Ushijima Shuichi B, Huynh Erik, Davis Ryan D, Tolbert Margaret A
Department of Chemistry, University of Colorado, Boulder, 215 UCB, Boulder, Colorado 80309, United States.
Cooperative Institute for Research in Environmental Science, University of Colorado, Boulder, 216 UCB, Boulder, Colorado 80309, United States.
J Phys Chem A. 2021 Oct 7;125(39):8668-8679. doi: 10.1021/acs.jpca.1c04471. Epub 2021 Sep 23.
Atmospheric aerosols are complex with both inorganic and organic components. The soluble inorganics can transition between aqueous and crystalline phases through efflorescence and deliquescence. This study focuses on the efflorescence of (NH)SO/organic particles by seeded crystal growth through contact with a crystal of (NH)SO. Seeded crystal growth is known to effectively shut down supersaturation of aqueous aerosols. Here, we investigate whether organics can inhibit seeded crystal growth. We demonstrate that poly(ethylene glycol) 400 (PEG-400), which phase-separates from the aqueous (NH)SO and forms a core-shell structure, did not inhibit seeded crystal growth of (NH)SO at all relative humidity (RH) values below deliquescence RH. The PEG-400 layer was not viscous enough to prevent the diffusion of species through the coating. In contrast, we find that although raffinose, which stays homogeneously mixed with (NH)SO, did not inhibit seeded crystal growth at RH > 45%, it did inhibit heterogeneous efflorescence at lower humidities. Viscosity measurements using an electrodynamic balance show a significant increase in viscosity as humidity was lowered, suggesting that inhibited diffusion of water and ions prevented efflorescence. The observed efflorescence at the higher RH also demonstrates that collisions can induce efflorescence of mixed aerosols that would otherwise not homogeneously effloresce.
大气气溶胶成分复杂,包含无机和有机成分。可溶性无机物可通过潮解和风化在水相和结晶相之间转变。本研究聚焦于通过与硫酸铵晶体接触的籽晶生长来研究硫酸铵/有机颗粒的风化。已知籽晶生长能有效消除水雾气溶胶的过饱和度。在此,我们研究有机物是否能抑制籽晶生长。我们证明,聚乙二醇400(PEG - 400)从硫酸铵水溶液中相分离并形成核壳结构,在低于潮解相对湿度(RH)的所有相对湿度值下,它对硫酸铵的籽晶生长完全没有抑制作用。PEG - 400层的粘性不足,无法阻止物质通过涂层扩散。相比之下,我们发现,虽然棉子糖与硫酸铵均匀混合,在相对湿度> 45%时它不抑制籽晶生长,但在较低湿度下它确实抑制非均相风化。使用电动天平进行的粘度测量表明,随着湿度降低,粘度显著增加,这表明水和离子扩散受阻阻止了风化。在较高相对湿度下观察到的风化也表明,碰撞可诱导混合气溶胶发生风化,否则这些混合气溶胶不会发生均相风化。