Size distribution and chemical composition of secondary organic aerosol formed from Cl-initiated oxidation of toluene

Secondary organic aerosol (SOA) formed from Cl-initiated oxidation of toluene was investigated in a home-made smog chamber. The size distribution and chemical composition of SOA particles were measured using aerodynamic particle sizer spectrometer and the aerosol laser time-of-flight mass spectrometer (ALTOFMS), respectively. According to a large number of single aerosol diameter and mass spectra, the size distribution and chemical composition of SOA were obtained statistically. Experimental results showed that SOA particles created by Cl-initiated oxidation of toluene is predominantly in the form of fine particles, which have diameters less than 2.5 m (i.e., PM2.5), and glyoxal, benzaldehyde, benzyl alcohol, benzoquinone, benzoic acid, benzyl hydroperoxide and benzyl methyl nitrate are the major products components in the SOA. The possible reaction mechanisms leading to these products are also proposed.     

大气中PAN的测定及其与前体物的关系

对北京中关村地区大气ＰＡＮ的监测结果表明：在强日照条件下，ＰＡＮ浓度随汽车等排放和ＮＯ２浓度的增加而增加，高ＰＡＮ浓度水平与高Ｏ３浓度相关联；夏季的ＰＡＮ浓度明显高于春季。模拟实验的结果证实：Ｃ３Ｈ６是大气中重要的ＰＡＮ前体物，在一定范围内，其浓度越高，ＰＡＮ浓度越大；Ｃ２Ｈ４生成ＰＡＮ是困难的，Ｈ２Ｏ２的存在对Ｃ２Ｈ４反应生成ＰＡＮ有促进作用；大气中ＳＯ２的存在可降低ＰＡＮ的生成速率。在〈４００     

地面氧化亚氮排放静态箱测定技术

氧化亚氮是最重要的温室效应气体之一,国际科学界对其进行了大量的研究。开展氧化亚氮研究最重要的方面是测定技术,目前主要有静态箱法和微气象法,而以静态箱技术的使用最为广泛。静态箱技术也有其优点和缺点。文章从基本原理、取样箱设计、取样时间策略、自动采样箱设计、气相色谱测定技术参数、计算方法及自动测定系统等方面,系统介绍静态箱技术。我国在氧化亚氮研究上还较少,已被测定的土地类型非常有限,文章将有助于促进我国在这方面的研究。     

氨对甲苯二次有机气溶胶形成和化学组分的影响研究

氨(NH_3)是大气中常见的主要碱性污染气体,能够影响二次有机气溶胶(SOA)的形成和化学组分.本文利用自制的烟雾腔系统开展了NH_3对甲苯SOA形成和化学组分的影响研究,先后采用扫描移动粒径谱仪(SMPS)、气溶胶激光飞行时间质谱仪(ALTOFMS)、紫外-可见分光光度计(UV-Vis)、衰减全反射傅里叶变换红外光谱仪(ATR-FTIR)和荧光光谱仪(MF)测量反应产生的SOA粒子的物理化学性质.结果显示,在光照60 min的时间范围内,有NH_3条件下形成的SOA质量浓度和中心粒径相比于无NH_3条件下分别增加了50%和25%,这说明NH_3能够显著促进甲苯SOA的形成.与无NH_3条件下相比,NH_3存在时甲苯SOA化学组分的紫外可见吸收光谱在270 nm处有明显的吸收峰;红外吸收光谱出现了CN、C—N、N—H键的吸收峰;激光解吸附质谱图中含有m/z=67(C_3H_3N_2~+)、m/z=41(C_2H_2N~+)和m/z=28(CH2N+)碎片峰.这些谱图信息综合表明是NH_3和甲苯SOA中的二醛组分反应形成了咪唑类新产物.这为研究人为源SOA的形成机制提供了实验依据.     

Gaseous mercury fluxes from the forest floor of the Adirondacks

The flux of gaseous elemental mercury (Hg⁰) from the forest floor of the Adirondack Mountains in New York (USA) was measured numerous times throughout 2005 and 2006 using a polycarbonate dynamic flux chamber (DFC). The Hg flux ranged between −2.5 and 27.2 ng m⁻² h⁻¹ and was positively correlated with temperature and solar radiation. The measured Hg emission flux was highest in spring, and summer, and lowest in winter. During leaf-off periods, the Hg emission flux was highly dependent on solar radiation and less dependent on temperature. During leaf-on periods, the Hg emission flux was fairly constant because the forest canopy was shading the forest floor. Two empirical models were developed to estimate yearly Hg⁰ emissions, one for the leaf-off period and one for the leaf-on period. Using the U.S. EPA's CASTNET meteorological data, the cumulative estimated emission flux was approx. 7.0 μg Hg⁰ m⁻² year⁻¹.     

Release flux of mercury from different environmental surfaces in Chongqing, China

An investigation was conducted to estimate mercury emission to the atmosphere from different environmental surfaces and to assess its contribution to the local mercury budget in Chongqing, China. Mercury flux was measured using dynamic flux chamber (DFC) at six soil sites of three different areas (mercury polluted area, farmland and woodland) and four water surfaces from August 2003 to April 2004. The mercury emission fluxes were 3.5 ± 1.2–8.4 ± 2.5 ng m⁻² h⁻¹ for three shaded forest sites, 85.8 ± 32.4 ng m⁻² h⁻¹ for farming field, 12.3 ± 9.8–733.8 ± 255 ng m⁻² h⁻¹ for grassland sites, and 5.9 ± 12.6–618.6 ± 339 ng m⁻² h⁻¹ for water surfaces. Mercury exchange fluxes were generally higher from air/water surfaces than from air/soil surfaces. The mercury negative fluxes were found in tow soil sites at overcast days (mean = −6.4 ± 1.5 ng m⁻² h⁻¹). The diurnal and seasonal variations of mercury flux were observed in all sites. The mercury emission responded positively to the solar radiation, but negatively to the relative humidity. The mercury flux from air/soil surfaces was significantly correlated with soil temperature, which was well described by an Arrhenius-type expression with activation energy of 31.1 kcal mol⁻¹. The annual mercury emission to the atmosphere from land surface is about 1.787 t of mercury in Chongqing.     

仲丁醇对苯乙烯臭氧化反应生成二次有机气溶胶的影响:实验和模型研究

通过烟雾箱实验,研究了仲丁醇对苯乙烯臭氧化反应生成二次有机气溶胶(SOA)的影响.结果发现,在烟雾箱实验中,过量仲丁醇的加入导致生成SOA的产率明显下降.同时,结合MCM气相机理和气-粒分配理论,将Criegee中间体与醛类的双分子反应添加到箱式模型中模拟烟雾箱中SOA的生成过程.模拟结果表明,在没有仲丁醇存在的情况下,次级臭氧化物在SOA组分中占1/2左右的比例.仲丁醇的加入消耗了大量的·OH,同时使得[HO_2]/[RO_2]比值升高,影响自由基相关的反应机制,使得SOA产率下降.另外,研究发现,Criegee中间体与醛类反应的速率常数也是影响SOA生成模拟的一个重要参数,需要进一步开展相关的动力学实验和理论研究.     

Investigation of basic properties of fly ash from urban waste incinerators in China

Basic properties of fly ash samples from different urban waste combustion facilities in China were analyzed using as X-ray fluorescence （XRF）, scanning electron microscopy （SEM）, X-ray diffraction （XRD）. The leaching toxicity procedure and some factors influencing heavy metals distribution in fly ash were further investigated. Experimental results indicate that the fly ash structures are complex and its properties are variable. The results of XRF and SEM revealed that the major elements （〉10000 mg/kg, listed in decreasing order of abundance） in fly ash are O, Ca, Cl, Si, S, K, Na, Al, Fe and Zn. These elements account for 93% to 97%, and the content of Cl ranges from 6.93% to 29.18 %, while that of SiO2 does from 4.48% to 24.84%. The minor elements （1000 to 10000 mg/kg） include Cr, Cu and Pb. Primary heavy metals in fly ash include Zn, Pb, Cr, Cu etc. According to standard leaching test, heavy metal leaching levels vary from 0 to 163.10 mg/L （Pb） and from 0.049 to 164.90 mg/L （Zn）, mostly exceeding the Chinese Identification Standard for hazardous wastes. Morphology of fly ash is irregular, with both amorphous structures and polycrystalline aggregates. Further research showed that heavy metals were volatilized at a high furnace temperature, condensed when cooling down during the post-furnace system and captured at air pollution control systems. Generally, heavy metals are mainly present in the forms of aerosol particulates or tiny particulates enriched on surfaces of fly ash particles. The properties of fly ash are greatly influenced by the treatment capacities of incinerators or the variation of waste retention time in chamber. Fly ash from combustors of larger capacities generally has higher contents of volatile component and higher leaching toxicity, while those of smaller capacities often produce fly ash containing higher levels of nonvolatile components and has lower toxicity. The content of heavy metals and leaching toxicity maybe have no convincing correlation, and high alkali content of CaO greatly contribute to leaching toxicity of heavy metal and acid neutralization capacity against acid rain.     

混响室与GTEM室中电磁辐照效应测试的相关性

在混响室和GTEM室中用连续波对同一敏感电路进行电磁辐照,测量电路的干扰阈值,统计分析实验数据,绘出混响室和GTEM室中电路干扰阈值的最小值、最大值和平均值随频率的变化曲线。据此对混响室和GTEM室的相关性进行定性分析;通过计算Pearson积差相关系数,对混响室和GTEM室的线性相关性进行定量分析。     

直接采样法确定面源恶臭挥发率的研究进展

确定面源恶臭挥发率的方法一般有两种:间接采样法和直接采样法.直接采样法由于具有许多优点而得到了广泛的应用.采样设备的选择会影响到恶臭样品的组成,通过对比可知,由动态采样器和静态采样器确定的恶臭挥发率的结果是不同的.用风洞法确定的恶臭挥发率与用问接法确定的恶臭挥发率有较好的一致性,可以作为恶臭扩散模型的输入参数.