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尺寸相关新生海雾气溶胶反弹分数与预估黏度:二价阳离子富化作用、表面张力和开尔文效应的作用。

Size-Dependent Nascent Sea Spray Aerosol Bounce Fractions and Estimated Viscosity: The Role of Divalent Cation Enrichment, Surface Tension, and the Kelvin Effect.

机构信息

Department of Chemistry & Biochemistry, University of California San Diego, La Jolla, California 92093, United States.

Department of Chemistry, California State University, Fullerton, California 92831, United States.

出版信息

Environ Sci Technol. 2024 Nov 5;58(44):19666-19678. doi: 10.1021/acs.est.4c04312. Epub 2024 Oct 23.

Abstract

Viscosity, or the "thickness," of aerosols plays a key role in atmospheric processes like ice formation, water absorption, and heterogeneous kinetics. However, the viscosity of sea spray aerosols (SSA) has not been widely studied. This research explored the relationship between particle size and viscosity of authentic SSA particles through particle bounce, atomic force microscopy analysis, and predictive viscosity modeling from molecular composition. The study found that 40 nm SSA particles had estimated viscosities around 10 Pa·s and bounce fractions three times higher than 100 and 200 nm particles with less than 10 Pa·s at a relative humidity (RH) of 60%. Additional studies revealed the Kelvin effect and particle density, influenced by particle size, have a greater impact on size-dependent bounce fractions than changes in RH across impactor stages. While changes in the level of surfactants can impact particle bounce, the increased viscosity in smaller SSA is attributed to the formation of gel-like phase states caused by cation-organic cross-links between divalent calcium ions and organic anions enriched in the smaller particles. This work shows the smallest gel-like SSA particles observed in the field are highly viscous, which has implications for cloud formation, secondary aerosol growth, and pollutant transport in coastal environments.

摘要

气溶胶的黏度,或“稠度”,在大气过程中起着关键作用,如冰形成、水吸收和非均相动力学。然而,海雾气溶胶(SSA)的黏度尚未得到广泛研究。本研究通过颗粒反弹、原子力显微镜分析以及从分子组成预测的黏度模型,探究了真实 SSA 颗粒的粒径与黏度之间的关系。研究发现,在相对湿度(RH)为 60%时,40nm 的 SSA 颗粒的估计黏度约为 10Pa·s,反弹分数比 100nm 和 200nm 颗粒高三倍,而后者的黏度小于 10Pa·s。进一步的研究揭示了 Kelvin 效应和颗粒密度的影响,粒径对大小依赖性反弹分数的影响大于 RH 在撞击器阶段的变化。虽然表面活性剂水平的变化会影响颗粒反弹,但较小的 SSA 中增加的黏度归因于二价钙离子与富含较小颗粒的有机阴离子之间形成的阳离子-有机交联导致的凝胶状相态的形成。这项工作表明,在现场观测到的最小凝胶状 SSA 颗粒具有高黏度,这对云形成、二次气溶胶生长以及沿海环境中的污染物传输具有重要意义。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72c1/11542888/42a4fa1b541b/es4c04312_0001.jpg

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