Particle number concentration, size distribution and chemical composition during haze and photochemical smog episodes in Shanghai

The aerosol number concentration and size distribution as well as size-resolved particle chemical composition were measured during haze and photochemical smog episodes in Shanghai in 2009. The number of haze days accounted for 43%, of which 30% was severe （visibility 〈 2 km） and moderate （2 km 〈 visibility 〈 3 km） haze, mainly distributed in winter and spring. The mean particle number concentration was about 17,000/cm3 in haze, more than 2 times that in clean days. The greatest increase of particle number concentration was in 0.5-1μm and 1-10 μm size fractions during haze events, about 17.78 times and 8.78 times those of clean days. The largest increase of particle number concentration was within 50-100 nm and 100-200 nm fractions during photochemical smog episodes, about 5.89 times and 4.29 times those of clean days. The particle volume concentration and surface concentration in haze, photochemical smog and clean days were 102, 49, 15 μm3/cm3 and 949, 649, 206 μm2/cm3, respectively. As haze events got more severe, the number concentration of particles smaller than 50 nm decreased, but the particles of 50-200 nm and 0.5-1μm increased. The diurnal variation of particle number concentration showed a bimodal pattern in haze days. All soluble ions were increased during haze events, of which NH4, SO24- and NO3 increased great/y, followed by Na＋, IC, Ca2＋ and CI-. These ions were very different in size-resolved particles during haze and photochemical smog episodes.     

基于大数据分析的雾霾污染预测研究

对雾霾的监控预测已成为城市重点监测指标,传统雾霾监测方法使用的是高斯预测模型,在预测过程中会使用大量的参数以及逻辑关系,在大数据分析的趋势下已经不能承接海量相关大数据,针对上述问题,提出一种基于大数据分析的雾霾污染预测方法.建立数据K模型承接海量数据,对大数据特点趋势加以分析,使用组合算子对雾霾污染度预测,摒弃逻辑关系束缚以及大数据的驱使性,对特征数据进行类别掌控完成预测结果.通过对比实验的方式对提出的方法进行检验,实验结果表明:(1)基于大数据分析的雾霾污染预测方法能够在大数据环境下对雾霾污染度进行高精度预测;(2)与传统方法相比较能够承接大数据的变化;(3)摒弃逻辑关系的制约可以实现随时预测;(4)极大的缩减预测成本.     

SO2-NO2-NH3-H2O四元反应体系中气溶胶的生成特性

通过烟雾箱实验,研究了SO₂-NO₂-NH₃-H₂O四元反应体系在气-粒转化过程中新形成颗粒物数浓度与粒径分布的变化.研究发现,SO₂-NO₂-NH₃-H₂O四元反应体系具有显著的成核能力,且其成核强度大,持续时间短.当SO₂、NO₂浓度为200mg/m³,NH₃浓度为12x10^-6时,反应体系的气溶胶总个数浓度在2min时达到峰值2.5x10⁶cm^-3.缺少任一种气体均会使气溶胶成核强度下降.SO₂、NO₂及NH₃浓度分别为0的工况下气溶胶总个数浓度峰值分别下降了41.0%、83.6%及98.5%.在电厂污染气体排放浓度区间内,NO₂对气溶胶生成影响大于SO₂.燃煤电厂控制NO_x排放浓度对改善烟囱出口气溶胶数浓度更有效.在实验基础上,对颗粒物成核特性进行拟合,反应体系在气-粒转化过程中产生的新颗粒物总个数浓度及中值粒径与气态前体物浓度线性相关;采用布朗团聚模型对气溶胶成核后的团聚过程总个数浓度及粒径变化进行模拟计算,根据给定的燃煤电厂SO₂、NO₂、NH₃排放浓度,给出预测气溶胶颗粒成核速率、粒径分布及总个数浓度变化的方法.     

Eperimental study of photooxidation products of ethylbenzene

Smog chamber experiments were performed to investigate the composition of products formed from photooxidation of aromatic hydrocarbon ethylbenzene.Vacuum ultraviolet photoionization mass spectrometer and aerosol time-of-flight mass spectrometer were used to measure the products in the gas and particle phases in real-time.Experimental results demonstrated that ethylphenol,methylglyoxal,phenol,benzaldehyde,and 2-ethylfurane were the predominant photooxidation products in both the gas and particle phases.However,there were some differences between detected gas phase products and those of particle phase,for example,2-ethylfurane,ethylglyoxylie acid,nitroethylbenzene,3,4-dioxopentanal and ethyl-nitrophenol were only existing in the particle-phase.The possible reaction mechanisms leading to these products were also discussed and proposed.     

Chemical composition and size distribution of secondary organic aerosol formed from the photooxidation of isoprene

Photooxidation of isoprene leads to the formation of secondary organic aerosol (SOA). In this study, the chemical composition of SOA formed from OH-initiated photooxidation of isoprene has been investigated with gas chromatography/mass spectrometry (GC/MS) and a home-made aerosol time-of-flight mass spectrometer. Sampling particles generated in a home-made smog chamber. The size distribution of SOA particles was detected by a TSI 3321 aerodynamic particle size spectrometer in real time. Results showed that SOA created by isoprene photooxidation was predominantly in the form of fine particles, which have diameters less than 2.5 m. The obtained mass spectra of individual particles show that products of the OH-initiated oxidation of isoprene contain methyl vinyl ketone, methacrolein, formaldehyde, and some other hydroxycarbonyls. The possible reaction mechanisms leading to these products were also discussed.     

硫酸铵气溶胶对甲苯-NOx-空气体系光化学反应的影响

利用大气模拟烟雾箱,研究了硫酸铵气溶胶对甲苯-NO_x-空气体系光化学反应的影响.结果表明,硫酸铵作为气溶胶种子,其存在可以加快反应过程中颗粒物（particle matter, PM）的生成速度,并提高甲苯的气溶胶产率.在高浓度的硫酸铵气溶胶种子条件下,其初始浓度对反应过程中NO_x、NO和O₃的浓度变化没有明显的影响,但对二次有机气溶胶（secondary organic aerosol, SOA）的生成有显著影响.在硫酸铵气溶胶种子浓度小于160 μg·m^-3时,SOA的产率随初始气溶胶种子浓度的增大而增大,从最小7.2％到最大11.7％,其增幅超过60％.     

京津冀PM2.5浓度控制目标可达性分析

雾霾污染已成为京津冀地区最突出的环境问题,国务院颁布了《大气污染防治行动计划》,明确提出了京津冀地区雾霾治理的浓度目标和减排措施。但是这些减排措施能否够实现PM2.5的浓度目标呢?本文基于数据分析方法,量化了2013—2014年京津冀地区PM2.5浓度与污染物排放量的关系,预测了现有减排措施可以达到的PM2.5浓度以及实现既定的PM2.5浓度目标的大气污染物减排要求,对"大气十条"减排政策的有效性进行了科学评估。结果显示,现有的减排措施难以实现PM2.5浓度控制目标,天津和河北的大多数地市需要进一步加大污染物减排力度。河北的部分地市即使实现了PM2.5浓度下降25%的目标,PM2.5浓度仍然过高,应改下降百分比为绝对值目标。北京的污染物减排率过高,减排难度较大,可以考虑一个现实合理的PM2.5浓度目标和污染物减排计划。由于污染物减排行动涉及区域经济和民生保障,PM2.5浓度受到风力等自然因素的影响较大,京津冀地区的雾霾治理应确定现实可行的浓度控制目标,并制定相应的污染物排放量管理目标。     

Smog chamber study on the evolution of fume from residential coal combustion

Domestic coal stoves are widely used in countryside and greenbelt residents in China for heating and cooking, and emit considerable pollutants to the atmosphere because of no treatment of their exhaust, which can result in deteriorating local air quality. In this study, a dynamic smog chamber was used to investigate the real-time emissions of gaseous and particulate pollutants during the combustion process and a static smog chamber was used to investigate the fume evolution under simulate light irradiation. The real-time emissions revealed that the total hydrocarbon (THC) and CO increased sharply after ignition, and then quickly decreased, indicating volatilization of hydrocarbons with low molecular weight and incomplete combustion at the beginning stage of combustion made great contribution to these pollutants. There was evident shoulder peak around 10 min combustion for both THC and CO, revealing the emissions from vitrinite combustion. Additionally, another broad emission peak of CO after 30 min was also observed, which was ascribed to the incomplete combustion of the inertinite. Compared with THC and CO, there was only one emission peak for NOx, SO₂ and particular matters at the beginning stage of combustion. The fume evolution with static chamber simulation indicated that evident consumption of SO₂ and NOx as well as new particle formation were observed. The consumption rates for SO₂ and NOx were about 3.44% hr^-1 and 3.68% hr^-1, the new particle formation of nuclei particles grew at a rate of 16.03 nm/hr during the first reaction hour, and the increase of the diameter of accumulation mode particles was evident. The addition of isoprene to the diluted mixture of the fume could promote O₃ and secondary particle formation.     

浅析光化学烟雾的污染问题

光化学烟雾频繁发生的罪魁祸首是工业废气和机动车尾气污染。本文在简要分析了光化学烟雾的形成机理、生成条件及对生物体的危害后,提出从控制污染源着手来预防光化学烟雾频发的对策。     

香港大气能见度与污染物长期变化的特征和相互关系

利用香港天文台40年(1968~2007年)的能见度数据,中西区空气监测站24年(1984~2007年)的空气质量数据,采用多元回归法,分析了香港地区大气环境状况与大气污染物变化的关系.结果表明,香港地区1968~2007年间低能见度时数百分比平均每10年上升3.1%,其中,其上升趋势在1968~1989年较为平缓(平均0.7%/10a),20世纪90年代后(1990~2007年)则较为明显(平均7.3%/10a),且与地面臭氧浓度呈同步上升趋势.1993年前,低能见度时数百分比与NO2和NOx相关性显著,1993年后,与其相关性显著的污染物则是O3、SO2和NO2.这说明香港地区能见度的恶化在1993年前与光化学烟雾有关,但在1993年后则同时受光化学烟雾和与硫酸盐粒子有关的气溶胶烟雾的共同影响.