ. The results indicate that PM2.5 abatement needs to prioritize secondary species.

Fast increasing of surface ozone concentrations in Pearl River Delta characterized by a regional air quality monitoring network during 2006–2011

Based on the observation by a Regional Air Quality Monitoring Network including 16 monitoring stations, temporal and spatial variations of ozone （O3）, NO2 and total oxidant （Ox） were analyzed by both linear regression and cluster analysis. A fast increase of regional O3 concentrations of 0.86 ppbWyr was found for the annual averaged values from 2006 to 2011 in Guangdong, China. Such fast O3 increase is accompanied by a correspondingly fast NOx reduction as indicated by a fast NO2 reduction rate of 0,61 ppbV/yr. Based on a cluster analysis, the monitoring stations were classified into two major categories - rural stations （non-urban） and suburban/urban stations. The 03 concentrations at rural stations were relatively conserved while those at suburban/urban stations showed a fast increase rate of 2.0 ppbV/yr accompanied by a NO2 reduction rate of 1.2 ppbV/yr. Moreover, a rapid increase of the averaged O3 concentrations in springtime （13%/yr referred to 2006 level） was observed, which may result from the increase of solar duration, reduction of precipitation in Guangdong and transport from Eastern Central China. Application of smog production algorithm showed that the photochemical O3 production is mainly volatile organic compounds （VOC）-controlled. However, the photochemical O3 production is sensitive to both NOx and VOC for O3 pollution episode. Accordingly, it is expected that a combined NOx and VOC reduction will be helpful for the reduction of the O3 pollution episodes in Pearl River Delta while stringent VOC emission control is in general required for the regional O3 pollution control.

A meteorologically adjusted ensemble Kalman filter approach for inversing daily emissions:A case study in the Pearl River Delta,China

The conventional Ensemble Kalman filter(EnKF),which is now widely used to calibrate emission inventories and to improve air quality simulations,is susceptible to simulation errors of meteorological inputs,making accurate updates of high temporal-resolution emission inventories challenging.In this study,we developed a novel meteorologically adjusted inversion method(MAEInv)based on the EnKF to improve daily emission estimations.The new method combines sensitivity analysis and bias correction to alleviate the inversion biases caused by errors of meteorological inputs.For demonstration,we used the MAEInv to inverse daily carbon monoxide(CO)emissions in the Pearl River Delta(PRD)region,China.In the case study,60%of the total CO simulation biases were associated with sensitive meteorological inputs,which would lead to the overestimation of daily variations of posterior emissions.Using the new inversion method,daily variations of emissions shrank dramatically,with the percentage change decreased by 30%.Also,the total amount of posterior CO emissions estimated by the MAEInv decreased by 14%,indicating that posterior CO emissions might be overestimated using the conventional EnKF.Model evaluations using independent observations revealed that daily CO emissions estimated by MAEInv better reproduce the magnitude and temporal patterns of ambient CO concentration,with a higher correlation coefficient(R,+37.0%)and lower normalized mean bias(NMB,-17.9%).Since errors of meteorological inputs are major sources of simulation biases for both low-reactive and reactive pollutants,the MAEInv is also applicable to improve the daily emission inversions of reactive pollutants.

Space view of the decadal variation for typical air pollutants in the Pearl River Delta （PRD） region in China

The Pearl River Delta （PRD） is one of the most industrialized, urbanized and populated regions in China, and thus has been long suffering from severe air pollutions. Space data provide a unique perspective for investigating the atmospheric environment at a regional scale. By utilizing multiple satellite retrievals from 2005 to 2013, this study presented, for the first time, the spatial patterns and temporal trends of typical air pollutants over PRD and its vicinity. As viewed from space, aerosol optical depth （AOD）, NO2 and SO2 all had their higher values at the central part of PRD, and showed clear descending gradients as moving to the outskirt of this region. As to the inter-annual variation, all these pollutants had decreasing trends in PRD during the study period, which generally agreed with the relevant in situ measurements. However, the satellite retrievals differed from ground measurements when addressing NO2 and SO2 in the vicinity of PRD. This work also provides the inter-comparison among PRD and three other metropolitan clusters in China： PRD had relatively high AOD, moderate NO2 and low SO2 levels, and it was the only region achieving the effective reduction of NO2 and SO2 during last decade. Unlike the previous three pollutants, HCHO observed by satellite showed very special patterns： it had a relatively homogeneous spatial distribution over both of PRD and its vicinity, and presented an opposite increasing trend from 2005 to 2010. Moreover, PRD had the highest HCHO level among all the metropolitan clusters, hinting a considerable contribution of biogenic origins of HCHO in PRD.