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1.
近年来近地面臭氧问题日益凸显,成为影响空气质量持续改善的瓶颈.本研究基于2017年8—9月在湖州市城区开展的为期1个月的臭氧及其前体物挥发性有机物（VOCs）和氮氧化物（NOx）在线观测数据,分析了臭氧及其前体物污染特征,利用正矩阵因子分析（PMF）解析了VOCs来源,并采用基于观测的模型（OBM）对臭氧生成机制进行研究.研究结果表明：1）观测期间湖州市VOCs平均体积分数为（24.78±9.10）×10-9,其中占比最高的组成为烷烃、含氧VOCs （OVOCs）和卤代烃;2）在臭氧非超标时段,湖州市臭氧生成处于VOCs控制区,而在臭氧重污染期间湖州市处于以VOCs控制为主的过渡区;3）在臭氧超标时段,对臭氧生成潜势（OFP）贡献最大的是芳香烃（39.6%）,其次是烯烃（21.5%）和OVOCs （19.4%）,排名前三的关键组分为甲苯、乙烯和间/对二甲苯;4）源解析结果显示观测期间湖州市VOCs的主要来源是溶剂使用（27.0%）、交通排放（22.7%）、背景+传输（19.3%）、工业排放（16.9%）、汽油挥发（7.7%）和植物排放（6.4%）,重污染过程期间对OFP贡献最大的两类源是交通排放源和溶剂使用源,贡献百分比分别为35.1%和30.5%.因此,对交通排放和溶剂使用方面进行控制管理对湖州市大气臭氧污染防控有重要意义. 相似文献
2.
利用气相色谱-质谱仪/火焰离子检测器（Online-GC-MS/FID）对2017年冬季山东德州大气中99种挥发性有机物（VOCs）进行连续测量,研究了VOCs浓度和组分特征、日变化趋势、来源及其对臭氧（O3）、二次有机气溶胶（SOA）生成的贡献.结果表明,德州大气VOCs平均体积分数为（47.74±33.11）×10-9,烷烃占比最大,为40.66%.总VOCs及其组分表现出早晚体积分数高、中午体积分数低的日变化规律.德州大气中丙烷、丙烯、苯及甲苯和二氯甲烷分别受到液化石油气挥发、生物质燃烧、机动车排放和溶剂使用等人为源的影响.反向轨迹模型分析发现,北方内陆气团对德州VOCs体积分数具有一定贡献.烷烃、烯烃、芳香烃的臭氧生成潜势分别为（34.87±33.60）、（120.48±118.76）和（59.77±94.14）μg/m3,乙烯、丙烯、甲苯和间/对二甲苯的贡献较大.芳香烃氧化主导了SOA生成,其贡献率为93.7%,甲苯、间/对二甲苯、苯对SOA生成的贡献最大.为解决大气复合污染问题、实现臭氧和PM2.5协同控制,德州应重点控制甲苯、间/对二甲苯等芳香烃的排放. 相似文献
3.
利用2019年8月13日—9月30日江苏省13个设区市离线监测的VOCs数据,对江苏省城区VOCs污染特征及其关键活性组分进行分析研究.结果表明,江苏省逐日VOCs的体积分数范围为8.83×10-9~45.11×10-9,表现为烷烃 > 芳香烃 > 烯烃 > 炔烃.江苏省13个设区市VOCs的体积分数为7.85×10-9~30.52×10-9,徐州市VOCs最高,这与徐州市监测点位置分布及其工业结构相关.全省13个设区市臭氧浓度处于优、良、轻度污染和中度污染时,VOCs总体积分数分别为14.96×10-9、17.96×10-9、25.85×10-9和25.11×10-9,臭氧浓度处于污染状态时的VOCs高于优、良状态,且炔烃占比随着臭氧污染程度的加重呈升高趋势,表明现阶段臭氧生成与人类活动关系密切.通过加权的方式筛选出间/对二甲苯、乙烯、甲苯、丙烯、异戊二烯、邻二甲苯等物种,它们是目前对江苏省城区影响程度较大且影响范围较广的关键活性物种. 相似文献
4.
餐饮排放是城市地区挥发性有机物（VOCs）重要的无组织来源,由于其排放特征复杂,是大气环境研究和管理的薄弱环节.本研究采用了现场和实验模拟两种采样方式,利用2,4-二硝基苯肼（DNPH）采样柱和不锈钢罐分别采集羰基化合物和全空气样品,然后利用高效液相色谱（HPLC）和气相色谱-质谱联用仪（GC-MS/FID）对116种组分进行定性定量分析.在此基础上,分析了餐饮源VOCs的排放特征及其影响因素.总体来看,含氧有机物（OVOCs）和烷烃是VOCs浓度的主要贡献者,但不同餐饮源的源谱特征差异较大.另外,通过比较发现食用油的种类、油的使用次数、加热方式、烹饪方式和调味料等因素会对餐饮源VOCs排放特征造成显著影响.进一步分析了不同菜系所排放VOCs的臭氧生成潜势（OFP）,关键组分主要是甲醛、乙醛、丁烯醛、乙烯和丙烯等.本研究成果能够补充我国餐饮源VOCs控制所需的基础数据. 相似文献
5.
臭氧污染是我国当前面临的重要大气环境问题,其不仅取决于大气化学反应过程,而且会受大气物理过程和各气象要素的影响,因此需要从化学和物理两个方向来研究近地面臭氧污染问题。本研究结合外场观测和欧拉光化学模式,解析了2022年秋季北京怀柔城区的一次光化学污染周期内的物理和化学过程。给出了温度、湿度和风速等气象因子,以及臭氧及其前体物挥发性有机物(VOCs)和氮氧化物(NOx,x=1、2)在此期间的日变化特征。通过源解析得到VOCs主要来源为交通排放(46%)、植物源(25%)、溶剂挥发(23%)和燃烧源(9%)。通过欧拉光化学模式确定了区域传输和本地VOCs对臭氧的贡献,结果显示强北风天气条件下,怀柔区臭氧以外来水平输送为主(贡献超过70%);当以弱的南风或东南风为主时,天气处于稳定状态,臭氧主要来自VOCs和NOx的二次转化。根据VOCs的臭氧潜势,在所有VOCs中对臭氧贡献最大的物质为烯烃,其贡献为67%,其次为芳香烃(16%)。通过敏感度分析,发现臭氧生成对物理因子中的光强、温度和边界层高度最敏感;在臭氧前体物中,活性较强的烯烃类物质的敏感度最... 相似文献
6.
近年来,我国东部地区夏季臭氧污染问题日渐凸显,成为影响空气质量、环境改善的重要因素之一,为量化评估臭氧前体物减排对臭氧污染的影响,本文以2021年6月19—30日中国东部地区臭氧污染过程为例,应用空气质量模型CMAQ-DDM方法与卫星遥感反演算法分析了东部地区臭氧浓度对人为源前体物排放敏感性的响应程度,并对臭氧前体物设置不同削减比例开展减排情景模拟,结果表明:1)2021年6月19—30日中国东部出现了一次长时间区域性臭氧污染过程,大部分城市达轻度至中度污染水平;2)整个污染时段东部地区主要以VOCs(Volatile Organic Compounds,挥发性有机物)控制区或VOCs与NOx协同控制区为主,模型模拟与卫星反演结果具有较好的一致性,污染过程前段(19—25日)东部地区对VOCs敏感性较高,污染后段(26—30日)大部分地区转为VOCs和NOx协同控制区,特别是河南、安徽、江苏部分地区,对NOx敏感性提高较为显著;3)在相同减排比例条件下(VOCs∶NOx=2∶1),减排幅度越大,臭氧降幅越大,当VOCs削减比例由20％提高到40％时,臭氧浓度降幅由1.7％增大至3.6％;由VOCs和NOx协同减排(2∶1)过渡为强化NOx减排(1∶1)的分阶段控制优于单一的减排控制方案,臭氧改善率平均增强0.1％;仅削减高架源NOx对臭氧降幅不显著。 相似文献
7.
挥发性有机物（VOCs）是臭氧和大气颗粒物的重要前体物,本研究利用在线气相色谱-质谱仪（Online-GC-MS）于2018年5—6月对江苏省泰州市大气中98种VOCs进行监测,依据监测结果对泰州市大气VOCs的组成特征、日变化趋势进行分析,对醛酮类VOCs数据进行参数化拟合探究其一次二次贡献,并采用正矩阵因子分解模型（PMF）对VOCs数据进行来源分析,用最大增量反应活性（MIR）计算臭氧生成潜势（OFP）.研究结果表明：泰州市大气VOCs中烷烃占比最高,其次为醛酮;烷烃、烯烃、卤代烃和芳香烃浓度日变化趋势明显,特征相近;参数化方法表明醛类物质主要来自于二次生成,而酮类物质主要来自一次排放;PMF模型结果表明泰州市VOCs的主要贡献源分别为机动车排放、油气溶剂挥发、生物质燃烧、其他工业和天然源;OFP的主要贡献物种为烯烃类,占比34.18%.研究结果表明,控制工业排放和溶剂使用是泰州市大气污染物控制的重点. 相似文献
8.
疫情期间全球各地一次排放大幅削减,而臭氧等二次污染的响应则存在着区域间差异.结合地面和卫星观测发现,同在氮氧化物大幅下降的情况下,臭氧在东亚和欧洲呈现出可达14ppb的上升信号,而北美则下降为主(约2-4ppb).我们结合气象分析和臭氧敏感性进一步讨论了臭氧响应差异性的原因,一方面受臭氧与前体物间关系的影响;另一方面来自于气象,尤其是温度.研究明晰了人为排放,化学和气象三者的内在关联,强调了在臭氧控制过程中考虑前体物削减和气象条件协同的重要性. 相似文献
9.
临安秋季近地层臭氧的形成及其前体物特征 总被引：11，自引：2，他引：11
应用浙江临安1999年秋季观测数据,分析了臭氧及其前体物特征与气象条件的关系。结果表明,该地区臭氧前体物丰富,在合适的天气条件、充足的日照下可以生成高浓度的臭氧;CO、NOx*等一次污染物浓度与大尺度大气扩散稀释能力有关;观测期间临安CO浓度很高;NMHCs以芳香烃含量最高,烷烃、烯烃、炔烃次之,生物排放的烃最少。以观测为基础的光化学模式计算表明,临安光化学臭氧生成率比损失率大一个数量级,中午净臭氧生成率最大可达14.8×10-9h-1。 相似文献
10.
传统的空气质量模型多使用简化的光化学反应机制来模拟大气污染物的形成.这些机制主要基于烟雾箱实验拟合的反应速率和产物来模拟二次产物（如臭氧（O3））前体物的氧化反应,具有一定的不确定性,导致模拟结果产生偏差.针对该问题,本研究将详细的大气化学机理（MCMv3.3.1）与美国国家环境保护局研制的第三代空气质量预报和评估系统CMAQ相结合（CMAQ-MCM）,模拟研究长三角地区2015年8月27—9月5日臭氧高发时段的空气质量.CMAQ-MCM模型可以较好地模拟长三角地区6个代表城市O3和其前体物随时间的变化趋势.对模拟的O3日最大8 h平均浓度的统计分析表明,徐州表现最好（标准平均误差=-0.15,标准平均偏差=0.23）.在长三角地区,居民源对挥发性有机物（VOCs）的贡献最大,占39.08%,其次是交通运输（33.25%）和工业（25.56%）.能源对总VOCs的贡献最小,约为2.11%.对活性氧化氮（NOy）的分析表明,其主要组分是NOx（80%）,其次是硝酸（HNO3）（<10%）.O3的空间分布与NOy和NOx非常相似.HCHO等其他氧化产物的分布与NOx相似,这很可能是由于在高NOx条件下VOCs氧化产生的产物.甲基乙烯基酮（MVK）和甲基丙烯醛（MACR）的空间分布与自然源VOCs （BVOCs）非常相似,表明长三角地区MVK和MACR主要由BVOCs氧化生成.长三角地区受到人为源和自然源排放相互作用的影响. 相似文献
11.
过氧乙酰硝酸酯（PAN）是由VOCs和NOx的光化学反应生成的一种典型二次污染物,比O3更适合作为光化学污染的指示剂.2019年6—10月对浙江中部盆地金华市大气中PAN进行了在线监测,并对影响其体积分数变化的因素进行了分析,同时还分析了一次典型的光化学污染过程.结果表明,观测期间PAN的平均体积分数为0.656×10-9,最高体积分数为4.348×10-9,日均体积分数水平在0.130×10-9~2.203×10-9之间.PAN日变化特征显著,9月为明显的双峰变化,其他月份均为单峰.受气象条件的影响,夏季的污染程度显著低于秋季.9月27—30日典型污染时段内,PAN的小时均值是整个观测期均值的2.8倍,污染以本地积累为主.前体物浓度水平差异与去除机制的不同是影响PAN和O3相关性的重要因素,此外NO/NO2的比值是影响PAN生成速率的重要因素,PAN的峰值基本出现在NO/NO2比值较低的时段.在生成PAN的VOCs物种中,丙烷、乙烷和间/对二甲苯所占比例较大. 相似文献
12.
Modeling of Regional High Ozone Episode Observed at Two Mountain Sites (Mt. Tai and Huang) in East China 总被引：3，自引：0，他引：3
Zifa Wang Jie Li Xiquan Wang Pakpong Pochanart Hajime Akimoto 《Journal of Atmospheric Chemistry》2006,55(3):253-272
A high O3 episode was observed during 23–25 May 2004 at two high-mountain sites reflecting the regional pattern of air pollutants over East China. This episode lasted about three days with the maximum hourly O3 mixing ratios reaching 111 and 114 ppbv at Mt. Tai and Huang, respectively. Backward trajectories and meteorological analysis indicated that regional transport, associated with a weak high pressure system over the East China Sea, might play an important role in the formation of this high ozone episode. The nested air quality prediction modeling system (NAQPMS) was applied to investigate the formation and evolution of this high O3 event. The comparison of model results with observations showed that NAQPMS successfully reproduced the main observed patterns of O3 and meteorological parameters during the simulated period. The model results with emission over the Yangtze Delta and the East Central China switched on/off clearly showed that ozone and its precursors transported from the Yangtze Delta and the East Central China enhanced the high ozone episode at two sites, with a contribution of 20%–50% during the episode. In addition, based on process analysis with the model, chemical production and regional transport appeared to be the main causes of high ozone episode involving a large amount of high-ozone air masses and precursors transported from the surrounding areas. The horizontal transport is more active during the period of high ozone episode than that during the non-episode at Mt. Tai as well as Mt. Huang. 相似文献
13.
O. Klemm W. R. Stockwell H. Schlager M. Krautstrunk 《Journal of Atmospheric Chemistry》2000,35(1):1-18
The ozone forming potential of VOCs and NOx for plumes observed from several cities and a power plant in eastern Germany was investigated. A closed box model with a gas phase photochemical reaction mechanism was employed to simulate several scenarios based upon aircraft observations. In several of the scenarios, the initial concentrations of NOx, VOCs, and SO2, were reduced to study the factors limiting the O3 production. Ozone production was limited by the initial VOC concentrations for all of the simulated plumes. Higher O3 concentrations were produced with reduced initial NOx. In one sample with high SO2 mixing ratios (>100 ppb), SO2 was also identified as a significant contributor to the production of O3. 相似文献
14.
Daily, weekly, and seasonal patterns of O3, NOx
x and VOCs and their relationship to meteorological conditions were studied in a semi-urban site near Barcelona by means of five-day long campaigns that included weekend and labor days in December, March, June, and October. The plant protection thresholds for ozone and NO2 were exceeded, respectively, on all the studied days in summer and on all the studied days. Ozone formation was predominantly local and relied on photochemical processes with VOCs playing a controlling role. Formaldehyde, acetaldehyde, methanol, toluene, isoprene, and acetone (in this order) presented the highest O3 formation potential during the studied periods. These results highlight the important role in O3 formation played by VOC species such as acetaldehyde, methanol, and acetone, that all have a significant biogenic component. Thus, these VOCs must be taken into account in the discussion of any ozone abatement strategy. 相似文献
15.
Meng CUI Xingqin AN Li XING Guohui LI Guiqian TANG Jianjun HE Xin LONG Shuman ZHAO 《大气科学进展》2021,38(7):1223-1237
This study uses the WRF-Chem model combined with the empirical kinetic modeling method (EKMA curve) to study the compound pollution event in Beijing that happened in 13-23 May 2017. Sensitivity tests are conducted to analyze ozone sensitivity to its precursors, and to develop emission reduction measures. The results suggest that the model can accurately simulate the compound pollution process of photochemistry and haze. When VOCs and NOx were reduced by the same proportion, the effect of O3 reduction at peak time was more obvious, and the effect during daytime was more significant than at night. The degree of change in ozone was peak time > daytime average. When reducing or increasing the ratio of precursors by 25％ at the same time, the effect of reducing 25％ VOCs on the average ozone concentration reduction was most significant. The degree of change in ozone decreased with increasing altitude, the location of the ozone maximum change shifted westward, and its range narrowed. As the altitude increases, the VOCs-limited zone decreases, VOCs sensitivity decreases, NOx sensitivity increases. The controlled area changed from near-surface VOCs-limited to high-altitude NOx-limited. Upon examining the EKMA curve, we have found that suburban and urban are sensitive to VOCs. The sensitivity tests indicate that when VOCs in suburban are reduced about 60％, the O3-1h concentration could reach the standard, and when VOCs of the urban decreased by about 50％, the O3-1h concentration could reach the standard. Thus, these findings could provide references for the control of compound air pollution in Beijing. 相似文献
16.
Temporal variations in surface ozone and its precursors and meteorological effects at an urban site in China 总被引：3，自引：2，他引：3
Continuous measurements of ozone and its precursors including NO, NO2, and CO at an urban site (32°03′N, 118°44′E) in Nanjing, China during the period from January 2000 to February 2003 are presented. The effects of local meteorological conditions and distant transports associated with seasonal changed Asian monsoons on the temporal variations of O3 and its precursors are studied by statistical, backward trajectory, and episode analyses. The diurnal variation in O3 shows high concentrations during daytime and low concentrations during late night and early morning, while the precursors show high concentrations during night and early morning and low concentrations during daytime. The diurnal variations in air pollutants are closely related to those in local meteorological conditions. Both temperature and wind speed have significant positive correlations with O3 and significant negative correlations with the precursors. Relative humidity has a significant negative correlation with O3 and significant positive correlations with the precursors. The seasonal variation in O3 shows low concentrations in late autumn and winter and high concentrations in late spring and early summer, while the precursors show high concentrations in late autumn and winter and low concentrations in summer. Local mobile and stationary sources make a great contribution to the precursors, but distant transports also play a very important role in the seasonal variations of the air pollutants. The distant transport associated with the southeastern maritime monsoon contributes substantially to the O3 because the originally clean maritime air mass is polluted when passing over the highly industrialized and urbanized areas in the Yangtze River Delta. The high frequency of this type of air mass in summer causes the fact that a common seasonal characteristic of surface O3 in East Asia, summer minimum, is not observed at this site. The distant transports associated with the northern continental monsoons that dominate in autumn and winter are related to the high concentrations of the precursors in these two seasons. This study can contribute to a better understanding of the O3 pollution in vast inland of China affected by meteorological conditions and the rapid urbanization and industrialization. 相似文献
17.
The halogen ions Br- and Cl- together with NO3
-, SO4
=, MSA- (methane sulfonate), Na+ and NH4
+ were analysed by ion chromatography in extracts of more than 800 aerosol cellulose filter samples taken at Ny Ålesund, Svalbard (79°N, 12°E) in spring 1996 (March 27 - May 16) within the European Union project ARCTOC (Arctic Tropospheric Ozone Chemistry). Anticorrelated variations between f-Br (filterable bromine, i.e. water soluble bromine species that can be collected by aerosol filters) and ozone within the arctic troposphere were evaluated at a resolution of 1 or 2 hours for periods with depleted ozone and 4 hours at normal ozone. A mean f-Br concentration of 11 ng m-3 (0.14 nmol m-3) was observed for the whole campaign, while maximum concentrations of 80 ng m-3 (1 nmol m-3) were detected during two total O3-depletion events (O3 drop to mixing ratios below the detection limit of < 2 ppb). Anticorrelation between f-Br and O3 was also seen during minor O3-depletion episodes (sudden drop in O3 by at least 10 ppb, but O3 still exceeding the detection limit) and even for ozone variations near its background level (40-50 ppb). A time lag of about 10 hours between the change of ozone and of f-Br concentrations could only be found during a total ozone depletion event, when f-Br reached its maximum values several hours after ozone was totally destroyed. Bromine oxide (BrO) concentrations, measured by DOAS (Differential Optical Absorption Spectroscopy), and f-Br showed a coincident variability during almost the entire campaign (except in the case of total O3-loss). Frequently enhanced anthropogenic nitrate and sulphate concentrations were observed during O3-depletion periods. At O3 concentrations < 10 ppb sulphate and nitrate exceed their typical mean level by 54% and 77%, respectively. This may indicate a possible connection between acidity and halogen release. 相似文献
18.
G. Salisbury P. S. Monks S. Bauguitte B. J. Bandy S. A. Penkett 《Journal of Atmospheric Chemistry》2002,41(2):163-187
Measurements of the sum of peroxy radicals [HO2 + RO2],NOx (NO + NO2) and NOy (the sum of oxidisednitrogen species) made at Mace Head, on the Atlantic coast of Ireland in summer 1996 and spring 1997 are presented. Together with a suite of ancillary measurements, including the photolysis frequencies of O3 O(1D)(j(O1D)) and NO2 (j(NO2)), the measured peroxy radicals are used to calculate meandailyozone tendency (defined as the difference of the in-situphotochemical ozone production and loss rates); these values are compared with values derived from the photochemical stationary state (PSS) expression. Although the correlation between the two sets of values is good, the PSS values are found to be significantly larger than those derived from the peroxy radical measurements, on average, in line with previous published work. Possible sources of error in these calculations are discussed in detail. The data are further divided up into five wind sectors, according to the instantaneous wind direction measured at the research station. Calculation of mean ozone tendencies by wind sector shows that ozone productivity was higher during spring (April–May) 1997 than during summer (July–August) 1996across all airmasses, suggesting that tropospheric photochemistry plays an important role in the widely-reported spring ozone maximum in the Northern Hemisphere. Ozone tendencies were close to zero for the relatively unpolluted south-west, west and north-west wind sectors in the summer campaign, whereas ozone productivity was greatest in the polluted south-east sector for both campaigns. Daytime weighted average ozone tendencies were +(0.3± 0.1) ppbv h–1 for summer 1996 and +(1.0± 0.5) ppbvh–1 for spring 1997. These figures reflect the higher mixing ratios of ozone precursors in spring overall, as well as the higher proportion of polluted air masses from the south-east arriving at the site during the spring campaign. The ozone compensation point, where photochemical ozone destruction and production processes are in balance, is calculated to be ca. 14 pptv NO for both campaigns. 相似文献