A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics

被引:510
作者
Donahue, N. M. [1 ]
Epstein, S. A. [1 ]
Pandis, S. N. [1 ]
Robinson, A. L. [1 ]
机构
[1] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA
关键词
AIR-QUALITY MODEL; ATMOSPHERIC PARTICULATE MATTER; ACTIVITY-COEFFICIENT MODELS; VAPOR-PRESSURES; EVAPORATION RATES; SOURCE APPORTIONMENT; DICARBOXYLIC-ACIDS; ALPHA-PINENE; SEMIVOLATILE ORGANICS; GAS-CHROMATOGRAPHY;
D O I
10.5194/acp-11-3303-2011
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
We develop the thermodynamic underpinnings of a two-dimensional volatility basis set (2D-VBS) employing saturation mass concentration (C-o) and the oxygen content (O:C) to describe volatility, mixing thermodynamics, and chemical evolution of organic aerosol. The work addresses a simple question: "Can we reasonably constrain organic-aerosol composition in the atmosphere based on only two measurable organic properties, volatility and the extent of oxygenation?" This is an extension of our earlier one-dimensional approach employing volatility only (C* = gamma C-o, where gamma is an activity coefficient). Using available constraints on bulk organic-aerosol composition, we argue that one can reasonably predict the composition of organics (carbon, oxygen and hydrogen numbers) given a location in the C-o - space. Further, we argue that we can constrain the activity coefficients at various locations in this space based on the O:C of the organic aerosol.
引用
收藏
页码:3303 / 3318
页数:16
相关论文
共 83 条
[21]   IN-SITU NONMETHANE HYDROCARBON MEASUREMENTS ON SAGA-3 [J].
DONAHUE, NM ;
PRINN, RG .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1993, 98 (D9) :16915-16932
[22]   Coupled partitioning, dilution, and chemical aging of semivolatile organics [J].
Donahue, NM ;
Robinson, AL ;
Stanier, CO ;
Pandis, SN .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (08) :2635-2643
[23]   A Semiempirical Correlation between Enthalpy of Vaporization and Saturation Concentration for Organic Aerosol [J].
Epstein, Scott A. ;
Riipinen, Ilona ;
Donahue, Neil M. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (02) :743-748
[24]   Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry [J].
Farmer, D. K. ;
Matsunaga, A. ;
Docherty, K. S. ;
Surratt, J. D. ;
Seinfeld, J. H. ;
Ziemann, P. J. ;
Jimenez, J. L. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2010, 107 (15) :6670-6675
[25]   Air quality model evaluation data for organics .4. C-2-C-36 non-aromatic hydrocarbons [J].
Fraser, MP ;
Cass, GR ;
Simoneit, BRT ;
Rasmussen, RA .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1997, 31 (08) :2356-2367
[26]   Air quality model evaluation data for organics.: 5.: C6-C22 nonpolar and semipolar aromatic compounds [J].
Fraser, MP ;
Cass, GR ;
Simoneit, BRT ;
Rasmussen, RA .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1998, 32 (12) :1760-1770
[27]   GROUP-CONTRIBUTION ESTIMATION OF ACTIVITY-COEFFICIENTS IN NONIDEAL LIQUID-MIXTURES [J].
FREDENSLUND, A ;
JONES, RL ;
PRAUSNITZ, JM .
AICHE JOURNAL, 1975, 21 (06) :1086-1099
[28]   Glyoxal uptake on ammonium sulphate seed aerosol: reaction products and reversibility of uptake under dark and irradiated conditions [J].
Galloway, M. M. ;
Chhabra, P. S. ;
Chan, A. W. H. ;
Surratt, J. D. ;
Flagan, R. C. ;
Seinfeld, J. H. ;
Keutsch, F. N. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (10) :3331-3345
[29]   Thermal desorption comprehensive two-dimensional gas chromatography for in-situ measurements of organic aerosols [J].
Goldstein, Allen H. ;
Worton, David R. ;
Williams, Brent J. ;
Hering, Susanne V. ;
Kreisberg, Nathan M. ;
Panic, Ognjen ;
Gorecki, Tadeusz .
JOURNAL OF CHROMATOGRAPHY A, 2008, 1186 (1-2) :340-347
[30]   Constraining the Volatility Distribution and Gas-Particle Partitioning of Combustion Aerosols Using Isothermal Dilution and Thermodenuder Measurements [J].
Grieshop, Andrew P. ;
Miracolo, Marissa A. ;
Donahue, Neil. M. ;
Robinson, Allen L. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2009, 43 (13) :4750-4756