Liquid-liquid phase separation in particles containing secondary organic material free of inorganic salts

被引:43
作者
Song, Mijung [1 ,2 ]
Liu, Pengfei [3 ]
Martin, Scot T. [3 ,4 ]
Bertram, Allan K. [2 ]
机构
[1] Chonbuk Natl Univ, Dept Earth & Environm Sci, Jeollabuk Do, South Korea
[2] Univ British Columbia, Dept Chem, Vancouver, BC V6T 1Z1, Canada
[3] Harvard Univ, John A Paulson Sch Engn & Appl Sci, Cambridge, MA 02138 USA
[4] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA
基金
美国国家科学基金会; 新加坡国家研究基金会; 加拿大自然科学与工程研究理事会;
关键词
COMPLEX REFRACTIVE-INDEXES; ALPHA-PINENE OZONOLYSIS; AEROSOL-PARTICLES; HYGROSCOPIC GROWTH; AMMONIUM-SULFATE; RELATIVE HUMIDITIES; MASS-SPECTROMETRY; MIXED PARTICLES; WATER-UPTAKE; RAIN-FOREST;
D O I
10.5194/acp-17-11261-2017
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Particles containing secondary organic material (SOM) are ubiquitous in the atmosphere and play a role in climate and air quality. Recently, research has shown that liquid-liquid phase separation (LLPS) occurs at high relative humidity (RH) (greater than similar to 95 %) in alpha-pinene-derived SOM particles free of inorganic salts, while LLPS does not occur in isoprene-derived SOM particles free of inorganic salts. We expand on these findings by investigating LLPS at 290 +/- 1K in SOM particles free of inorganic salts produced from ozonolysis of beta-caryophyllene, ozonolysis of limonene, and photo-oxidation of toluene. LLPS was observed at greater than similar to 95% RH in the biogenic SOM particles derived from beta-caryophyllene and limonene while LLPS was not observed in the anthropogenic SOM particles derived from toluene. This work combined with the earlier work on LLPS in SOM particles free of inorganic salts suggests that the occurrence of LLPS in SOM particles free of inorganic salts is related to the oxygen-to-carbon elemental ratio (O : C) of the organic material. These results help explain the difference between the hygroscopic parameter K of SOM particles measured above and below water saturation in the laboratory and field, and have implications for predicting the cloud condensation nucleation properties of SOM particles.
引用
收藏
页码:11261 / 11271
页数:11
相关论文
共 77 条
[1]   The effect of photochemical ageing and initial precursor concentration on the composition and hygroscopic properties of β-caryophyllene secondary organic aerosol [J].
Alfarra, M. R. ;
Hamilton, J. F. ;
Wyche, K. P. ;
Good, N. ;
Ward, M. W. ;
Carr, T. ;
Barley, M. H. ;
Monks, P. S. ;
Jenkin, M. E. ;
Lewis, A. C. ;
McFiggans, G. B. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (14) :6417-6436
[2]   Time-resolved molecular characterization of limonene/ozone aerosol using high-resolution electrospray ionization mass spectrometry [J].
Bateman, Adam P. ;
Nizkorodov, Sergey A. ;
Laskin, Julia ;
Laskin, Alexander .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2009, 11 (36) :7931-7942
[3]   Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component [J].
Bertram, A. K. ;
Martin, S. T. ;
Hanna, S. J. ;
Smith, M. L. ;
Bodsworth, A. ;
Chen, Q. ;
Kuwata, M. ;
Liu, A. ;
You, Y. ;
Zorn, S. R. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (21) :10995-11006
[4]   CCN activation of slightly soluble organics: the importance of small amounts of inorganic salt and particle phase [J].
Bilde, M ;
Svenningsson, B .
TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 2004, 56 (02) :128-134
[5]   Redistribution of black carbon in aerosol particles undergoing liquid-liquid phase separation [J].
Brunamonti, S. ;
Krieger, U. K. ;
Marcolli, C. ;
Peter, T. .
GEOPHYSICAL RESEARCH LETTERS, 2015, 42 (07) :2532-2539
[6]   Mass spectral characterization of submicron biogenic organic particles in the Amazon Basin [J].
Chen, Q. ;
Farmer, D. K. ;
Schneider, J. ;
Zorn, S. R. ;
Heald, C. L. ;
Karl, T. G. ;
Guenther, A. ;
Allan, J. D. ;
Robinson, N. ;
Coe, H. ;
Kimmel, J. R. ;
Pauliquevis, T. ;
Borrmann, S. ;
Poeschl, U. ;
Andreae, M. O. ;
Artaxo, P. ;
Jimenez, J. L. ;
Martin, S. T. .
GEOPHYSICAL RESEARCH LETTERS, 2009, 36
[7]   Particle-Phase Chemistry of Secondary Organic Material: Modeled Compared to Measured O:C and H:C Elemental Ratios Provide Constraints [J].
Chen, Qi ;
Liu, Yingjun ;
Donahue, Neil M. ;
Shilling, John E. ;
Martin, Scot T. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2011, 45 (11) :4763-4770
[8]   Liquid-Liquid Phase Separation in Mixed Organic/Inorganic Aerosol Particles [J].
Ciobanu, V. Gabriela ;
Marcolli, Claudia ;
Krieger, Ulrich K. ;
Weers, Uwe ;
Peter, Thomas .
JOURNAL OF PHYSICAL CHEMISTRY A, 2009, 113 (41) :10966-10978
[9]   Water uptake by biomass burning aerosol at sub- and supersaturated conditions: closure studies and implications for the role of organics [J].
Dusek, U. ;
Frank, G. P. ;
Massling, A. ;
Zeromskiene, K. ;
Iinuma, Y. ;
Schmid, O. ;
Helas, G. ;
Hennig, T. ;
Wiedensohler, A. ;
Andreae, M. O. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (18) :9519-9532
[10]   Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies [J].
Ervens, B. ;
Turpin, B. J. ;
Weber, R. J. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (21) :11069-11102