利用2016年1~3月在青岛采集的Anderson分级气溶胶样品,分析其中10种微量元素总浓度和溶解态浓度,讨论了微量元素的浓度及溶解度的粒径谱分布特征及大气酸化过程的影响.结果表明,微量元素总浓度的粒径谱多数呈现单峰分布,Fe、Al、Ba、Sr等地壳元素总浓度的50%~60%出现在2.1~7.0μm粗粒子上;Cd、As、Zn、Pb等人为元素总浓度的60%~70%出现在0.43~2.1μm细粒子上;但Mn和Ni的粒径谱分布没有明显优势.溶解态微量元素的粒径谱也多呈现单峰分布,70%左右的Fe、Al、Ba、Sr、Mn集中在0.43~4.7μm粒子上;80%左右的Cd、As、Zn、Pb集中在0.43~2.1μm细粒子上;Ni的粒径谱分布与其总浓度的相似,在各粒级上无明显优势.微量元素溶解度的粒径谱分布呈现细粒子中的高于粗粒子中的,尤其是地壳元素这种分布趋势更为明显.气溶胶pH值的粒径谱分布特征及其与微量元素溶解度的显著相关关系表明,大气酸化过程是控制微量元素溶解度随粒径变化的主要因子.
Size-segregated atmospheric aerosol particles collected at a suburban site in Qingdao during January and March, 2016 were used to investigate size distributions of ten trace elements in mass concentration as well as their size-dependent solubility in relation to atmospheric acid processes. In general, size distributions of the total mass concentrations of the trace elements exhibited a uni-modal pattern. For example, Fe, Al, Ba and Sr, which are expected to mainly originate from crustal sources, mostly existed in the coarse particles(2.1~7.0μm), and the part mass accounted for 50%~60% of their total mass concentrations. Cd, As, Zn and Pb, which are expected to have strong anthropogenic contributors, were mainly distributed in the range of 0.43~2.1μm where the part mass accounted for 60%~70% of their total concentrations. However, there were no size trend for the total mass of Mn and Ni. The size distributions of water-soluble trace elements in mass concentration also exhibited a unimodal pattern. ~70% of water-soluble Fe, Al, Ba, Sr and Mn are distributed in the broad size range of 0.43~4.7μm, and nearly 80% of soluble Cd, As, Zn and Pb in mass concentration existed in the fine particles at 0.43~2.1μm. No size trend was found for the soluble Ni. The solubility of the trace elements was higher in fine particles than in coarse particles and this is particularly true for those derived from crustal sources. Moreover, the size distributions of the aerosol in-situ pH and the correlations between the pH and the elements' solubility implied that acidification processes in the atmosphere played a key role in determining the size-dependent solubility of the trace elements.