Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, Hangzhou 310027, China.
Department of Atmospheric Sciences, Texas A&M University, College Station, Texas 77843, United States.
Environ Sci Technol. 2021 Dec 21;55(24):16339-16346. doi: 10.1021/acs.est.1c05901. Epub 2021 Dec 12.
A large fraction of secondary aerosol particles are liquid-liquid phase-separated with an organic shell and an inorganic core. This has the potential to regulate the hygroscopicity of such particles, with significant implications for their optical properties, reactivity, and lifetime. However, it is unclear how this phase separation affects the hygroscopic growth of the particles. Here, we showed a large variation in hygroscopic growth (e.g., 1.14-1.32 under a relative humidity (RH) of 90%) of particles from the forest and urban atmosphere, which had different average core-shell ratios. For this reason, a controlled laboratory experiment further quantifies the impact of the organic shell on particle growth with different RH values. Laboratory experiments demonstrated that (NH)SO particles with thicker secondary organic shells have a lower growth factor at an RH below 94%. Organic shells started to deliquesce first (RH > 50%) and the phase changes of sulfate cores from solid to liquid took place at an RH higher than 80% as deliquescence relative humidity of pure (NH)SO. Our study provides the first direct evidence on an individual particle basis that hygroscopic growth behavior of phase-separated particles is dependent on the thickness of organic shells, highlighting the importance of organic coating in water uptake and possible heterogeneous reactions of the phase-separated particles.
大量二次气溶胶颗粒具有有机壳和无机核的液-液相分离结构。这有可能调节此类颗粒的吸湿性,对其光学性质、反应性和寿命有重大影响。然而,目前尚不清楚这种相分离如何影响颗粒的吸湿性增长。在这里,我们展示了来自森林和城市大气的颗粒的吸湿性增长(例如,在相对湿度 (RH) 为 90%的情况下为 1.14-1.32)存在很大差异,这些颗粒具有不同的平均核壳比。因此,一项受控的实验室实验进一步量化了不同 RH 值下有机壳对颗粒生长的影响。实验室实验表明,具有较厚二次有机壳的(NH)SO 颗粒在 RH 低于 94%时的生长因子较低。有机壳首先开始潮解(RH > 50%),硫酸盐核的相变为液态发生在 RH 高于 80%的情况下,这是纯(NH)SO 的 50%相对湿度。我们的研究首次提供了关于相分离颗粒的个体颗粒基础上的直接证据,表明相分离颗粒的吸湿性增长行为取决于有机壳的厚度,突出了有机涂层在吸水和可能的相分离颗粒的非均相反应中的重要性。