Fattori I, Becagli S, Bellandi S, Castellano E, Innocenti M, Mannini A, Severi M, Vitale V, Udisti R
Department of Chemistry, University of Florence-Scientific Pole, Department of Analytical Chemistry, Via della Lastruccia 3, I-50019, Sesto Fiorentino (FI), Italy.
J Environ Monit. 2005 Dec;7(12):1265-74. doi: 10.1039/b507327h. Epub 2005 Oct 20.
During the 2002-2003 austral summer field season, aerosol samples were collected at a coastal (Terra Nova Bay--Northern Victoria Land) and an inland site (Dome C--East Antarctic Plateau). The sampling was carried out by stacked filter units made up of two filters at different porosity (5.0 and 0.4 microm at Terra Nova Bay and 3.0 and 0.4 microm at Dome C), able to roughly separate a coarse from a fine fraction. At Dome C, a further investigation on aerosol size distribution was performed by an inertial impactor able to collect aerosol particles on 8 size classes (from 10 to 0.4 microm). Atomic Force Microscopy was applied to the filter collecting the finer fraction in both sites in order to assess the real cut-off value of the filter sandwich apparatus and to reconstruct the volume size distribution. At the employed flow conditions, the real cut-off value was revealed to be about one third with respect to the filter nominal porosity in both stations. The size distribution plots showed a bimodal distribution with a mode centered around 0.22 microm in both the sites and a second broader mode which is centered between 0.3 microm and 1.2 microm diameter at Terra Nova Bay and shifted toward higher values (centred around 1.0 microm diameter) at Dome C. Each filter was analysed for the main and trace ionic components allowing evaluation of the contributions of primary and secondary aerosol sources at the two sites as a function of the particle size class. The coastal site is mainly affected by primary and secondary marine inputs: the sea spray contribution (Na+, Mg2+, Cl- and ssSO4(2-)) is dominant (77% w/w) in the coarse fraction whereas the biogenic source (methanesulfonate and nssSO4(2-)) prevails (67.5% w/w) in the fine fraction. In this fraction a significant contribution (15.5% w/w) is provided by ammonium likely to be related to surrounding penguin colonies. Dome C atmosphere is characterised by fine particles arising from secondary sources and long-range transport processes. The main component in the fine and coarse fractions at Dome C is sulfate whose nssSO4(2-) represents the 99.5% and the 92.3%(w/w) in fine and coarse fraction, respectively. The observed agreement between nssSO4(2-) and methanesulfonate temporal profiles in the fine fraction demonstrates that biogenic emissions dominate the inland background aerosol. Results from the sampling by the 8-stage impactor at Dome C are presented here: chloride and nitrate are mainly deposited on the 10-2.1 microm stages while the highest sulfate concentration was found in the submicrometric fraction which turned out to be the most acidic. Such a distribution is able to prevent nitrate and chloride re-emission as gaseous HCl and HNO3 in the 10-2.1 microm stages, arising from the exchange reaction between chloride and nitrate salts and sulfuric acid. Moreover, the concentration peak observed for nitrate in coarser fractions is probably related also to the formation of hygroscopic NH4NO3 particles and nitrate adsorption on sea salt particles.
在2002 - 2003年澳大利亚夏季野外考察季期间,在一个沿海站点(特拉诺瓦湾 - 维多利亚地北部)和一个内陆站点( Dome C - 东南极高原)采集了气溶胶样本。采样通过由两个不同孔隙率的滤膜组成的叠层过滤装置进行(特拉诺瓦湾的孔隙率为5.0和0.4微米, Dome C的孔隙率为3.0和0.4微米),能够大致分离出粗颗粒和细颗粒部分。在Dome C,通过一个惯性撞击器对气溶胶粒径分布进行了进一步研究,该撞击器能够收集8个粒径级别的气溶胶颗粒(从10到0.4微米)。原子力显微镜应用于两个站点收集细颗粒部分的滤膜,以评估滤膜夹层装置的实际截止值并重建体积粒径分布。在所采用的流动条件下,两个站点的实际截止值相对于滤膜标称孔隙率约为三分之一。粒径分布图显示出双峰分布,两个站点的一个峰都集中在0.22微米左右,在特拉诺瓦湾第二个更宽的峰集中在直径0.3微米到1.2微米之间,而在Dome C则向更高值移动(集中在直径1.0微米左右)。对每个滤膜的主要和痕量离子成分进行了分析,从而能够评估两个站点主要和次要气溶胶源随粒径级别的贡献。沿海站点主要受主要和次要海洋输入的影响:海浪喷雾贡献(Na +、Mg2 +、Cl - 和ssSO4(2 -))在粗颗粒部分占主导(77% w/w),而生物源(甲磺酸盐和nssSO4(2 -))在细颗粒部分占优(67.5% w/w)。在这个部分,铵有显著贡献(15.5% w/w),可能与周围的企鹅群落有关。Dome C的大气特征是由次要源和长距离传输过程产生的细颗粒。Dome C细颗粒和粗颗粒部分的主要成分都是硫酸盐,其nssSO4(2 -)在细颗粒和粗颗粒部分分别占99.5%和92.3%(w/w)。在细颗粒部分观察到的nssSO4(2 -)和甲磺酸盐时间剖面之间的一致性表明生物源排放主导了内陆背景气溶胶。这里展示了在Dome C通过八级撞击器采样的结果:氯化物和硝酸盐主要沉积在10 - 2.1微米级上,而在亚微米级部分发现了最高的硫酸盐浓度,该部分也是酸性最强的。这种分布能够防止在10 - 2.1微米级上由于氯化物和硝酸盐盐与硫酸之间的交换反应而使硝酸盐和氯化物以气态HCl和HNO3的形式重新排放。此外,在较粗颗粒部分观察到的硝酸盐浓度峰值可能也与吸湿性NH4NO3颗粒的形成以及硝酸盐在海盐颗粒上的吸附有关。