A global perspective on aerosol from low-volatility organic compounds

被引:209
作者
Pye, H. O. T. [1 ]
Seinfeld, J. H. [1 ]
机构
[1] CALTECH, Dept Chem Engn, Pasadena, CA 91125 USA
基金
美国国家科学基金会;
关键词
CHEMICAL-TRANSPORT MODEL; AIR-POLLUTION SOURCES; CARBONACEOUS AEROSOLS; TROPOSPHERIC CHEMISTRY; AROMATIC-HYDROCARBONS; SEMIVOLATILE ORGANICS; RADIOCARBON ANALYSIS; SOURCE APPORTIONMENT; DRY DEPOSITION; UNITED-STATES;
D O I
10.5194/acp-10-4377-2010
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Global production of organic aerosol from primary emissions of semivolatile (SVOCs) and intermediate (IVOCs) volatility organic compounds is estimated using the global chemical transport model, GEOS-Chem. SVOC oxidation is predicted to be a larger global source of net aerosol production than oxidation of traditional parent hydrocarbons (terpenes, isoprene, and aromatics). Using a prescribed rate constant and reduction in volatility for atmospheric oxidation, the yield of aerosol from SVOCs is predicted to be about 75% on a global, annually-averaged basis. For IVOCs, the use of a naphthalene-like surrogate with different high-NOx and low-NOx parameterizations produces a global aerosol yield of about 30%, or roughly 5 Tg/yr of aerosol. Estimates of the total global organic aerosol source presented here range between 60 and 100 Tg/yr. This range reflects uncertainty in the parameters for SVOC volatility, SVOC oxidation, SVOC emissions, and IVOC emissions, as well as wet deposition. The highest estimates result if SVOC emissions are significantly underestimated (by more than a factor of 2) or if wet deposition of the gas-phase semivolatile species is less effective than previous estimates. A significant increase in SVOC emissions, a reduction of the volatility of the SVOC emissions, or an increase in the enthalpy of vaporization of the organic aerosol all lead to an appreciable reduction of prediction/measurement discrepancy. In addition, if current primary organic aerosol (POA) inventories capture only about one-half of the SVOC emission and the Henrys Law coefficient for oxidized semivolatiles is on the order of 10(3) M/atm, a global estimate of OA production is not inconsistent with the top-down estimate of 140 Tg/yr by (Goldstein and Galbally, 2007). Additional information is needed to constrain the emissions and treatment of SVOCs and IVOCs, which have traditionally not been included in models.
引用
收藏
页码:4377 / 4401
页数:25
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