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DOI | 10.5194/acp-18-1611-2018 |
Effects of NOx and SO2 on the secondary organic aerosol formation from photooxidation of alpha-pinene and limonene | |
Zhao, Defeng1; Schmitt, Sebastian H.1; Wang, Mingjin1,2; Acir, Ismail-Hakki1,3; Tillmann, Ralf1; Tan, Zhaofeng1,2; Novelli, Anna1; Fuchs, Hendrik1; Pullinen, Iida1,4; Wegener, Robert1; Rohrer, Franz1; Wildt, Juergen1; Kiendler-Scharr, Astrid1; Wahner, Andreas1; Mentel, Thomas F.1 | |
2018-02-05 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:3页码:1611-1628 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany; Peoples R China; Finland |
英文摘要 | Anthropogenic emissions such as NOx and SO2 influence the biogenic secondary organic aerosol (SOA) formation, but detailed mechanisms and effects are still elusive. We studied the effects of NOx and SO2 on the SOA formation from the photooxidation of alpha-pinene and limonene at ambient relevant NOx and SO2 concentrations (NOx: < 1 to 20 ppb, SO2: < 0.05 to 15 ppb). In these experiments, monoterpene oxidation was dominated by OH oxidation. We found that SO2 induced nucleation and enhanced SOA mass formation. NOx strongly suppressed not only new particle formation but also SOA mass yield. However, in the presence of SO2 which induced a high number concentration of particles after oxidation to H2SO4, the suppression of the mass yield of SOA by NOx was completely or partly compensated for. This indicates that the suppression of SOA yield by NOx was largely due to the suppressed new particle formation, leading to a lack of particle surface for the organics to condense on and thus a significant influence of vapor wall loss on SOA mass yield. By compensating for the suppressing effect on nucleation of NOx, SO2 also compensated for the suppressing effect on SOA yield. Aerosol mass spectrometer data show that increasing NOx enhanced nitrate formation. The majority of the nitrate was organic nitrate (57-77 %), even in low-NOx conditions (< similar to 1 ppb). Organic nitrate contributed 7-26% of total organics assuming a molecular weight of 200 g mol(-1). SOA from alpha-pinene photooxidation at high NOx had a generally lower hydrogen to carbon ratio (H / C), compared to low NOx. The NOx dependence of the chemical composition can be attributed to the NOx dependence of the branching ratio of the RO2 loss reactions, leading to a lower fraction of organic hydroperoxides and higher fractions of organic nitrates at high NOx. While NOx suppressed new particle formation and SOA mass formation, SO2 can compensate for such effects, and the combining effect of SO2 and NOx may have an important influence on SOA formation affected by interactions of biogenic volatile organic compounds (VOCs) with anthropogenic emissions. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000424122600003 |
WOS关键词 | VAPOR WALL LOSS ; CONTROLLED CHEMICAL CONDITIONS ; GAS-PHASE REACTIONS ; SULFURIC-ACID ; BETA-PINENE ; TROPOSPHERIC DEGRADATION ; PHOTOLYSIS FREQUENCIES ; ATMOSPHERIC CHEMISTRY ; CHAMBER EXPERIMENTS ; HYGROSCOPIC GROWTH |
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/27328 |
专题 | 地球科学 |
作者单位 | 1.Forschungszentrum Julich, IEK Troposphere 8, Inst Energy & Climate Res, D-52425 Julich, Germany; 2.Peking Univ, Coll Environm Sci & Engn, Beijing 100871, Peoples R China; 3.Univ Bonn, Inst Nutr & Food Sci, D-53115 Bonn, Germany; 4.Univ Eastern Finland, Dept Appl Phys, Kuopio 7021, Finland |
推荐引用方式 GB/T 7714 | Zhao, Defeng,Schmitt, Sebastian H.,Wang, Mingjin,et al. Effects of NOx and SO2 on the secondary organic aerosol formation from photooxidation of alpha-pinene and limonene[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(3):1611-1628. |
APA | Zhao, Defeng.,Schmitt, Sebastian H..,Wang, Mingjin.,Acir, Ismail-Hakki.,Tillmann, Ralf.,...&Mentel, Thomas F..(2018).Effects of NOx and SO2 on the secondary organic aerosol formation from photooxidation of alpha-pinene and limonene.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(3),1611-1628. |
MLA | Zhao, Defeng,et al."Effects of NOx and SO2 on the secondary organic aerosol formation from photooxidation of alpha-pinene and limonene".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.3(2018):1611-1628. |
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