Frontier Science Organization, Kanazawa University, Kanazawa, Ishikawa 920-1192, Japan.
Proc Natl Acad Sci U S A. 2010 Oct 19;107(42):17905-10. doi: 10.1073/pnas.1008235107. Epub 2010 Oct 4.
The chemical history of dust particles in the atmosphere is crucial for assessing their impact on both the Earth's climate and ecosystem. So far, a number of studies have shown that, in the vicinity of strong anthropogenic emission sources, Ca-rich dust particles can be converted into aqueous droplets mainly by the reaction with gaseous HNO(3) to form Ca(NO(3))(2). Here we show that other similar processes have the potential to be activated under typical remote marine atmospheric conditions. Based on field measurements at several sites in East Asia and thermodynamic predictions, we examined the possibility for the formation of two highly soluble calcium salts, Ca(NO(3))(2) and CaCl(2), which can deliquesce at low relative humidity. According to the results, the conversion of insoluble CaCO(3) to Ca(NO(3))(2) tends to be dominated over urban and industrialized areas of the Asian continent, where the concentrations of HNO(3) exceed those of HCl ([HNO(3)/HCl] > ∼ 1). In this regime, CaCl(2) is hardly detected from dust particles. However, the generation of CaCl(2) becomes detectable around the Japan Islands, where the concentrations of HCl are much higher than those of HNO(3) ([HNO(3)/HCl] < ∼ 0.3). We suggest that elevated concentrations of HCl in the remote marine boundary layer are sufficient to modify Ca-rich particles in dust storms and can play a more important role in forming a deliquescent layer on the particle surfaces as they are transported toward remote ocean regions.
大气中尘埃颗粒的化学历史对于评估其对地球气候和生态系统的影响至关重要。到目前为止,许多研究表明,在强人为排放源附近,富钙尘埃颗粒可以通过与气态 HNO(3)反应主要转化为含水液滴,形成 Ca(NO(3))(2)。在这里,我们表明,在典型的远程海洋大气条件下,其他类似的过程也有可能被激活。基于东亚几个站点的现场测量和热力学预测,我们研究了两种高溶解性钙盐 Ca(NO(3))(2)和 CaCl(2)形成的可能性,这两种盐在低相对湿度下会潮解。根据结果,不溶性 CaCO(3)向 Ca(NO(3))(2)的转化在亚洲大陆的城市和工业化地区占主导地位,那里 HNO(3)的浓度超过 HCl([HNO(3)/HCl]>∼1)。在这种情况下,尘埃颗粒中几乎检测不到 CaCl(2)。然而,在日本群岛周围可以检测到 CaCl(2 的生成,那里 HCl 的浓度远高于 HNO(3)([HNO(3)/HCl]<∼0.3)。我们认为,远程海洋边界层中 HCl 浓度的升高足以改变尘埃暴中的富钙颗粒,并在它们向远程海洋区域输送时,在颗粒表面形成更具吸湿性的层,从而发挥更重要的作用。