灰霾天气期间南京气溶胶的化学组成及光学特性研究

利用2013年6月—12月灰霾天气期间南京城郊气溶胶采样结果,研究气溶胶中水溶性离子的特征和相关性;结合同期城区的大气成分逐时观测资料,分析黑碳的日变化及其与气态污染物的关系;运用光学参量计算模型(OPAC)和辐射传输模型(TUV)研究气溶胶的光学特性及辐射强迫。结果表明:发生灰霾天气时南京城郊主要大气污染物是细颗粒,其中SO2-4与NO-3是最主要的水溶性无机盐离子,NO-3/SO2-4质量比较高,呈现硫酸盐和硝酸盐混合型污染特征。黑碳浓度具有明显的日变化特征,呈双峰型结构。灰霾期间硫酸盐气溶胶在大气层顶和地面造成的平均辐射强迫分别为-10.6 W/m2和-10.8 W/m2,黑碳气溶胶在正午大气层顶和地面造成的平均辐射强迫分别为9.12 W/m2和-29.77 W/m2。     

南极大气气溶胶中铅同位素比值的研究

通过对电感耦合等离子体质谱(ICP-MS)的工作条件和参数进行优化,建立了ICP-MS测定铅同位素比值的精确方法,测量了2007—2009年南极中山站采集到的气溶胶样品中208Pb/206Pb、207Pb/206Pb和206Pb/207Pb的比值。结果表明,南极大气气溶胶中铅同位素比值在逐年缓慢地发生线性变化,线性相关系数为0.996 2;气溶胶铅同位素示踪揭示南极附近国家(除南非)释放的铅可能成为南极大气中铅的重要来源。     

Aerosol optical properties and the mixing state of black carbon at a background mountainous site in Eastern China

In-situ measurements of aerosol optical properties were conducted at Mt. Huang from September 23 to October 28, 2012. Low averages of 82.2, 10.9, and 14.1 Mm~(-1) for scattering coefficient(σ_(sp, neph, 550)), hemispheric backscattering coefficient(σ_(hbsp, neph, 550)), and absorption coefficient(σ_(ap, 550)), respectively, were obtained. Atmospheric aging process resulted in the increase of σap, 550 but the decrease of the single scattering albedo(ω_(550)) at constant aerosol concentration. However, the proportion of non-light-absorbing components(non-BCs) was getting higher during the aging process, resulting in the increase of aerosol diameter, which also contributed to relatively higher σ_(sp, neph, 550) and ω_(550). Diurnal cycles of σ_(sp, neph, 550) and σ_(ap, 550) with high values in the morning and low values in the afternoon were observed closely related to the development of the planetary boundary layer and the mountain-valley breeze. BC mixing state, represented by the volume fraction of externally mixed BC to total BC(r), was retrieved by using the modified Mie model.The results showed r reduced from about 70% to 50% when the externally mixed non-BCs were considered. The periodical change and different diurnal patterns of r were due to the atmospheric aging and different air sources under different synoptic systems. Local biomass burning emissions were also one of the influencing factors on r. Aerosol radiative forcing for different mixing state were evaluated by a "two-layer-single-wavelength" model,showing the cooling effect of aerosols weakened with BC mixing state changing from external to core-shell mixture.     

Au nanoring arrays as surface enhanced Raman spectroscopy substrate for chemical component study of individual atmospheric aerosol particle

Monolayer-ordered gold nanoring arrays were prepared by ion-sputtering method and used as surface enhanced Raman spectroscopy (SERS) substrates to test the individual atmospheric aerosols particle. Compared to other methods used for testing atmospheric aerosols particles, the collection and subsequent detection in our work is performed directly on the gold nanoring SERS substrate without any treatment of the analyte. The SERS performance can be tuned by changing the depth of the gold nanoring cavity as originating from coupling of dipolar modes at the inner and outer surfaces of the nanorings. The electric field exhibits uniform enhancement and polarization in the ordered Au nanoring substrate, which can improve the accuracy for detecting atmospheric aerosol particles. Combined with Raman mapping, the information about chemical composition of individual atmospheric aerosols particle and distribution of specific components can be presented visually. The results show the potential of SERS in enabling improved analysis of aerosol particle chemical composition, mixing state, and other related physicochemical properties.     

Application of an aerosol electrical mobility spectrum analyzer: Charged-particle polarity ratio measurement in the Antarctic and Arctic regions

An aerosol electrical mobility spectrum analyzer (AEMSA), developed at Hanyang University, was employed to investigate the particle charge characteristics in the Antarctic and Arctic regions. The particle charge characteristics in these areas were compared with the charging state in Ansan, South Korea, located in the midlatitude, where artificial factors, such as human activity, urbanization, and traffic, might result in a higher total concentration. Furthermore, in Ansan, South Korea, the charged-particle polarity ratio was very stable and was close to 1. However, notably different particle charge characteristics were obtained in the Antarctic and Arctic regions. The imbalance between the numbers of positively and negatively charged particles was evident, resulting in more positive charges on the atmospheric particles. On average, the positively charged particle concentrations in the Antarctic and Arctic areas were 1.4 and 2.8 times higher, respectively, compared with the negatively charged particles. The developed AEMSA system and the findings of this study provide useful information on the characteristics of atmospheric aerosols in the Antarctic and Arctic regions and can be further utilized to study particle formation mechanisms.     

Analysis of surface and aerosol polarized reflectance for aerosol retrievals from polarized remote sensing in PRD urban region

A precise estimate of polarization induced by surface is crucial for polarized remote sensing dedicated to monitoring aerosol properties over urban area. The accurate knowledge of interaction between surface and aerosol polarized reflectance is essential for accurately achieving aerosol properties. In order to study surface and aerosol polarized reflectance for aerosol retrievals over urban area, a new airborne directional polarimetric camera (DPC) with high spatial resolution (4 m at 4000 m a.g.l) was developed. The surface polarized reflectance over distinct surface covers of urban area (forest, shrub, and soil) were studied using DPC measurements during a field campaign in the Pearl River Delta (PRD), China. The large variations were found in surface polarized reflectance of distinct urban covers due to surface type variability. For all surface types, the empirical BPDF model cannot describe accurately surface polarized reflectance at all possible illumination and observation geometries. From the quantitatively study of relationship between surface and aerosol polarized contribution to DPC measurements, we show that the polarized contributions of aerosol, which optical properties were defined by ground-based measurements, are much larger than the polarized contribution of surface, and found that the polarized contribution of surface covers increases with decreasing NDVI. The effect of polarization accuracy of measurements on aerosol retrieval was also investigated using DPC measurements, and found that 0.1% polarization accuracy of measurements can be neglected when AOD is retrieved using polarized measurements. Based on the information of effects of polarized reflectance differences between distinct surface covers and polarization accuracy of polarized measurements on retrieved aerosols over urban area, we found that the accuracy of aerosol retrieval over forest covers is higher than other surface types using polarized remote sensing.     

Aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing in Guangzhou during the 2006 Pearl River Delta campaign

Optical and chemical aerosol measurements were obtained from 2 to 31 July 2006 at an urban site in the metropolitan area of Guangzhou (China) as part of the Program of Regional Integrated Experiment of Air Quality over Pearl River Delta (PRIDE-PRD2006) to investigate aerosol chemistry and the effect of aerosol water content on visibility impairment and radiative forcing. During the PRIDE-PRD2006 campaign, the average contributions of ammonium sulfate, organic mass by carbon (OMC), elemental carbon (EC), and sea salt (SS) to total PM_2.5 mass were measured to be 36.5%, 5.7%, 27.1%, 7.8%, and 3.7%, respectively. Compared with the clean marine period, (NH₄)₂SO₄, NH₄NO₃, and OMC were all greatly enhanced (by up to 430%) during local haze periods via the accumulation of a secondary aerosol component. The OMC dominance increased when high levels of biomass burning influenced the measurement site while (NH₄)₂SO₄ and OMC did when both biomass burning and industrial emissions influenced it. The effect of aerosol water content on the total light-extinction coefficient was estimated to be 34.2%, of which 25.8% was due to aerosol water in (NH₄)₂SO₄, 5.1% that in NH₄NO₃, and 3.3% that in SS. The average mass-scattering efficiency (MSE) of PM₁₀ particles was determined to be 2.2 ± 0.6 and 4.6 ± 1.7 m² g⁻¹ under dry (RH < 40%) and ambient conditions, respectively. The average single-scattering albedo (SSA) was 0.80 ± 0.08 and 0.90 ± 0.04 under dry and ambient conditions, respectively. Not only are the extinction and scattering coefficients greatly enhanced by aerosol water content, but MSE and SSA are also highly sensitive. It can be concluded that sulfate and carbonaceous aerosol, as well as aerosol water content, play important roles in the processes that determine visibility impairment and radiative forcing in the ambient atmosphere of the Guangzhou urban area.     

Size-resolved carbonaceous components and water-soluble ions measurements of ambient aerosol in Beijing

A MOUDI-120 sampler was used in Beijing to collect multi-stage samples in the summer and winter of 2013 to 2015. Thirty-three sample sets were collected during the daytime,nighttime, and different pollution levels. The actual relative humidity in the impactors was calculated for the first time. The carbonaceous components(organic and elemental carbon,OC and EC, respectively) and water-soluble inorganic ions(Na~+, NH_4~+, K~+, Mg~(2+), Ca~(2+), Cl~-, NO_3~-,and SO_4~(2-)) were analyzed in each sample. The characteristics of the mass concentration distribution and charge balance were discussed. On the basis of relative humidity in the impactors, aerosols less than 1.0 μm were sampled under relatively dry conditions in most cases. The concentration levels for the chemical species were higher in the winter than in the summer. Three modes(condensation mode, droplet mode, and coarse mode) could be identified from the distributions of NH_4~+, NO_3~-, SO_4~(2-), Cl~-, K~+, OC and EC. The distribution characteristics for the pollution dissipation process were different from the pollution accumulation process. NO_3~-and NO_2~-contributed most of the negative electric charges in the stage below 0.1 μm. In the condensation mode, the cations were dominated by NH_4~+, which was sufficient to balance the anions. In the droplet mode of the heavily polluted samples,the ammonium was not sufficient to balance the anions. In the coarse mode, the positive electric charges were primarily composed of metal cations. The analyzed anions were not sufficient to neutralize the measured cations.     

The characterization of heat transfer fluid P-NF aerosol combustion: Ignitable region and flame development

Heat transfer fluids tend to form aerosols due to the operating conditions at high pressure when accidental leaking occurs in pipelines or storage vessels, which may cause serious fires and explosions. Due to the physical property complexity of aerosols, it is difficult to define a standard term of “flammability limits” as is possible for gases. The study discussed in this paper primarily focuses on the characterization of ignition conditions and flame development of heat transfer fluid aerosols. The flammable region of a widely-used commercial heat transfer fluid, Paratherm NF (P-NF), was analyzed by electro-spray generation with a laser diffraction particle analysis method. The aerosol ignition behavior depends on the droplet size and concentration of the aerosol. From the adjustment of differently applied electro-spray voltages (7–10 kV) and various liquid feeding rates, a flammable condition distribution was obtained by comparison of droplet size and concentration. An appropriate amount (0.3–1.2 ppm) of smaller droplets (80–110 μm) existing in a given space could result in successful flame formation, while larger droplets (up to 190 μm) have a relatively narrowed range of flammable conditions (0.7–0.9 ppm). It is possible to generate a more useful reference for industry and lab scale consideration when handling liquids. This paper provides initial flammability criteria for analyzing P-NF aerosol fire hazards in terms of droplet size and volumetric concentration, discusses the observation of aerosol combustion processes, and summarizes an ignition delay phenomenon. All of the fundamental study results are to be applied to practical cases with fire hazards analysis, pressurized liquid handling, and mitigation system design once there is a better understanding of aerosols formed by high-flash point materials.     

杭州市大气气溶胶光学特性研究

利用太阳分光光度计（CE-318）对杭州市地面的气溶胶光学特性进行观测,并对卫星反演的中分辨率成像光谱仪（Moderate Resolution Imaging Spectroradiometer,MODIS）气溶胶产品进行验证.结果表明,MODIS气溶胶产品在杭州地区的精度较高,3个站点全部数据回归曲线的斜率和截距分...