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DOI | 10.1029/2018JD028786 |
Wintertime Gas-Particle Partitioning and Speciation of Inorganic Chlorine in the Lower Troposphere Over the Northeast United States and Coastal Ocean | |
Haskins, Jessica D.1; Jaegle, Lyatt1; Shah, Viral1; Lee, Ben H.1; Lopez-Hilfiker, Felipe D.1,2; Campuzano-Jost, Pedro3,4; Schroder, Jason C.3,4; Day, Douglas A.3,4; Guo, Hongyu5; Sullivan, Amy P.6; Weber, Rodney5; Dibb, Jack7; Campos, Teresa8; Jimenez, Jose L.3,4; Brown, Steven S.9; Thornton, Joel A.1 | |
2018-12-13 | |
发表期刊 | JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES |
ISSN | 2169-897X |
EISSN | 2169-8996 |
出版年 | 2018 |
卷号 | 123期号:22页码:12897-12916 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Switzerland |
英文摘要 | The formation of photolabile chlorine reservoirs depend on how much chloride is available in the particle to react, which requires the chlorine partitioning to the particle in the troposphere to be well understood. However, limited measurements of gas and particle composition necessary to constrain this chemistry exist. We present measurements from the Wintertime Investigation of Transport, Emissions, and Reactivity (WINTER) aircraft campaign that show inorganic tropospheric chlorine compounds (Cl-y) measured in the lower troposphere are dominated by HCl and PM4 particulate chloride (pCl(-)), with contributions from trace chlorine species like nitryl chloride (ClNO2), hypochlorous acid (HOCl), and molecular chlorine (Cl-2). We observed elevated Cly mixing ratios over the ocean (540-625 pptv) compared to over land (178-225 pptv). Observations show 0-20% (0-0.2 mu g/m(3)) of measured chlorine partitions into particles with a diameter less than 1 mu m under typical WINTER conditions. The thermodynamic model, ISORROPIA II, overpredicts submicron pCl(-) by a factor of 2 but is brought into agreement, assuming a small fraction of unmeasured, refractory sea salt <0.1 mu g/m(3) exists. The model-measurement disagreement could also be caused by an effective equilibrium constant for HCl that is too large. We derive a lower-limit equilibrium function (Keq = 2.5 x 10(6) exp[5,208(1/T - 1/T-0)] mol(2).kg(-2).atm(-1)) that lowers the model value's temperature dependency. This work provides constraints on Cly in the troposphere, addresses the sensitivity of chlorine partitioning to minor changes in environmental variables, and highlights the remaining questions interfering with our ability to correctly model pCl(-) concentrations. |
领域 | 气候变化 |
收录类别 | SCI-E |
WOS记录号 | WOS:000452994100024 |
WOS关键词 | IONIZATION MASS-SPECTROMETER ; NITRYL CHLORIDE ; THERMODYNAMIC MODEL ; HIGH-RESOLUTION ; GASEOUS N2O5 ; AEROSOL ; CLNO2 ; CHEMISTRY ; WATER ; CL-2 |
WOS类目 | Meteorology & Atmospheric Sciences |
WOS研究方向 | 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/34077 |
专题 | 气候变化 |
作者单位 | 1.Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA; 2.Paul Scherrer Inst, Lab Atmospher Chem, Villigen, Switzerland; 3.Univ Colorado, Dept Chem, Boulder, CO 80309 USA; 4.Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA; 5.Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA; 6.Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA; 7.Univ New Hampshire, Inst Study Earth Oceans & Space, Durham, NH 03824 USA; 8.Natl Ctr Atmospher Res, POB 3000, Boulder, CO 80307 USA; 9.NOAA, Div Chem Sci, Earth Syst Res Lab, Boulder, CO USA |
推荐引用方式 GB/T 7714 | Haskins, Jessica D.,Jaegle, Lyatt,Shah, Viral,et al. Wintertime Gas-Particle Partitioning and Speciation of Inorganic Chlorine in the Lower Troposphere Over the Northeast United States and Coastal Ocean[J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES,2018,123(22):12897-12916. |
APA | Haskins, Jessica D..,Jaegle, Lyatt.,Shah, Viral.,Lee, Ben H..,Lopez-Hilfiker, Felipe D..,...&Thornton, Joel A..(2018).Wintertime Gas-Particle Partitioning and Speciation of Inorganic Chlorine in the Lower Troposphere Over the Northeast United States and Coastal Ocean.JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES,123(22),12897-12916. |
MLA | Haskins, Jessica D.,et al."Wintertime Gas-Particle Partitioning and Speciation of Inorganic Chlorine in the Lower Troposphere Over the Northeast United States and Coastal Ocean".JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES 123.22(2018):12897-12916. |
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