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DOI | 10.5194/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 |
ISSN | 1680-7316 |
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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