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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.
于2016年7月-2017年6月在武汉市典型居民区对大气中101种挥发性有机物（VOCs）进行了监测,以便研究武汉市典型居民区周边VOCs的组成特征和变化规律,并探讨了其主要来源.结果表明,武汉市空气中VOCs的体积分数为（46.24±24.57）×10-9,表现为烷烃>含氧有机物>烯烃>卤代烃>芳香烃.受交通排放影响烷烃的比例上午高于下午,1月机动车尾气为武汉市主要的VOCs排放源,夏季含氧类化合物浓度高于冬季,可能更多地受本地喷涂等溶剂使用行业和光化学反应生成的影响,5-9月表现出明显的生物源排放特征.利用正交矩阵因子分析（PMF）得到武汉市居民区大气VOCs主要有6个来源,分别为燃烧源、机动车尾气、工业排放、溶剂使用、汽油挥发和植物排放.其中,燃烧源、机动车尾气贡献比例最高,是该区域VOCs控制的重要排放源.  相似文献   

3.
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   

4.
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   

5.
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   

6.
近年来武汉市臭氧污染日益严峻,成为影响空气质量达标的瓶颈,弄清臭氧及其前体物非线性关系是臭氧防控的关键和基础.本研究基于武汉中心城区2018年4—9月臭氧及其前体物在线观测数据,分析出武汉市臭氧浓度受前体物和气象条件等因素的共同影响,呈较为明显的季节变化和日变化特征.观测期间武汉市大气挥发性有机物（VOCs）平均体积分数为32.5×10-9,烷烃是武汉市VOCs的主要组分,其次是含氧VOCs （OVOCs）和卤代烃.利用基于观测的模型定量分析臭氧与前体物之间的关系,发现削减VOCs会引起臭氧生成潜势的显著下降,而削减氮氧化物则会使臭氧生成潜势升高,说明武汉市臭氧生成处于VOCs控制区.在人为源VOCs中,间/对二甲苯和邻二甲苯的相对增量反应活性（RIR）最高,是影响臭氧生成的关键组分.  相似文献   

7.
PMF和PCA/APCS模型对南京北郊大气VOCs源解析对比研究   总被引：6，自引：0，他引：6  
利用PMF模型和PCA/APCS模型对南京北郊大气VOCs进行定性和定量的源解析,并对比了两种模型的结果。结果表明：PMF模型对不同VOCs种类的模拟效果差别较大,而PCA/APCS对不同VOCs种类的模拟效果相近;PMF模型解析的源个数多于PCA/APCS模型,两种模型结果的源性质方面存在很大相似性,但PCA/APCS模型未能区分汽油挥发和汽车尾气源;两种模型源解析出的植物排放源、工业生产源的贡献率较接近,而其他源的贡献率存在差异,PCA/APCS模型解析的溶剂使用源的贡献率高于PMF模型结果,PMF模型解析出的汽油挥发+汽车尾气源的贡献率高于PCA/APCS模型结果。  相似文献   

8.
为了解2021年南京市新冠疫情期间城市大气污染物浓度的变化和成因,利用南京大学SORPES站点2021年7月1日—2021年8月30日大气污染物在线监测数据,分析疫情前、中、后颗粒物及气态污染物的浓度变化,针对臭氧(O3)的关键前体物,挥发性有机物(Volatile Organic Compounds,VOCs)采用正定矩阵因子分解法模型(Positive Matrix Factorization,PMF)、拉格朗日粒子输送与扩散模型(Lagrangian Particle Distribution Model,LPDM)分析其污染来源。结果表明:疫情封闭期间,南京市PM2.5质量浓度较疫情前降低了40％～50％,组分中硝酸盐、有机物质量浓度降幅最为显著,分别下降了34.0％和16.5％。臭氧体积浓度不降反升,城中区域增幅最显著站点可达50％左右。其气态前体物氮氧化物(NOx)及VOCs浓度变化呈相反态势,分别较疫情前降低28％、升高49.6％。模型及卫星遥感结果表明,疫情期间南京市臭氧属于协同偏VOCs控制区。气团溯源结果显示,南京市受本地及周边区域传输的共同影响,疫情封闭期间省外上海方向、省内苏州-无锡-镇江-南通方向的气团贡献增大。PMF解析了南京市本地VOCs主要来源于机动车排放源、植物源、溶剂源、工业生产源以及油气挥发源,其中机动车源占比变幅最大,疫情封闭期间下降了15.1％,疫情后上升了4.3％。其次为油气挥发源、溶剂源,这两项污染源疫情封闭期间分别上升了11.2％、1.7％,疫情后则分别下降了4.8％、4.3％。  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.
As Volatile Organic Compounds(VOCs) are one of the precursors of ozone, their distribution and variable concentrations are highly related to local ozone pollution control. In this study, we obtained vertical profiles of VOCs in Shanghai's Jinshan district on 8 September and 9 September in 2016 to investigate their distribution and impact on local atmospheric oxidation in the near surface layer. Vertical samples were collected from heights between 50 m and 400 m by summa canisters using an unmanned aerial vehicle(UAV). Concentrations of VOCs(VOCs refers to the 52 species measured in this study) varied minimally below 200 m, and decreased by 21.2% from 100 m to 400 m. The concentrations of VOCs above 200 m decreased significantly in comparison to those below 200 m. The proportions of alkanes and aromatics increased from 55.2% and 30.5% to 57.3% and 33.0%, respectively. Additionally, the proportion of alkenes decreased from 13.2% to 8.4%. Toluene and m/p-xylene were the key species in the formation of SOA and ozone. Principal component analysis(PCA) revealed that the VOCs measured in this study mainly originated from industrial emissions.  相似文献   

12.
The vertical observation of volatile organic compounds(VOCs) is an important means to clarify the mechanisms of ozone formation. To explore the vertical evolution of VOCs in summer, a field campaign using a tethered balloon during summer photochemical pollution was conducted in Shijiazhuang from 8 June to 3 July 2019. A total of 192 samples were collected, 23 vertical profiles were obtained, and the concentrations of 87 VOCs were measured. The range of the total VOC concentration was 41–48 ppbv below 600 m. It then slightly increased above 600 m, and rose to 58 ± 52 ppbv at 1000 m.The proportion of alkanes increased with height, while the proportions of alkenes, halohydrocarbons and acetylene decreased. The proportion of aromatics remained almost unchanged. A comparison with the results of a winter field campaign during 8–16 January 2019 showed that the concentrations of all VOCs in winter except for halohydrocarbons were more than twice those in summer. Alkanes accounted for the same proportion in winter and summer. Alkenes,aromatics, and acetylene accounted for higher proportions in winter, while halohydrocarbons accounted for a higher proportion in summer. There were five VOC sources in the vertical direction. The proportions of gasoline vehicular emissions + industrial sources and coal burning were higher in winter. The proportions of biogenic sources + long-range transport, solvent usage, and diesel vehicular emissions were higher in summer. From the surface to 1000 m, the proportion of gasoline vehicular emissions + industrial sources gradually increased.  相似文献   

13.
As the key precursors of O_3, anthropogenic non-methane volatile organic compounds(NMVOCs) have been studied intensively. This paper performed a meta-analysis on the spatial and temporal variations of NMVOCs, their roles in photochemical reactions, and their sources in China, based on published research. The results showed that both nonmethane hydrocarbons(NMHCs) and oxygenated VOCs(OVOCs) in China have higher mixing ratios in the eastern developed cities compared to those in the central and western areas. Alkanes are the most abundant NMHCs species in all reported sites while formaldehyde is the most abundant among the OVOCs. OVOCs have the highest mixing ratios in summer and the lowest in winter, which is opposite to NMHCs. Among all NMVOCs, the top eight species account for 50%-70% of the total ozone formation potential(OFP) with different compositions and contributions in different areas. In devolved regions, OFP-NMHCs are the highest in winter while OFP-OVOCs are the highest in summer. Based on positive matrix factorization(PMF) analysis, vehicle exhaust, industrial emissions, and solvent usage in China are the main sources for NMHCs. However, the emission trend analysis showed that solvent usage and industrial emissions will exceed vehicle exhaust and become the two major sources of NMVOCs in near future. Based on the meta-analysis conducted in this work,we believe that the spatio-temporal variations and oxidation mechanisms of atmospheric OVOCs, as well as generating a higher spatial resolution of emission inventories of NMVOCs represent an area for future studies on NMVOCs in China.  相似文献   

14.
Emissions of hexanal, heptanal, octanal, nonanal, and decanal from 6 different plant species were measured in continuously stirred tank reactors when the plants were exposed to ozone. Pathogen- and insect attack on plants also led to these emissions. The emission rates of individual aldehydes were related to each other implying a common mechanism for the emissions of these aldehydes. Furthermore, the emission pattern was similar in all cases indicating a similar emission mechanism for different plant species and different elicitors. Measurements with ozone exposed Scots pine plants (Pinus sylvestris L.) showed that the emission rates were dependent on temperature as well as on the ozone flux into the plants. The diurnal variation of aldehyde emissions from ozone exposed Scots pine were described quite well using a formalism including temperature and ozone flux as variables. Assuming the aldehyde emissions to be general for plants exposed to ozone, the global emissions were estimated to be in the range between 7 and 22 Tg/a. Because these emissions can be induced by other factors than ozone uptake alone this estimate may be a lower limit.Now atNow at  相似文献   

15.
This overview compiles the actual knowledge of the biogenic emissions of some volatile organic compounds (VOCs), i.e., isoprene, terpenes, alkanes, alkenes, alcohols, esters, carbonyls, and acids. We discuss VOC biosynthesis, emission inventories, relations between emission and plant physiology as well as temperature and radiation, and ecophysiological functions. For isoprene and monoterpenes, an extended summary of standard emission factors, with data related to the plant genus and species, is included. The data compilation shows that we have quite a substantial knowledge of the emission of isoprene and monoterpenes, including emission rates, emission regulation, and biosynthesis. The situation is worse in the case of numerous other compounds (other VOCs or OVOCs) being emitted by the biosphere. This is reflected in the insufficient knowledge of emission rates and biological functions. Except for the terpenoids, only a limited number of studies of OVOCs are available; data are summarized for alkanes, alkenes, carbonyls, alcohols, acids, and esters. In addition to closing these gaps of knowledge, one of the major objectives for future VOC research is improving our knowledge of the fate of organic carbon in the atmosphere, ending up in oxidation products and/or as aerosol particles.  相似文献   

16.
北京奥运会期间CBM-Z化学机制的模拟应用   总被引：1，自引：0，他引：1  
利用CBM-Z化学机制模拟了中国科学院大气物理研究所气象塔站在北京奥运会期间高臭氧时段O3浓度的日变化,评估了气象条件、北京奥运会加强控制措施以及O3前体物浓度对近地面O3生成的影响。结果表明:(1)CBM-Z化学机制较好地模拟了北京奥运会期间典型时段气象塔站O3、NO、NO2日变化特征。(2)有利于局地高臭氧事件发生的气象条件非常相似;北京奥运会加强控制措施的实施显著减少了NOx及VOCs的排放量,导致近地面O3浓度的明显下降。(3)奥运会期间VOCs和CO是影响气象塔站O3生成量的关键因素。  相似文献   

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