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DOI | 10.5194/acp-19-12515-2019 |
Liquid-liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors | |
Song, Mijung1,2; Maclean, Adrian M.2; Huang, Yuanzhou2; Smith, Natalie R.3; Blair, Sandra L.3; Laskin, Julia4; Laskin, Alexander4; DeRieux, Wing-Sy Wong3; Li, Ying3; Shiraiwa, Manabu3; Nizkorodov, Sergey A.3; Bertram, Allan K.2 | |
2019-10-08 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2019 |
卷号 | 19期号:19页码:12515-12529 |
文章类型 | Article |
语种 | 英语 |
国家 | South Korea; Canada; USA |
英文摘要 | Information on liquid-liquid phase separation (LLPS) and viscosity (or diffusion) within secondary organic aerosol (SOA) is needed to improve predictions of particle size, mass, reactivity, and cloud nucleating properties in the atmosphere. Here we report on LLPS and viscosities within SOA generated by the photooxidation of diesel fuel vapors. Diesel fuel contains a wide range of volatile organic compounds, and SOA generated by the photooxidation of diesel fuel vapors may be a good proxy for SOA from anthropogenic emissions. In our experiments, LLPS occurred over the relative humidity (RH) range of similar to 70 % to similar to 100 %, resulting in an organic-rich outer phase and a water-rich inner phase. These results may have implications for predicting the cloud nucleating properties of anthropogenic SOA since the presence of an organic-rich outer phase at high-RH values can lower the supersaturation with respect to water required for cloud droplet formation. At <= 10 % RH, the viscosity was >= 1 x 10(8) Pa s, which corresponds to roughly the viscosity of tar pitch. At 38 %-50 % RH, the viscosity was in the range of 1 x 10(8) to 3 x 10(5) Pas. These measured viscosities are consistent with predictions based on oxygen to carbon elemental ratio (O : C) and molar mass as well as predictions based on the number of carbon, hydrogen, and oxygen atoms. Based on the measured viscosities and the Stokes-Einstein relation, at <= 10 % RH diffusion coefficients of organics within diesel fuel SOA is <= 5.4 x 10(-17) cm(2) s(-1) and the mixing time of organics within 200 nm diesel fuel SOA particles (tau(mixing)) is 50 h. These small diffusion coefficients and large mixing times may be important in laboratory experiments, where SOA is often generated and studied using low-RH conditions and on timescales of minutes to hours. At 38 %-50 % RH, the calculated organic diffusion coefficients are in the range of 5.4 x 10(-17) to 1.8 x 10(-13) cm(2) s(-1) and calculated tau(mixing) values are in the range of similar to 0.01 h to similar to 50 h. These values provide important constraints for the physicochemical properties of anthropogenic SOA. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000489597200003 |
WOS关键词 | SIZE DISTRIBUTION DYNAMICS ; ALPHA-PINENE OZONOLYSIS ; LONG-RANGE TRANSPORT ; GLASS-TRANSITION ; RELATIVE HUMIDITIES ; HYGROSCOPIC GROWTH ; AMMONIUM-SULFATE ; ICE NUCLEATION ; MOLECULAR CHARACTERIZATION ; DIFFUSION-COEFFICIENTS |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/187596 |
专题 | 地球科学 |
作者单位 | 1.Chonbuk Natl Univ, Dept Earth & Environm Sci, Jeollabuk Do 54896, South Korea; 2.Univ British Columbia, Dept Chem, Vancouver, BC V6T 1Z1, Canada; 3.Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA; 4.Purdue Univ, Dept Chem, W Lafayette, IN 47907 USA |
推荐引用方式 GB/T 7714 | Song, Mijung,Maclean, Adrian M.,Huang, Yuanzhou,et al. Liquid-liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(19):12515-12529. |
APA | Song, Mijung.,Maclean, Adrian M..,Huang, Yuanzhou.,Smith, Natalie R..,Blair, Sandra L..,...&Bertram, Allan K..(2019).Liquid-liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(19),12515-12529. |
MLA | Song, Mijung,et al."Liquid-liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.19(2019):12515-12529. |
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