大气颗粒物中无机元素特性的研究

介绍用ICP-MS方法分析大气颗粒物中的无机元素,研究了部分污染元素在不同粒径颗粒物中的富集特征以及不同季节的浓度变化,并采用富集因子法对颗粒物的来源进行初步探讨。     

上海不同强度干霾期间气溶胶垂直分布特征

利用美国宇航局(NASA)的CALIPSO星载激光雷达资料,通过分析后向散射系数、体积退偏比和色比等参量揭示了上海地区发生不同强度干霾时气溶胶的垂直分布特征,并结合地面气溶胶观测进行了分析.结果表明,发生干霾时,低层大气(2km以下)污染最严重,气溶胶的后向散射系数主要集中在0.0015~0.0035km-1×sr-1,体积退偏比集中在0~15%,色比集中在0.2~0.8;2~10km高度内,散射系数相对较小,其中2~8km的值主要集中在0.0008~0.0025 km-1×sr-1,8~10km的值则主要集中0.0008~0.0015 km-1×sr-1,气溶胶体积退偏比和色比在2~4km、4~6km、6~8km和8~10km各高度内分别集中在0~20%和0~0.6.在0~10km高度内,相对于轻微干霾和轻度干霾,中度干霾时气溶胶的散射能力和不规则性最强,粒径也最大.     

兰州市化石燃料燃烧源排放VOCs的臭氧及二次有机气溶胶生成潜势

随着我国工业的快速发展和城市化进程的加快,化石燃料的大量使用造成了严重的二氧化硫、颗粒物和挥发性有机物(volatile organic compounds,VOCs)等大气污染.目前,对化石燃料燃烧排放挥发性有机物环境影响的研究较少,本文计算了兰州市化石燃料燃烧源排放VOCs及其相应的臭氧生成潜势(ozone formation potential,OFP)和二次有机气溶胶生成潜势(secondary organic aerosols formation potential,SOAFP),其中水泥制造业的OFP和SOAFP占比最大,分别为45. 3%、50. 9%;其次为砖瓦制造业,但其吨标煤燃烧排放VOCs的OFP和SOAFP值最高,折为吨标煤后天然气燃烧产生VOCs的O_3和SOA最小.兰州市主城区化石燃料燃烧源OFP和SOAFP主要为电力和热力的生产供应以及西固区工业企业排放VOCs的贡献,其它地区为水泥制造业、砖瓦制造业、钢铁冶炼业等高能耗的行业的贡献为主.芳香烃是化石燃料燃烧源排放VOCs中对OFP和SOAFP均贡献最大的一类物质,占比分别为40. 0%和67. 2%,并且在生成潜势贡献前10的物种中芳香烃为主要物种.与生物质燃烧源相比,化石燃料燃烧源具有较强的O_3和SOA生成能力(2. 58 t·t~(-1)和3. 16 kg·t~(-1)).     

铵盐气溶胶对烟气排放连续监测系统颗粒物比对监测的影响研究

利用拉曼光谱对采样后的滤筒进行分析,发现废气中的硫酸铵-硫酸氢铵气溶胶是造成成都市部分企业烟气排放连续监测系统(CEMS)颗粒物比对监测结果不合格的主要原因。通过比较分析得出:在对含硫酸铵-硫酸氢铵气溶胶废气进行颗粒物浓度比对监测时,参比方法(重量法)测定的颗粒物浓度是一定标干采样体积下废气中固体微粒和硫酸铵-硫酸氢铵液体微粒结晶后产生的晶体的总质量,基于光散射法的CEMS颗粒物浓度测试系统测定的颗粒物浓度只是一定标干采样体积下废气中固体微粒的质量,由此导致参比方法测出的颗粒物浓度远大于CEMS测出的浓度,造成比对误差远超出允许值范围。     

2006年秋冬两季图们市大气气溶胶中多环芳烃分布规律

大气气溶胶是目前大多数城市的首要污染物,其中的多环芳烃是对人体健康危害最大的环境污染物之一。通过图们市2006年9月、12月4个采样点的大气气溶胶样品分析,研究了大气气溶胶中多环芳烃的分布规律。采用超声波萃取法提取样品中的多环芳烃,然后对其进行旋蒸浓缩,氮气吹至1ml,用高效液相色谱进行定性和定量分析。实验结果表明,美国EPA优先控制的16种多环芳烃普遍存在于图们市区的大气气溶胶中。图们市不同时空大气气溶胶中多环芳烃的分布具有一定的规律性。     

珠江三角洲气溶胶中正构烷烃分布规律、来源及其时空变化

珠江三角洲地区主要城市气溶胶中正构烷烃分布可分为３种类型，第一类为前峰型，主要来源于汽车尾气；第二类为后峰型，主要来源于植物蜡；第三类为双峰型，来源于植物蜡，燃料燃烧和尾气。     

Reconstructed mass-spectrometric pattern for characterization of carbon compounds in smoker's lung in situ

BACKGROUND: Cigarette smoke is a major anthropogenic pollutant and contributes to the permanent load of ambient particulate matter in the air, particularly indoors. It is the leading risk factor for premature loss of life due to chronic bronchitis, emphysema and lung cancer. Smoker's lung and graphite pneumoconiosis are pathological states characterized by the deposition of carbonaceous particles. METHODS: Mass spectrometry was used to evaluate unstained lung sections obtained in vivo from a heavy smoker and a patient with occupationally acquired graphite pneumoconiosis. RESULTS AND DISCUSSION: The composition of carbon compounds deposited in lung tissue samples is demonstrated here for the first time. Thirty carbonaceous-containing microareas from ten biopsies (three areas per biopsy) of lung tissues were analyzed mass-spectrometrically. In each case, the samples were taken from a smoker's lung or those demonstrating a graphite pneumoconiosis. The lung-tissue samples were selected by light microscopy before they were evaporated for mass spectrometry. First-order criteria were anionic and cationic mass peaks which occur within the mass patterns in lung tissues of smoker's lung, although not in graphite pneumoconiosis. Second-order criteria were mass peaks from smoker's lung with standard deviations SD < or = 14% of the mean value. First and second-order mass peaks matched the mass peaks of experimental cigarette-smoke condensate in 9 out of 11 peaks. A software program was developed that enabled fast, automated recognition of the typical mass peaks, and thereby confirmed the histological diagnosis of smoker's lung. CONCLUSIONS: The analysis of carbonaceous particles within lung biopsies from a heavy smoker corresponded to the spectra of tobacco condensate and not to the investigated biopsies of graphite peneumoconiosis. RECOMMENDATION AND OUTLOOK: The analyses were performed in order to find out whether mass-spectrometric criteria exist for the differentiation of carbonaceous lung-tissue deposits. Mass spectrometry may be a valuable tool in determining the composition of carbon compounds deposited in human lung tissue. So far, qualitative assessment of the composition of deposits in lung tissue is only possible after the patient is deceased (autopsy).     

Experiments probing the influence of air exchange rates on secondary organic aerosols derived from indoor chemistry

Reactions between ozone and terpenes have been shown to increase the concentrations of submicron particles in indoor settings. The present study was designed to examine the influence of air exchange rates on the concentrations of these secondary organic aerosols as well as on the evolution of their particle size distributions. The experiments were performed in a manipulated office setting containing a constant source of d-limonene and an ozone generator that was remotely turned “on” or “off” at 6 h intervals. The particle number concentrations were monitored using an optical particle counter with eight-channels ranging from 0.1–0.2 to>2.0 μm diameter. The air exchange rates during the experiments were either high (working hours) or low (non-working hours) and ranged from 1.6 to>12 h⁻¹, with intermediate exchange rates. Given the emission rates of ozone and d-limonene used in these studies, at an air exchange rate of 1.6 h⁻¹ particle number concentration in the 0.1–0.2 μm size-range peaked 1.2 h after the ozone generator was switched on. In the ensuing 4.8 h particle counts increased in successive size-ranges up to the 0.5–0.7 μm diameter range. At higher air exchange rates, the resulting concentrations of total particles and particle mass (calculated from particle counts) were smaller, and at exchange rates exceeding 12 h⁻¹, no excess particle formation was detectable with the instrument used in this study. Particle size evolved through accretion and, in some cases, coagulation. There was evidence for coagulation among particles in the smallest size-range at low air exchange rates (high particle concentrations) but no evidence of coagulation was apparent at higher air exchange rates (lower particle concentrations). At higher air exchange rates the particle count or size distributions were shifted towards smaller particle diameters and less time was required to achieve the maximum concentration in each of the size-ranges where discernable particle growth occurred. These results illustrate still another way in which ventilation affects human exposures in indoor settings. However, the ultimate effects of these exposures on health and well being remain to be determined.     

北京地区对流层低层臭氧及硫酸盐气溶胶的时空分布

基于OMI/Aura卫星资料,分析了北京地区2007~2016年近10a对流层O₃浓度（0~3km）、硫酸盐气溶胶光学厚度（0~2km）、SO₂（边界层以内）柱浓度时空演变特征.结果表明,近10a来北京地区O₃浓度总体呈现上升趋势,最低值在2007年,浓度为33.65 μg/m³;硫酸盐气溶胶污染总体变化呈现先下降后增长的趋势,2007年硫酸盐气溶胶污染最为严重,2011年污染最轻,对应的AOD值为0.252,但在2014年以后,硫酸盐气溶胶污染又出现增长趋势;SO₂浓度在2007~2016年总体呈现下降的变化趋势,且下降趋势明显,最高值为2007年,最低值出现在2016年,最低值比最高值降低了60.42%,但在2011年污染出现反弹.北京O₃季节变化明显,夏季高、春秋次之、冬季低;硫酸盐气溶胶污染季节特征与O₃相同;SO₂污染主要集中在冬季,采暖期污染程度高于非采暖期.     

大气气溶胶粒子质量浓度分布规律研究

在可吸入性颗粒物粒径范围内(d_p<10μm),上海市区大气中气溶胶粒子质量浓度分布为双峰型,峰值出现在1.0μm左右(积聚模态粒子区)和4.5μm左右(粗粒子区),且呈现大粒径处峰值大于小粒径处峰值的趋势。与质量浓度分布曲线相似,质量概率密度分布也为双峰型,峰值出现在0.8μm左右和4.0μm左右。模拟结果表明,上海市区大气中气溶胶粒子质量概率密度分布规律符合双重分布函数:y=exp[-(a_4d~4 a_3d~3 a_2d~2 a_1d a_0)],所表征的类型,应用双重分布函数能解释大气气溶胶粒子的分布规律。