Effects of Atmospheric Aging Processes on Nascent Sea Spray Aerosol Physicochemical Properties.
Effects of Atmospheric Aging Processes on Nascent Sea Spray Aerosol Physicochemical Properties.
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DOI：
10.1021/acsearthspacechem.2c00258
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发表时间：
2022-11-17
影响因子：
3.4
通讯作者：
V. Tivanski, Alexei
中科院分区：
文献类型：
--
作者：
Kaluarachchi, Chathuri P.;Or, Victor W.;Lan, Yiling;Hasenecz, Elias S.;Kim, Deborah;Madawala, Chamika K.;Dorc, Glorianne P.;Mayer, Kathryn J.;Sauer, Jonathan S.;Lee, Christopher;Cappa, Christopher D.;Bertram, Timothy H.;Stone, Elizabeth A.;Prather, Kimberly A.;Grassian, Vicki H.;V. Tivanski, Alexei
关键词：
大气老化对单颗粒新生海浪气溶胶 (nSSA) 物理化学性质（例如形态、成分、相态和吸水量）的影响对于了解其对地球气候的影响非常重要。本研究通过关注老化的SSA（尺寸范围为0.1-0.6μm）并与类似尺寸范围的nSSA进行比较来研究这些特性，这两种SSA都是在中生态研究期间在浮游植物繁殖高峰期产生的。老化的 SSA 是通过将 nSSA 暴露于 OH 自由基中而产生的，暴露量相当于 4-5 天的大气老化。利用基于互补滤光片的热光学分析、原子力显微镜 (AFM) 和 AFM 光热红外光谱。 nSSA 和老化 SSA 的有机质量分数随着粒径的减小而增加。此外，老化导致有机质量分数进一步增加，这可归因于新颗粒的形成和挥发性有机化合物的氧化，然后在预先存在的颗粒上凝结。结果与单颗粒测量结果一致，单颗粒测量结果表明，相对于 nSSA，老化的 SSA 核壳丰度相对增加，有机涂层厚度显着更高。观察到老化的 SSA 核壳的吸湿性增加，其中含有更多的含氧有机物质。圆形nSSA和老化SSA具有相似的吸湿性并且成分没有明显变化。观察到的老化 SSA 物理化学性质的变化显示出显着的尺寸依赖性和颗粒间的变异性。总体而言，结果表明，大气老化可以显着影响nSSA的理化性质，从而改变SSA对气候的影响。
The effects of atmospheric aging on single-particle nascent sea spray aerosol (nSSA) physicochemical properties, such as morphology, composition, phase state, and water uptake, are important to understanding their impacts on the Earth’s climate. The present study investigates these properties by focusing on the aged SSA (size range of 0.1–0.6 μm) and comparing with a similar size range nSSA, both generated at a peak of a phytoplankton bloom during a mesocosm study. The aged SSAs were generated by exposing nSSA to OH radicals with exposures equivalent to 4–5 days of atmospheric aging. Complementary filter-based thermal optical analysis, atomic force microscopy (AFM), and AFM photothermal infrared spectroscopy were utilized. Both nSSA and aged SSA showed an increase in the organic mass fraction with decreasing particle sizes. In addition, aging results in a further increase of the organic mass fraction, which can be attributed to new particle formation and oxidation of volatile organic compounds followed by condensation on pre-existing particles. The results are consistent with single-particle measurements that showed a relative increase in the abundance of aged SSA core–shells with significantly higher organic coating thickness, relative to nSSA. Increased hygroscopicity was observed for aged SSA core–shells, which had more oxygenated organic species. Rounded nSSA and aged SSA had similar hygroscopicity and no apparent changes in the composition. The observed changes in aged SSA physicochemical properties showed a significant size-dependence and particle-to-particle variability. Overall, results showed that the atmospheric aging can significantly influence the nSSA physicochemical properties, thus altering the SSA effects on the climate.
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影响因子：
5.2
作者：
Cappa, Christopher D.;Ristenpart, William D.;Roman, Sanziana A.
通讯作者：
Roman, Sanziana A.
影响因子：
5.7
作者：
Cochran, Richard E.;Jayarathne, Thilina;Grassian, Vicki H.
通讯作者：
Grassian, Vicki H.
影响因子：
3.8
作者：
Collins, D. B.;Zhao, D. F.;Prather, K. A.
通讯作者：
Prather, K. A.
影响因子：
5
作者：
George, I. J.;Chang, R. Y. -W.;Abbatt, J. P. D.
通讯作者：
Abbatt, J. P. D.
影响因子：
11.4
作者：
Ault, Andrew P.;Moffet, Ryan C.;Grassian, Vicki H.
通讯作者：
Grassian, Vicki H.