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DOI | 10.5194/acp-17-7529-2017 |
Uncertain Henry's law constants compromise equilibrium partitioning calculations of atmospheric oxidation products | |
Wang, Chen1; Yuan, Tiange1; Wood, Stephen A.1; Goss, Kai-Uwe2,3; Li, Jingyi4,5; Ying, Qi4; Wania, Frank1 | |
2017-06-22 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2017 |
卷号 | 17期号:12 |
文章类型 | Article |
语种 | 英语 |
国家 | Canada; Germany; USA; Peoples R China |
英文摘要 | Gas-particle partitioning governs the distribution, removal, and transport of organic compounds in the atmosphere and the formation of secondary organic aerosol (SOA). The large variety of atmospheric species and their wide range of properties make predicting this partitioning equilibrium challenging. Here we expand on earlier work and predict gas-organic and gas-aqueous phase partitioning coefficients for 3414 atmospherically relevant molecules using COSMOtherm, SPARC Performs Automated Reasoning in Chemistry (SPARC), and poly-parameter linear free-energy relationships. The Master Chemical Mechanism generated the structures by oxidizing primary emitted volatile organic compounds. Predictions for gas-organic phase partitioning coefficients (K-WIOM/G) by different methods are on average within 1 order of magnitude of each other, irrespective of the numbers of functional groups, except for predictions by COSMOtherm and SPARC for compounds with more than three functional groups, which have a slightly higher discrepancy. Discrepancies between predictions of gas-aqueous partitioning (K-W/G) are much larger and increase with the number of functional groups in the molecule. In particular, COSMOtherm often predicts much lower K-W/G for highly functionalized compounds than the other methods. While the quantum-chemistry-based COSMOtherm accounts for the influence of intra-molecular interactions on conformation, highly functionalized molecules likely fall outside of the applicability domain of the other techniques, which at least in part rely on empirical data for calibration. Further analysis suggests that atmospheric phase distribution calculations are sensitive to the partitioning coefficient estimation method, in particular to the estimated value of K-W/G. The large uncertainty in K-W/G predictions for highly functionalized organic compounds needs to be resolved to improve the quantitative treatment of SOA formation. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000404049500001 |
WOS关键词 | SECONDARY ORGANIC AEROSOL ; VAPOR-PRESSURE ESTIMATION ; FREE-ENERGY RELATIONSHIPS ; PHASE DISTRIBUTION ; AQUEOUS-PHASE ; COSMO-RS ; PREDICTION ; SULFATE ; COEFFICIENT ; TEMPERATURE |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/30439 |
专题 | 地球科学 |
作者单位 | 1.Univ Toronto Scarborough, Dept Phys & Environm Sci, 1265 Mil Trail, Toronto, ON M1C 1A4, Canada; 2.Ctr Environm Res UFZ Leipzig Halle, Dept Analyt Environm Chem, Permoserstr 15, D-04318 Leipzig, Germany; 3.Univ Halle Wittenberg, Inst Chem, Kurt Mothes Str 2, D-06120 Halle, Germany; 4.Texas A&M Univ, Zachry Dept Civil Engn, Environm & Water Resources Div, College Stn, TX 77843 USA; 5.Nanjing Univ Informat Sci & Technol, Sch Environm Sci & Engn, 219 Ningliu Rd, Nanjing 210044, Jiangsu, Peoples R China |
推荐引用方式 GB/T 7714 | Wang, Chen,Yuan, Tiange,Wood, Stephen A.,et al. Uncertain Henry's law constants compromise equilibrium partitioning calculations of atmospheric oxidation products[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2017,17(12). |
APA | Wang, Chen.,Yuan, Tiange.,Wood, Stephen A..,Goss, Kai-Uwe.,Li, Jingyi.,...&Wania, Frank.(2017).Uncertain Henry's law constants compromise equilibrium partitioning calculations of atmospheric oxidation products.ATMOSPHERIC CHEMISTRY AND PHYSICS,17(12). |
MLA | Wang, Chen,et al."Uncertain Henry's law constants compromise equilibrium partitioning calculations of atmospheric oxidation products".ATMOSPHERIC CHEMISTRY AND PHYSICS 17.12(2017). |
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