Water uptake of internally mixed ammonium sulfate and dicarboxylic acid particles probed by infrared spectroscopy

被引:31
作者
Minambres, Lorena [1 ]
Mendez, Estibaliz [1 ]
Sanchez, Maria N. [1 ]
Castano, Fernando [1 ]
Basterretxea, Francisco J. [1 ]
机构
[1] Univ Basque Country, Dept Quim Fis, Fac Ciencia & Tecnol, UPV EHU, Leioa 48940, Spain
关键词
Tropospheric aerosols; Deliquescence; Hygroscopicity; Vibrational spectrum; Band broadening; Ion-molecule interactions; HYGROSCOPIC PROPERTIES; DELIQUESCENCE PROPERTIES; PHASE-TRANSITIONS; EFFLORESCENCE; AEROSOLS; SALT;
D O I
10.1016/j.atmosenv.2013.01.007
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Tropospheric aerosols are usually mixtures of inorganic and organic compounds in variable proportions, and the relative amount of organic fraction can influence the hygroscopic properties of the particles. Infrared spectra of submicrometer internally mixed dry particles of ammonium sulfate (AS) with various dicarboxylic acids (oxalic, malonic, maleic, glutaric and pimelic) have been measured in an aerosol flow tube at several solute mass ratios. The spectra show a notable broadening in the bandwidth of sulfate ion v(3) vibrational band near 1115 cm(-1) with respect to pure AS. We attribute these perturbations, that are biggest at AS/organic acid mass ratio near unity, to intermolecular interactions between inorganic ions and organic acid molecules in the internally mixed solids. The water uptake behavior of internally mixed particles has been measured by recording the infrared integrated absorbance of liquid water as a function of relative humidity (RH). The amount of water present in the particles prior to deliquescence correlates partially with the water solubilities of the dicarboxylic acids, and also with the relative magnitudes of intermolecular interactions in the internally mixed dry solids. Phase change of ammonium sulfate in the internally mixed particles with RH has been spectrally monitored, and it is shown that water uptaken before full deliquescence produces structural changes in the particles that are revealed by their vibrational spectra. (C) 2013 Elsevier Ltd. All rights reserved.
引用
收藏
页码:108 / 116
页数:9
相关论文
共 39 条
[1]   Interactions of atmospheric trace gases with ice surfaces: Adsorption and reaction [J].
Abbatt, JPD .
CHEMICAL REVIEWS, 2003, 103 (12) :4783-4800
[2]  
[Anonymous], 1997, CRC HDB CHEM PHYS
[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]   Solid/Liquid Phase Diagram of the Ammonium Sulfate/Maleic Acid/Water System [J].
Beyer, Keith D. ;
Schroeder, Jason R. ;
Pearson, Christian S. .
JOURNAL OF PHYSICAL CHEMISTRY A, 2011, 115 (47) :13842-13851
[5]   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
[6]   Phase transitions of malonic and oxalic acid aerosols [J].
Braban, CF ;
Carroll, MF ;
Styler, SA ;
Abbatt, JPD .
JOURNAL OF PHYSICAL CHEMISTRY A, 2003, 107 (34) :6594-6602
[7]   Deliquescence behavior of organic/ammonium sulfate aerosol [J].
Brooks, SD ;
Wise, ME ;
Cushing, M ;
Tolbert, MA .
GEOPHYSICAL RESEARCH LETTERS, 2002, 29 (19) :23-1
[8]  
BROOKS SD, 2003, J GEOPHYS RES, V108, P10
[9]   Measurements of the hygroscopic and deliquescence properties of organic compounds of different solubilities in water and their relationship with cloud condensation nuclei activities [J].
Chan, Man Nin ;
Kreidenweis, Sonia M. ;
Chan, Chak K. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (10) :3602-3608
[10]   The effects of organic species on the hygroscopic behaviors of inorganic aerosols [J].
Choi, MY ;
Chan, CK .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2002, 36 (11) :2422-2428