Gas-Particle Uptake and Hygroscopic Growth by Organosulfate Particles
Gas-Particle Uptake and Hygroscopic Growth by Organosulfate Particles
复制标题
有机硫酸盐颗粒的气体颗粒吸收和吸湿生长
DOI：
10.1021/acsearthspacechem.2c00195
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发表时间：
2022
影响因子：
3.4
通讯作者：
Thomson, Regan J.
中科院分区：
文献类型：
--
作者：
Ohno, Paul E.;Wang, Junfeng;Mahrt, Fabian;Varelas, Jonathan G.;Aruffo, Eleonora;Ye, Jianhuai;Qin, Yiming;Kiland, Kristian J.;Bertram, Allan K.;Thomson, Regan J.
在地球大气的某些区域，有机硫酸盐化合物构成了粒子质量浓度的很大一部分，并且有机硫酸盐颗粒可以具有足够高的粘度来限制气体-颗粒相互作用的速率。粘度随相对湿度（RH）而变化。本文将有机硫酸盐颗粒暴露于α-蒎烯光氧化的气相产物中。在299 K条件下，在15 ~ 70% RH和<1 ~ 16 ppb NO条件下，研究了这些物种的气粒分配。α-蒎烯氧化产物的吸收随相对湿度的增加而增加，气相NO浓度的增加导致氮化合物颗粒相浓度的增加。用光学显微镜观察颗粒的吸湿性。在较高RH下的吸湿生长足以解释RH依赖的摄取测量，并且未观察到与颗粒粘度相关的动力学限制。缺乏动力学限制和Stokes-Einstein方程意味着粘度远小于1 × 106Pa s。该值与基于文献参数化的估计粘度一致，该参数化基于15% RH下至少0.05的颗粒中的水质量分数。总的来说，这些结果表明，有机硫酸盐的吸湿性在其粘度中起着关键作用，因此在调节气体-颗粒分配中起着关键作用，从而简化了地球大气模型中大气化学和污染物运输的处理。预计有机硫酸盐在预测未来排放趋势方面的作用将越来越重要。
Organosulfate compounds make up a substantial fraction of the particle mass concentration in some regions of the Earth’s atmosphere, and organosulfate particles can have sufficiently high viscosity to limit rates of gas-particle interactions. Viscosity varies with relative humidity (RH). Herein, organosulfate particles were exposed to the gas-phase products of α-pinene photooxidation. The gas-particle partitioning of these species was studied from 15 to 70% RH and <1 to 16 ppb NO at 299 K. The uptake of the α-pinene oxidation products increased with the increase in RH, and higher gas-phase NO concentrations resulted in increased particle-phase concentrations of nitrogen compounds. Particle hygroscopicity was examined by optical microscopy. Hygroscopic growth at elevated RH was sufficient to explain the RH-dependent uptake measurements, and kinetic limitations tied to particle viscosity were not observed. The lack of kinetic limitations combined with the Stokes–Einstein equation implied a viscosity much less than 1 × 106Pa s. This value is consistent with estimated viscosities based on literature parameterizations for water mass fractions in the particles of at least 0.05 at 15% RH. Overall, these results suggest that organosulfate hygroscopicity plays a key role in their viscosity and hence in regulating gas-particle partitioning, thereby simplifying the treatment of atmospheric chemistry and transport of pollutants in models of the Earth’s atmosphere. The role of organosulfates is expected to take on increasing importance for projected future emission trends.
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影响因子：
11.4
作者：
Aruffo, Eleonora;Wang, Junfeng;Ye, Jianhuai;Ohno, Paul;Qin, Yiming;Stewart, Matthew;McKinney, Karena;Di Carlo, Piero;Martin, Scot T.
通讯作者：
Martin, Scot T.
影响因子：
--
作者：
R. Stokes;R. Robinson
通讯作者：
R. Stokes;R. Robinson
影响因子：
3.4
作者：
Yuzhi Chen;T. Dombek;J. Hand;Zhenfa Zhang;A. Gold;A. Ault;K. Levine;J. Surratt
通讯作者：
Yuzhi Chen;T. Dombek;J. Hand;Zhenfa Zhang;A. Gold;A. Ault;K. Levine;J. Surratt
影响因子：
6.3
作者：
D. Spracklen;J. Jimenez;K. Carslaw;D. Worsnop;M. J. Evans;G. Mann;Q. Zhang;M. Canagaratna;
通讯作者：
D. Spracklen;J. Jimenez;K. Carslaw;D. Worsnop;M. J. Evans;G. Mann;Q. Zhang;M. Canagaratna;
影响因子：
2.3
作者：
M. Iwamatsu
通讯作者：
M. Iwamatsu