Atmospheric aerosol models for systems including the ions H+, NH4+, Na+, SO42-, NO3-,Cl-, Br-, and H2O -: art. no. 4207

被引:411
作者
Wexler, AS
Clegg, SL
机构
[1] Univ Calif Davis, Dept Mech & Aeronaut Engn, Davis, CA 95616 USA
[2] Univ Calif Davis, Dept Civil & Environm Engn, Davis, CA 95616 USA
[3] Univ Calif Davis, Dept Land Air & Water Resources, Davis, CA 95616 USA
[4] Univ E Anglia, Sch Environm Sci, Norwich NR4 7TJ, Norfolk, England
关键词
aerosols; thermodynamics; Henry's law; phase equilibrium; Gibbs energy;
D O I
10.1029/2001JD000451
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] Mole fraction based equations for aqueous phase activities, together with equilibrium constants for the formation of gases and solids, have been combined with a Gibbs free energy minimization algorithm to create equilibrium phase partitioning models of inorganic atmospheric aerosols. The water content, phase state (solid or liquid), and gas/aerosol partitioning are predicted for known ionic composition, relative humidity, and temperature. The models are valid from <200 to 328 K for the subsystems (H+-SO42-NO3- -Cl- -Br- -H2O) and (H+ -NH4+-SO42--NO3- -H2O), and 298.15 K only for (H+-NH4+ Na+ -SO42--NO3--Cl- -H2O). The models involve no simplifying assumptions and include all solid phases identified in bulk experiments, including hydrated and double salt forms not treated in most other studies. The Henry's law constant of H2SO4 is derived as a function of temperature, based upon available data, and the model treatment of the solubility of HBr in aqueous H2SO4 is revised. Phase diagrams are calculated for the (NH4)(2)SO4/H2SO4/H2O system to low temperature. The models are also used to explore the importance of the double salts in urban inorganic aerosols. These Aerosol Inorganics Model (AIM) models can be run on the Web for a variety of problem types at http:// mae.ucdavis.edu/wexler/aim.htmlandhttp://www.uea. ac. uk/similar toe770/ aim. html, and their use is summarized here.
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共 45 条
[1]   Prediction of multicomponent inorganic atmospheric aerosol behavior [J].
Ansari, AS ;
Pandis, SN .
ATMOSPHERIC ENVIRONMENT, 1999, 33 (05) :745-757
[2]   ON THE VAPOR-PRESSURE OF SULFURIC-ACID [J].
AYERS, GP ;
GILLETT, RW ;
GRAS, JL .
GEOPHYSICAL RESEARCH LETTERS, 1980, 7 (06) :433-436
[3]   ATMOSPHERIC EQUILIBRIUM-MODEL OF SULFATE AND NITRATE AEROSOLS [J].
BASSETT, M ;
SEINFELD, JH .
ATMOSPHERIC ENVIRONMENT, 1983, 17 (11) :2237-2252
[4]   THERMODYNAMIC ACTIVITIES AND EQUILIBRIUM PARTIAL PRESSURES FOR AQUEOUS SULFURIC-ACID-SOLUTIONS [J].
BOLSAITIS, P ;
ELLIOTT, JF .
JOURNAL OF CHEMICAL AND ENGINEERING DATA, 1990, 35 (01) :69-85
[5]   A THERMODYNAMIC MODEL OF THE SYSTEM HCL-HNO3-H2SO4-H2O, INCLUDING SOLUBILITIES OF HBR, FROM LESS-THAN-200 TO 328 K [J].
CARSLAW, KS ;
CLEGG, SL ;
BRIMBLECOMBE, P .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (29) :11557-11574
[6]   Water activity and equilibrium freezing temperatures of aqueous NH4HSO4 solutions from-30 to 25°C [J].
Chelf, JH ;
Martin, ST .
GEOPHYSICAL RESEARCH LETTERS, 1999, 26 (15) :2391-2394
[7]  
Clegg S. L., 1998, J PHYS CHEM A, V102, P2127
[8]   Thermodynamic model of the system H+-NH4+-Na+-SO42--NB3--Cl--H2O at 298.15 K [J].
Clegg, SL ;
Brimblecombe, P ;
Wexler, AS .
JOURNAL OF PHYSICAL CHEMISTRY A, 1998, 102 (12) :2155-2171
[9]   APPLICATION OF A MULTICOMPONENT THERMODYNAMIC MODEL TO ACTIVITIES AND THERMAL-PROPERTIES OF 0-40-MOL KG(-1) AQUEOUS SULFURIC-ACID FROM LESS-THAN-200-K TO 328-K [J].
CLEGG, SL ;
BRIMBLECOMBE, P .
JOURNAL OF CHEMICAL AND ENGINEERING DATA, 1995, 40 (01) :43-64
[10]   CORRECTION [J].
CLEGG, SL .
JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (16) :6854-6854