Pelimanni Eetu, Saak Clara-Magdalena, Michailoudi Georgia, Prisle Nønne, Huttula Marko, Patanen Minna
Nano and Molecular Systems Research Unit, Faculty of Science, University of Oulu, Box 3000, 90014, Finland.
Department of Physics and Astronomy, Uppsala University, Box 516, 75120 Uppsala, Sweden.
Phys Chem Chem Phys. 2022 Feb 2;24(5):2934-2943. doi: 10.1039/d1cp04953d.
The formation of multicomponent aerosol particles from precursor solution droplets often involves segregation and surface enrichment of the different solutes, resulting in non-homogeneous particle structures and diverse morphologies. In particular, these effects can have a significant influence on the chemical composition of the particle-vapor interface. In this work, we investigate the bulk/surface partitioning of inorganic ions, Na, Mg, Ca, Cl and Br, in atomiser-generated submicron aerosols using synchrotron radiation based X-ray photoelectron spectroscopy (XPS). Specifically, the chemical compositions of the outermost few nm thick surface layers of non-supported MgCl/CaCl and NaBr/MgBr particles are determined. It is found that in MgCl/CaCl particles, the relative abundance of the two species in the particle surface correlates well with their mixing ratio in the parent aqueous solution. In stark contrast, extreme surface enrichment of Mg is observed in NaBr/MgBr particles formed from both aqueous and organic solution droplets, indicative of core-shell structures. Structural properties and hydration state of the particles are discussed.
由前驱体溶液滴形成多组分气溶胶颗粒通常涉及不同溶质的分离和表面富集,从而导致颗粒结构不均匀和形态多样。特别是,这些效应会对颗粒 - 蒸汽界面的化学成分产生重大影响。在这项工作中,我们使用基于同步辐射的X射线光电子能谱(XPS)研究雾化产生的亚微米气溶胶中无机离子Na、Mg、Ca、Cl和Br的体相/表面分配。具体而言,确定了无支撑的MgCl/CaCl和NaBr/MgBr颗粒最外层几纳米厚表面层的化学成分。研究发现,在MgCl/CaCl颗粒中,颗粒表面两种物质的相对丰度与其在母液中的混合比密切相关。与此形成鲜明对比的是,在由水溶液和有机溶液滴形成的NaBr/MgBr颗粒中观察到Mg的极端表面富集,这表明存在核壳结构。还讨论了颗粒的结构性质和水合状态。