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1.
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   

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.
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   

4.
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   

5.
了解涂装行业挥发性有机物(VOCs)的排放特征是制定山东地区臭氧(O3)和PM2.5防控策略的重要环节.本研究在山东地区测定了两家典型食品金属包装企业喷涂过程中VOCs的排放组成,企业产品以饮料罐和罐头为主.结果表明:两家企业排放的总VOCs质量浓度水平相当,质量浓度变化范围在50~1 500 μg/m3;但两家企业喷涂过程中VOCs的排放组成具有一定的差异,以生产铝罐和马口铁罐为主的企业中的含氧挥发性有机物(OVOCs)含量最多,占比89.71%(质量分数,下同);而生产铝罐的企业芳香烃(56.15%)是首要的排放种类,其次是OVOCs (32.32%).通过分析两家企业内外喷涂工艺的VOCs源成分谱,发现同一企业不同工艺之间有一定差异,多种罐生产企业的内、外喷涂中乙醇占比最高,分别为94.28%、84.46%;单铝罐生产企业的内喷涂2-丁酮(24.33%)是重要组分,外喷涂中甲苯(36.40%)含量较高.  相似文献   

6.
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   

7.
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   

8.
本文利用气体组分及大气气溶胶在线监测系统(MARGA ADI 2080)观测武汉市2018年1月9—26日大气气溶胶中的8种水溶性离子(NH+4、NO-3、SO2-4、Cl-、K+、Ca2+、Na+和Mg2+),结合气象要素数据,使用主成分分析(PCA)、正定矩阵因子分析法(PMF)、HYSPLIT后向轨迹模式、潜在源区贡献(PSCF)和浓度权重轨迹(CWT),对霾污染过程中水溶性离子进行了全面的来源解析,探究了霾不同阶段下来源差异和空间分布特征。结果表明:(1)本次霾污染中的8种水溶性离子和4种污染气体,PCA解析出的源和占比分别为二次源和燃煤源的混合源(41.28%)、工业排放和土壤扬尘混合源(27.73%)和机动车排放源(9.63%),PMF解析出的源和占比分别为燃煤与土壤扬尘混合源(18.57%)、机动车排放源(20.74%)、二次源(18.30%)、光化学污染源(22.24%)和燃煤源(20.15%)。(2)霾在不同阶段下水溶性离子和4种污染气体的来源存在差异,在清洁天和霾消散阶段,光化学的贡献最高,占比分别为31.42%和36.07%;在霾发生阶段燃煤与土壤扬尘源的贡献最高,其贡献为40.94%;在霾发展阶段,最大的控制源为二次源,贡献占比为37.51%。(3)此次武汉市霾污染中PM2.5浓度和NH+4、NO-3和SO2-4的潜在源区为皖豫鄂三省和赣湘鄂三省交界处。霾污染中PM2.5的主要影响范围是武汉市南部和北部省份,NO-3、NH+4和SO2-4的主要影响区域为武汉市东北方向的城市、湖南省和江西省。  相似文献   

9.
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   

10.
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   

11.
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   

12.
Satellite measurements of tropospheric column O3 and NO2 in eastern and southeastern Asia are analyzed to study the spatial and seasonal characteristics of pollution in these regions. Tropospheric column O3 is derived from differential measurements of total column ozone from Total Ozone Mapping Spectrometer (TOMS), and stratospheric column ozone from the Microwave Limb Sounder (MLS) instrument on the Upper Atmosphere Research Satellite (UARS). The tropospheric column NO2 is measured by Global Ozone Monitoring Experiment (GOME). A global chemical and transport model (Model of Ozone and Related Chemical Tracers, version 2; MOZART-2) is applied to analyze and interpret the satellite measurements. The study, which is based on spring, summer, and fall months of 1997 shows generally good agreement between the model and satellite data with respect to seasonal and spatial characteristics of O3 and NO2 fields. The analysis of the model results show that the industrial emission of NOx (NO + NO2) contributes about 50%–80% to tropospheric column NO2 in eastern Asia and about 20%–50% in southeastern Asia. The contribution of industrial emission of NOx to tropospheric column O3 ranges from 10% to 30% in eastern Asia. Biomass burning and lightning NOx emissions have a small effect on tropospheric O3 in central and eastern Asia, but they have a significant impact in southeastern Asia. The varying effects of NOx on tropospheric column ozone are attributed to differences in relative abundance of volatile organic compounds (VOCs) with respect to total nitrogen in the two regions.  相似文献   

13.
大气污染严重威胁了我国陆地生态系统的固碳能力,但随着减污降碳协同治理的快速推进,减缓大气污染将有利于提升陆地碳汇,并切实推动碳达峰碳中和目标的实现。为了更好地理解大气污染与生态系统固碳的关系,本文以主要空气污染物臭氧(O3)为例,基于田间控制实验的整合分析、剂量响应关系及机理模型三种评估方法综述了近地层O3污染对植被碳固定影响的最新进展。尽管不同作物种类以及品种、不同功能型木本植物对O3的响应有着显著的差异,且各种方法的评估结果也不尽相同,但目前O3浓度造成我国粮食作物减产、森林生产力降低已是不争的事实。持续升高的O3浓度将严重威胁我国陆地生态系统的固碳能力。利用我国作物和树木的O3剂量响应方程进行评估的结果表明,在CO2减排和O3污染协同治理下,预计2060年我国树木生物量和作物产量将比当前显著提高,增加陆地生态系统碳汇,助力碳中和目标。最后,对如何提高O3污染环境下植物固碳能力也进行了展望。  相似文献   

14.
Summer and winter campaigns for the chemical compositions and sources of nonmethane hydrocarbons(NMHCs)and oxygenated volatile organic compounds(OVOCs)were conducted in Xi’an.Data from 57 photochemical assessment monitoring stations for NMHCs and 20 OVOC species were analyzed.Significant seasonal differences were noted for total VOC(TVOC,NMHCs and OVOCs)concentrations and compositions.The campaign-average TVOC concentrations in winter(85.3±60.6 ppbv)were almost twice those in summer(47.2±31.6 ppbv).Alkanes and OVOCs were the most abundant category in winter and summer,respectively.NMHCs,but not OVOCs,had significantly higher levels on weekends than on weekdays.Total ozone formation potential was higher in summer than in winter(by 50%)because of the high concentrations of alkenes(particularly isoprene),high temperature,and high solar radiation levels in summer.The Hybrid Environmental Receptor Model(HERM)was used to conduct source apportionment for atmospheric TVOCs in winter and summer,with excellent accuracy.HERM demonstrated its suitability in a situation where only partial source profile data were available.The HERM results indicated significantly different seasonal source contributions to TVOCs in Xi’an.In particular,coal and biomass burning had contributions greater than half in winter(53.4%),whereas traffic sources were prevalent in summer(53.1%).This study’s results highlight the need for targeted and adjustable VOC control measures that account for seasonal differences in Xi’an;such measures should target not only the severe problem with VOC pollution but also the problem of consequent secondary pollution(e.g.,from ozone and secondary organic aerosols).  相似文献   

15.
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   

16.
Tianjin is the third largest megacity and the fastest growth area in China, and consequently faces the problems of surface ozone and haze episodes. This study measures and characterizes volatile organic compounds(VOCs), which are ozone precursors, to identify their possible sources and evaluate their contribution to ozone formation in urban and suburban Tianjin,China during the Ha Chi(Haze in China) summer campaign in 2009. A total of 107 species of ambient VOCs were detected,and the average concentrations of VOCs at urban and suburban sites were 92 and 174 ppbv, respectively. Of those, 51 species of VOCs were extracted to analyze the possible VOC sources using positive matrix factorization. The identified sources of VOCs were significantly related to vehicular activities, which specifically contributed 60% to urban and 42% to suburban VOCs loadings in Tianjin. Industrial emission was the second most prominent source of ambient VOCs in both urban and suburban areas, although the contribution of industry in the suburban area(36%) was much higher than that at the urban area(16%). We conclude that controlling vehicle emissions should be a top priority for VOC reduction, and that fast industrialization and urbanization causes air pollution to be more complex due to the combined emission of VOCs from industry and daily life, especially in suburban areas.  相似文献   

17.
Abstract

The dependence of ozone formation on the mixing ratios of volatile organic compounds (VOCs) and nitrogen oxides (NOx) has been widely studied. In addition to the atmospheric levels of VOCs and NOx, the extent of photochemical processing of VOCs has a strong impact on ozone levels. Although methods for measuring atmospheric mixing ratios of VOCs and NOx are well established and results of those measurements are widely available, determination of the extent of photochemical processing of VOCs, known as photochemical age (PCA), is difficult. In this article a recently developed methodology for the determination of PCA for individual compounds based on the change in their stable carbon isotope composition is used to investigate the dependence between ozone and VOC or NOx mixing ratios at a rural site in Ontario, Canada, during fall and winter. The results show that under these conditions the variability in VOC mixing ratios is predominantly a result of the varying impact of local emissions and not a result of changes in the extent of atmospheric processing. This explains why the mixing ratio of ozone shows no systematic dependence on the mixing ratios of VOCs or NOx in this environment and at this time of the year.  相似文献   

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