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DOI10.5194/acp-18-357-2018
Coupling of organic and inorganic aerosol systems and the effect on gas-particle partitioning in the southeastern US
Pye, Havala O. T.1; Zuend, Andreas2; Fry, Juliane L.3; Isaacman-VanWertz, Gabriel4,5; Capps, Shannon L.6; Appel, K. Wyat1; Foroutan, Hosein1,7; Xu, Lu8; Ng, Nga L.9,10; Goldstein, Allen H.5,11
发表日期2018-01-12
ISSN1680-7316
卷号18期号:1页码:357-370
英文摘要

Several models were used to describe the partitioning of ammonia, water, and organic compounds between the gas and particle phases for conditions in the southeastern US during summer 2013. Existing equilibrium models and frameworks were found to be sufficient, although additional improvements in terms of estimating pure-species vapor pressures are needed. Thermodynamic model predictions were consistent, to first order, with a molar ratio of ammonium to sulfate of approximately 1.6 to 1.8 (ratio of ammonium to 2 x sulfate, R-N/2S approximate to 0.8 to 0.9) with approximately 70% of total ammonia and ammonium (NHx) in the particle. Southeastern Aerosol Research and Characterization Network (SEARCH) gas and aerosol and Southern Oxidant and Aerosol Study (SOAS) Monitor for AeRosols and Gases in Ambient air (MARGA) aerosol measurements were consistent with these conditions. CMAQv5.2 regional chemical transport model predictions did not reflect these conditions due to a factor of 3 overestimate of the nonvolatile cations. In addition, gas-phase ammonia was overestimated in the CMAQ model leading to an even lower fraction of total ammonia in the particle. Chemical Speciation Network (CSN) and aerosol mass spectrometer (AMS) measurements indicated less ammonium per sulfate than SEARCH and MARGA measurements and were inconsistent with thermodynamic model predictions. Organic compounds were predicted to be present to some extent in the same phase as inorganic constituents, modifying their activity and resulting in a decrease in [H+](air) (H+ in mu g m(-3) air), increase in ammonia partitioning to the gas phase, and increase in pH compared to complete organic vs. inorganic liquid-liquid phase separation. In addition, accounting for nonideal mixing modified the pH such that a fully interactive inorganic-organic system had a pH roughly 0.7 units higher than predicted using traditional methods (pH = 1.5 vs. 0.7). Particle-phase interactions of organic and inorganic compounds were found to increase partitioning towards the particle phase (vs. gas phase) for highly oxygenated (O : C >= 0.6) compounds including several isoprene-derived tracers as well as levoglucosan but decrease particle-phase partitioning for low O : C, monoterpene-derived species.


语种英语
WOS记录号WOS:000419987100002
来源期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
来源机构美国环保署
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/61696
作者单位1.US EPA, Natl Exposure Res Lab, Res Triangle Pk, NC 27709 USA;
2.McGill Univ, Dept Atmospher & Ocean Sci, Montreal, PQ, Canada;
3.Reed Coll, Dept Chem, Portland, OR 97202 USA;
4.Virginia Polytech Inst & State Univ, Dept Civil & Environm Engn, Blacksburg, VA 24061 USA;
5.Univ Calif Berkeley, Dept Environm Sci Policy & Management, Berkeley, CA 94720 USA;
6.Drexel Univ, Civil Architectural & Environm Engn, Philadelphia, PA 19104 USA;
7.Virginia Polytech Inst & State Univ, Dept Biomed Engn & Mech, Blacksburg, VA 24061 USA;
8.CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91125 USA;
9.Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA;
10.Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA;
11.Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USA
推荐引用方式
GB/T 7714
Pye, Havala O. T.,Zuend, Andreas,Fry, Juliane L.,et al. Coupling of organic and inorganic aerosol systems and the effect on gas-particle partitioning in the southeastern US[J]. 美国环保署,2018,18(1):357-370.
APA Pye, Havala O. T..,Zuend, Andreas.,Fry, Juliane L..,Isaacman-VanWertz, Gabriel.,Capps, Shannon L..,...&Goldstein, Allen H..(2018).Coupling of organic and inorganic aerosol systems and the effect on gas-particle partitioning in the southeastern US.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(1),357-370.
MLA Pye, Havala O. T.,et al."Coupling of organic and inorganic aerosol systems and the effect on gas-particle partitioning in the southeastern US".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.1(2018):357-370.
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