有机气溶胶的来源与形成研究现状

介绍了有机气溶胶来源与形成的研究现状,从有机气溶胶的化学组成特征、一次有机气溶胶的来源和二次有机气溶胶的形成机制论述其研究进展.一次有机气溶胶主要来源于烹调油烟、机动车排放、生物质燃烧、工业或民用燃油锅炉释放出的有机物,还有道路扬尘、沥青、刹车尘、轮胎屑、室外香烟烟雾、以及高等植物蜡、细菌活动和草本植物等.大气中的半挥发性有机物可通过物理和化学吸附形成二次有机气溶胶,一些挥发性有机物可通过气相化学反应转化为低挥发性的物质并形成二次有机气溶胶,其主要前体物是芳香族化合物,如苯、甲苯、二甲苯,以及烯烃、烷烃、环烷烃、萜烯和生物排放的非饱和氧化物.     

北京市PM2.5水溶性有机物污染特征

用离子色谱技术对北京市2001~2002年大气PM2.5中7种水溶性有机物(WSOC)(甲酸、乙酸、甲磺酸、乙二酸、丙二酸、丁二酸、戊二酸)及12种无机离子(F-、Cl-、NO2-、NO3-、SO32-、SO42-、PO43-、Na 、NH4 、K 、Mg2 、Ca2 )的污染水平进行了同步测定.结果表明,SO42-、NO3-及NH4 为PM2.5中主要的水溶性物种,分别占PM2.5质量的10.6%、7.4%和5.7%;7种WSOC的浓度为0.011~0.118靏/m3,占PM2.5质量浓度的0.01%~0.1%,其中浓度最高的为乙二酸,其次为乙酸、丙二酸、丁二酸等;对PM2.5各化学组分浓度的季节变化特征的分析表明,PM2.5及OC的高浓度污染均出现在冬季采暖期,而WSOC则出现在夏季;对乙二酸与其他各组分进行相关性分析表明,乙二酸与SO42-、K 、NH4 、NO3-有较强的线性相关性(r=0.83,0.57,0.49,0.33),而与Cl-、Na 、Mg2 、Ca2 、EC、OC相关性较差(r=0.24, 0.22,0.12,0.05,0.13,0.10).由乙二酸季节变化特征及与其他物种相关性等特征初步推断,北京市PM2.5二元羧酸的主要来源为光化学反应而形成的二次污染物,而非来源于机动车、海盐或土壤的一次排放.     

Characteristics of Carbonaceous Aerosol at Taichung Harbor, Taiwan during Summer and Autumn Period of 2005

In recent years, suspended particle pollution has become a serious problem in Taiwan. The carbonaceous materials EC and OC are play important roles in various atmospheric processes. The primary OC/EC ratio approach is applied to assess the contribution of secondary organic aerosol (SOA) to the PM_2.5 and PM₁₀ mass at the Taichung harbor sampling site. The results indicated that the average EC and OC concentration were 1.06 and 6.50 μg m⁻³, respectively, in fine particulate. And the average EC and OC concentration were 4.04 and 40.32 μg m⁻³, respectively, in coarse particulate at Taichung Harbor sampling site. In addition, and the average EC/OC rations was 8.72 in fine particle, respectively, at Taichung Harbor, Taiwan during summer and autumn period of 2005. The fine particle exhibited high particulate concentrations in October, and lower concentration particulate occurred in August. And in this study OC and EC concentrations in this study are compared with those in other cities. The results of EC and OC concentration in this study are also compare with those other cities.     

Monitoring of Seasonal Vegetables for Pesticide Residues

Market samples (60) of six seasonal vegetables were monitoredduring 1996–1997 to determine the magnitude of pesticidalcontamination. The estimation of insecticide residuesrepresenting four major chemical groups i.e. organochlorine,organophosphorous, synthetic pyrethroid and carbamate, was doneby adopting a multiresidue analytical technique employingGC-ECD and GC-NPD systems with capillary columns. The testedsamples showed 100% contamination with low but measurableamounts of residues. Among the four chemical groups, theorganophosphates were dominant followed by organochlorines,synthetic pyrethroids and carbamates. About 23% of the samplesshowed contamination with organophosphorous compounds abovetheir respective MRL values. More extensive studies coveringdifferent regions of Haryana state are suggested to get a clearidea of the magnitude of vegetable contamination with pesticideresidues.     

树叶烟尘中的有机碳和元素碳

为了探讨不同燃烧条件下树叶烟尘中有机碳(OC)、元素碳(EC)及8种碳组分(OC1~OC4、POC、EC1~EC3)的质量分数及分布,利用自制的燃烧采样装置,对10种绿叶进行了阴、明燃两种条件的燃烧,并用热/光碳分析仪对产生的烟尘进行了测定.结果表明,10种绿叶阴燃烟尘中的OC、EC质量分数均值分别为48.9%和4.5%,焦炭char-EC(定义为EC1-POC)的质量分数均值为4.4%.该条件下绿叶燃烧的烟尘(PM)、OC及EC的排放因子均值分别为102.4、50.0和4.7 g·kg-1,烟尘中OC/EC、OC1/OC2及焦炭和炭灰的比值char-EC/soot-EC(定义为EC1-POC/EC2+EC3)的均值分别为11.5、1.9和48.1.明燃条件下,10种绿叶烟尘中OC、EC及char-EC的质量分数均值分别为44.9%、10.9%和10.7%,PM、OC及EC的排放因子均值分别为59.2、26.6和6.0 g·kg-1.10种绿叶明燃烟尘中上述三特征比值的均值分别为4.8、1.1和133.0.树叶阴燃烟尘中OC1质量分数及OC1/OC2值均显著高于明燃,而明燃烟尘中的char-EC质量分数及char-EC/soot-EC显著大于阴燃.树叶烟尘中OC、EC的组成在不同树种及燃烧条件间均体现出一些差异,同时也明显区别于其他生物质烟尘.     

长三角典型站点冬季大气PM2.5中OC、EC污染特征

对2015年1月9日~2015年1月31日临安、南京和苏州3个站点采集的PM_(2.5)样品(共计279组),使用热光反射法(thermal/optical reflectance,TOR)分析了样品中有机碳(OC)与元素碳(EC)的含量,并研究了长三角地区冬季PM_(2.5)中OC和EC的污染特征.结果表明,采样期间临安、南京和苏州的PM_(2.5)平均质量浓度分别为(123.56±61.11)、(144.77±62.91)和(156.5±68.97)μg·m-3,均超过我国《环境空气质量标准》(GB 3095-2012)规定的PM_(2.5)日均值75μg·m-3;其中3个站点OC与EC的平均质量浓度依次分别为(21.93±11.69)/(6±3.6)、(20.32±10.3)/(5.39±3.07)和(27.08±14.35)/(6.4±4.29)μg·m-3.临安作为长三角大气环境背景点,OC与EC的污染也较为严重.3个站点OC与EC的相关性为临安(R2=0.83)、南京(R2=0.72)和苏州(R2=0.72),表明冬季长三角地区的碳质气溶胶的来源较为一致和稳定.3个站点样品中的OC/EC值均大于2.0,样品的OC/EC值主要分布在2.5~6.0这个区间内,表明燃煤源和机动车尾气排放源是OC与EC的主要来源.使用EC示踪法估算临安、南京和苏州3个站点的二次有机碳(SOC)平均质量浓度分别为(9.23±5.26)、(6.82±4.36)和(12.56±7.52)μg·m-3,在OC中占比为42%、34%和46%,表明SOC是OC的重要组成部分.后向轨迹显示,PM_(2.5)、OC和EC的质量浓度与主要气团的传输路径有较好的相关性,自空气质量较差区域气团的PM_(2.5)、OC和EC的质量浓度是来自空气质量较好区域的1.14~1.7倍、1.55~2.1倍和1.94~2.47倍.     

Carbonaceous species in fine particles at the background sites in Korea between 1994 and 1999

Organic carbon (OC) and elemental carbon (EC) in fine particles (PM_2.5) at two background sites, Kosan and Kangwha in Korea were measured during intensive field studies between 1994 and 1999. Fine particles were collected on pre-fired quartz filters in a low-volume sampler and analyzed using the selective thermal oxidation method with MnO₂ catalyst. The OC and EC concentrations at Kosan located at western tip of Cheju Island in southern Korea are lower than those at Kangwha located at western coastal area in mid-Korean peninsula. Still, the OC concentrations at Kosan are generally higher than those at other background areas in Japan and USA. The EC concentrations at Kosan are lower than or comparable to those at other background areas. The total carbon (TC, sum of OC and EC) to EC ratio values at both sites were higher than those at other background areas in Japan and USA. At Kosan, the OC and EC concentrations when air parcels were from southern China were higher than those when air parcels were coming from northern China. However, at Kangwha, the differences were statistically not clear since most air parcels were from northern China. Except when air parcels were from the North Pacific during summer, the OC and EC concentrations are well correlated indicating that both OC and EC share the same emission/transport characteristics. From the gaseous hydrocarbon data and the OC and EC relationship, it was found that during summer local biogenic emissions of OC might be significant at Kosan.     

Effects of a diesel oxidation catalyst on gaseous pollutants and fine particles from an engine operating on diesel and biodiesel

The effects of a diesel oxidation catalytic (DOC) converter on diesel engine emissions were investigated on a diesel bench at various loads for two steady-state speeds using diesel fuel and B20. The DOC was very effective in hydrocarbon (HC) and CO oxidation. Approximately 90%–95% reduction in CO and 36%–70% reduction in HC were realized using the DOC. Special attention was focused on the effects of the DOC on elemental carbon (EC) and organic carbon (OC) fractions in fine particles (PM_2.5) emitted from the diesel engine. The carbonaceous compositions of PM_2.5 were analyzed by the method of thermal/optical reflectance (TOR). The results showed that total carbon (TC), OC and EC emissions for PM_2.5 from diesel fuel were generally reduced by the DOC. For diesel fuel, TC emissions decreased 22%–32% after the DOC depending on operating modes. The decrease in TC was attributed to 35%–97% decrease in OC and 3%–65% decrease in EC emissions. At low load, a significant increase in the OC/EC ratio of PM_2.5 was observed after the DOC. The effect of the DOC on the carbonaceous compositions in PM_2.5 from B20 showed different trends compared to diesel fuel. At low load, a slight increase in EC emissions and a significant decrease in OC/EC ratio of PM_2.5 after DOC were observed for B20.     

上海市秋季典型大气高污染过程中颗粒物的化学组成变化特征

于2010年10月1日至11月30日在上海市城区对大气中颗粒物质量浓度及细粒子化学组分进行了在线连续观测,获得了秋季大气灰霾和沙尘等典型污染过程中颗粒物质量浓度和化学组成的变化特性.观测结果显示,在大气灰霾污染过程中PM₁₀和PM_2.5的日均最高浓度分别达到216~293 μg·m^-3和130~204 μg·m^-3,PM_2.5/PM₁₀的比值在65%以上,总的可溶性无机离子(TWSII)占PM_2.5质量浓度的50%以上,有机碳(OC)和元素碳(EC)的总和占25%~30%.二次可溶性离子(SO₄^2-, NO₃^-, NH₄⁺)占TWSII的83.3%~87.5%,OC/EC的比值在5左右,表明在灰霾污染过程中二次组分对PM_2.5的贡献较大;沙尘天气以粗粒子污染为主,TWSII、OC和EC分别仅占PM_2.5质量浓度的27.2%、13.4%和2.0%,二次可溶性离子(SO₄^2-, NO₃^-, NH₄⁺)占TWSII的55.7%,Ca²⁺、Mg²⁺等地壳组分的比例较灰霾天气明显升高.研究结果还显示,SO₄^2-和NO₃^-等二次离子组分的生成与颗粒物中硫与氮的氧化速率有关,在大气灰霾过程中硫转化率(SOR)和氮转化率(NOR)值较高,分别为0.24±0.10和0.15±0.06,说明SO₂通过二次反应生成SO₄^2-的能力较强,在污染的环境下高浓度的NO₂更有利于向NO₃^-转化.     

机动车源和民用燃料源颗粒物中有机碳和元素碳的排放特征

为了获取机动车源尾气和主要民用燃料源燃烧过程排放的颗粒物中含碳气溶胶的排放特征,使用多功能便携式稀释通道采样器和Model 5L-NDIR型OC/EC分析仪,采集分析了典型机动车源(汽油车、轻柴油车、重柴油车)、民用煤(块煤和型煤)和生物质燃料(麦秆、木板、葡萄树树枝)的PM₁₀和PM_2.5样品中的有机碳(OC)和元素碳(EC).结果表明,不同排放源释放的PM₁₀和PM_2.5中含碳气溶胶的质量分数存在显著差异.总碳(TC)在不同源PM₁₀和PM_2.5中的质量分数范围分别为40.8%～68.5%和30.5%～70.9%,OC/EC范围分别为1.49～31.56和1.90～87.57.不同源产生的含碳气溶胶均以OC为主,OC在PM₁₀和PM_2.5中的质量分数范围分别为56.3%～97.0%和65.0%～98.7%.在PM₁₀和PM_2.5的含碳气溶胶中OC质量分数按照从高到低...