Deliquescence and Efflorescence Behavior of Ternary Inorganic/Organic/Water Aerosol Particles

被引：34

作者：

Peckhaus, Andreas ^{[1
]}

Grass, Stefan ^{[1
]}

Treuel, Lennart ^{[1
]}

Zellner, Reinhard ^{[1
]}

机构：

[1] Univ Duisburg Essen, Inst Phys Chem, D-45117 Essen, Germany

来源：

JOURNAL OF PHYSICAL CHEMISTRY A | 2012年 / 116卷 / 24期

关键词：

MIXED AMMONIUM-SULFATE; DISSOLVED INORGANIC SALTS; UNIFAC GROUP-CONTRIBUTION; LIQUID PHASE-SEPARATION; ACTIVITY-COEFFICIENTS; THERMODYNAMIC MODEL; ORGANIC-COMPOUNDS; MALONIC-ACID; HYGROSCOPIC PROPERTIES; DICARBOXYLIC-ACIDS;

D O I：

10.1021/jp211522t

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The deliquescence behavior of ternary inorganic (ammonium sulfate and ammonium nitrate)/organic (glutaric acid and malonic acid)/water aerosol particles has been investigated at 293 K using a novel surface aerosol microscopy (SAM) technique. The results obtained for the deliquescence relative humidities (DRH) for particles of variable inorganic/organic contents show a eutectic behavior with the mixed particles showing deliquescence at lower DRH compared to the pure inorganic and organic components, respectively. This behavior has been quantitatively modeled using the extended aerosol inorganics (E-AIM) thermodynamic model of Clegg et al. in combination with the UNIFAC group activity approach to account for organic molecular solutes. In addition, we have investigated the crystallization behavior of supersatured and formerly deliquesced ternary solution droplets using space resolved Raman spectroscopy. It is found that such droplets produce solid particles in which the inorganic and organic phases show some spatial separation with the organic component being predominantly found at the outer part of the particle. Independent measurements of the contact angles of such ternary droplets reveal that their angles are within experimental error identical to those of the purely organic/water solutions.

引用

页码：6199 / 6210

页数：12

共 114 条

[1] General circulation model assessment of direct radiative forcing by the sulfate-nitrate-ammonium-water inorganic aerosol system [J].

Adams, PJ ;

Seinfeld, JH ;

Koch, D ;

Mickley, L ;

Jacob, D .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2001, 106 (D1) :1097-1111

[2] A phase equilibrium model for atmospheric aerosols containing inorganic electrolytes and organic compounds (UHAERO), with application to dicarboxylic acids [J].

Amundson, N. R. ;

Caboussat, A. ;

He, J. W. ;

Martynenko, A. V. ;

Seinfeld, J. H. .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2007, 112 (D24)

[3]

[Anonymous], PHASE BEHAV BINARY T

[4]

[Anonymous], 1996, AIR QUAL CRIT PART M

[5] Carboxylic acids in gas and particulate phase above the Atlantic Ocean [J].

Baboukas, ED ;

Kanakidou, M ;

Mihalopoulos, N .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2000, 105 (D11) :14459-14471

[6] UNIFAC parameters for four new groups [J].

Balslev, K ;

Abildskov, J .

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2002, 41 (08) :2047-2057

[7] 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

[8] Surface tension of mixed inorganic and dicarboxylic acid aqueous solutions at 298.15 K and their importance for cloud activation predictions [J].

Booth, Alastair Murray ;

Topping, David Owen ;

McFiggans, Gordon ;

Percival, Carl John .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2009, 11 (36) :8021-8028

[9] VIBRATIONAL-SPECTRA AND DYNAMICS OF CRYSTALLINE MALONIC-ACID AT ROOM-TEMPERATURE [J].

BOUGEARD, D ;

DEVILLEPIN, J ;

NOVAK, A .

SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1988, 44 (12) :1281-1286

[10] A study of the phase transition behavior of internally mixed ammonium sulfate-malonic acid aerosols [J].

Braban, CF ;

Abbatt, JPD .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2004, 4 :1451-1459

← 1 2 3 4 5 6 7 8 9 10 →