Ferdousi-Rokib Nahin, A Malek Kotiba, Mitchell Ian, M Fierce Laura, Asa-Awuku Akua A
Department of Chemical and Biomolecular Engineering, A. James Clark School of Engineering, University of Maryland, College Park, College Park, Maryland 20742, United States.
Pacific Northwest National Laboratory, Richland, Washington 99354, United States.
ACS EST Air. 2025 Jul 7;2(8):1454-1467. doi: 10.1021/acsestair.4c00303. eCollection 2025 Aug 8.
The partitioning between inorganic salts and organic compounds within individual particles is a key factor that influences the uptake of water by particles. In this study, we investigated the aerosol hygroscopicity of ammonium sulfate (AS) and 2-methylglutaric acid (2-MGA) mixtures. 2-MGA is a moderately surface-active compound. Dilute surface tension measurements of 2-MGA/AS mixtures were taken by using a pendant drop goniometer. Hygroscopicity at subsaturated conditions was determined using a hygroscopicity tandem differential mobility analyzer (H-TDMA) and relative humidity was kept constant at 89 ± 0.9% RH. The droplet activation was also measured at supersaturated conditions using a cloud condensation nuclei counter (CCNC) from 0.4 to 1% supersaturation (SS). The single-hygroscopicity parameter κ was derived from measurements. Mixtures predominantly composed of AS, up to a 60 wt% 2-MGA, exhibit κ-values close to pure AS. However, κ decreases significantly as the organic fraction increases (>60 wt% 2-MGA). Previous predictions of κ-hygroscopicity assume full dissolution of both the organic and inorganic compounds. However, organic partitioning can influence the κ-hygroscopicity. A coverage-based parametrization, ϕ, assumes the probability of surface-active organics at the droplet surface. By estimation of the bulk and surface organic contribution, overall κ-hygroscopicity can be calculated. The model is computationally efficient, and the results indicate that organic solute depletion should be considered for fully soluble surface-active organics. Hygroscopicity predictions that account for the role of organic surface-active partitioning agree best with experimental results ( > 0.95). Therefore, this study helps to enhance our understanding of cloud-forming properties of complex chemical mixtures containing surface-active organic and inorganic compounds.
单个颗粒内无机盐与有机化合物之间的分配是影响颗粒吸水性的关键因素。在本研究中,我们调查了硫酸铵(AS)和2-甲基戊二酸(2-MGA)混合物的气溶胶吸湿性。2-MGA是一种中度表面活性化合物。使用悬滴测角仪对2-MGA/AS混合物进行了稀溶液表面张力测量。使用吸湿性串联差分迁移率分析仪(H-TDMA)测定了亚饱和条件下的吸湿性,相对湿度保持在89±0.9%RH不变。还使用云凝结核计数器(CCNC)在0.4%至1%过饱和度(SS)的过饱和条件下测量了液滴活化情况。从测量结果中得出了单一吸湿性参数κ。主要由AS组成的混合物,2-MGA含量高达60 wt%时,其κ值接近纯AS。然而,随着有机成分增加(>60 wt% 2-MGA),κ值会显著降低。先前对κ-吸湿性的预测假定有机和无机化合物都能完全溶解。然而,有机分配会影响κ-吸湿性。基于覆盖率的参数化方法ϕ假定了液滴表面存在表面活性有机物的概率。通过估算本体和表面有机成分的贡献,可以计算出整体κ-吸湿性。该模型计算效率高,结果表明对于完全可溶的表面活性有机物应考虑有机溶质耗尽的情况。考虑有机表面活性分配作用的吸湿性预测与实验结果最吻合(>0.95)。因此,本研究有助于增进我们对含有表面活性有机和无机化合物的复杂化学混合物成云特性的理解。