Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limonene
Anthropogenic emissions such as NO<sub><i>x</i></sub> and SO<sub>2</sub> influence the biogenic secondary organic aerosol (SOA) formation, but detailed mechanisms and effects are still elusive. We studied the effects of NO<sub><i>x</i></sub&...
| Main Authors: | , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2018-02-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://www.atmos-chem-phys.net/18/1611/2018/acp-18-1611-2018.pdf |
| _version_ | 1818139323856322560 |
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| author | D. Zhao S. H. Schmitt M. Wang M. Wang I.-H. Acir I.-H. Acir R. Tillmann Z. Tan Z. Tan A. Novelli H. Fuchs I. Pullinen I. Pullinen R. Wegener F. Rohrer J. Wildt A. Kiendler-Scharr A. Wahner T. F. Mentel |
| author_facet | D. Zhao S. H. Schmitt M. Wang M. Wang I.-H. Acir I.-H. Acir R. Tillmann Z. Tan Z. Tan A. Novelli H. Fuchs I. Pullinen I. Pullinen R. Wegener F. Rohrer J. Wildt A. Kiendler-Scharr A. Wahner T. F. Mentel |
| author_sort | D. Zhao |
| collection | DOAJ |
| description | Anthropogenic emissions such as NO<sub><i>x</i></sub> and SO<sub>2</sub> influence the biogenic
secondary organic aerosol (SOA) formation, but detailed mechanisms and
effects are still elusive. We studied the effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on
the SOA formation from the photooxidation of <i>α</i>-pinene and limonene at
ambient relevant NO<sub><i>x</i></sub> and SO<sub>2</sub> concentrations (NO<sub><i>x</i></sub>: < 1to 20 ppb, SO<sub>2</sub>: < 0.05 to 15 ppb). In these experiments,
monoterpene oxidation was dominated by OH oxidation. We found that SO<sub>2</sub>
induced nucleation and enhanced SOA mass formation. NO<sub><i>x</i></sub> strongly
suppressed not only new particle formation but also SOA mass yield. However,
in the presence of SO<sub>2</sub> which induced a high number concentration of
particles after oxidation to H<sub>2</sub>SO<sub>4</sub>, the suppression of the mass
yield of SOA by NO<sub><i>x</i></sub> was completely or partly compensated for. This indicates
that the suppression of SOA yield by NO<sub><i>x</i></sub> 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 NO<sub><i>x</i></sub>, SO<sub>2</sub> also compensated for the suppressing effect
on SOA yield. Aerosol mass spectrometer data show that increasing NO<sub><i>x</i></sub>
enhanced nitrate formation. The majority of the nitrate was organic nitrate
(57–77 %), even in low-NO<sub><i>x</i></sub> conditions (< ∼ 1 ppb). Organic nitrate contributed 7–26 % of total organics assuming a
molecular weight of 200 g mol<sup>−1</sup>. SOA from <i>α</i>-pinene photooxidation at
high NO<sub><i>x</i></sub> had a generally lower hydrogen to carbon ratio (H ∕ C), compared to
low NO<sub><i>x</i></sub>. The NO<sub><i>x</i></sub> dependence of the chemical composition can be
attributed to the NO<sub><i>x</i></sub> dependence of the branching ratio of the RO<sub>2</sub>
loss reactions, leading to a lower fraction of organic hydroperoxides and
higher fractions of organic nitrates at high NO<sub><i>x</i></sub>. While NO<sub><i>x</i></sub>
suppressed new particle formation and SOA mass formation, SO<sub>2</sub> can
compensate for such effects, and the combining effect of SO<sub>2</sub> and
NO<sub><i>x</i></sub> may have an important influence on SOA formation affected by
interactions of biogenic volatile organic compounds (VOCs) with anthropogenic
emissions. |
| first_indexed | 2024-12-11T10:26:16Z |
| format | Article |
| id | doaj.art-487d02d5eda34525828259bcd869ae6d |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-12-11T10:26:16Z |
| publishDate | 2018-02-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-487d02d5eda34525828259bcd869ae6d2022-12-22T01:11:09ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242018-02-01181611162810.5194/acp-18-1611-2018Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limoneneD. Zhao0S. H. Schmitt1M. Wang2M. Wang3I.-H. Acir4I.-H. Acir5R. Tillmann6Z. Tan7Z. Tan8A. Novelli9H. Fuchs10I. Pullinen11I. Pullinen12R. Wegener13F. Rohrer14J. Wildt15A. Kiendler-Scharr16A. Wahner17T. F. Mentel18Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyCollege of Environmental Science and Engineering, Peking University, Beijing, 100871, ChinaInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, Germanynow at: Institute of Nutrition and Food Sciences, University of Bonn, 53115 Bonn, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyCollege of Environmental Science and Engineering, Peking University, Beijing, 100871, ChinaInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, Germanynow at: Department of Applied Physics, University of Eastern Finland, 7021 Kuopio, FinlandInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyInstitute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich, 52425 Jülich, GermanyAnthropogenic emissions such as NO<sub><i>x</i></sub> and SO<sub>2</sub> influence the biogenic secondary organic aerosol (SOA) formation, but detailed mechanisms and effects are still elusive. We studied the effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the SOA formation from the photooxidation of <i>α</i>-pinene and limonene at ambient relevant NO<sub><i>x</i></sub> and SO<sub>2</sub> concentrations (NO<sub><i>x</i></sub>: < 1to 20 ppb, SO<sub>2</sub>: < 0.05 to 15 ppb). In these experiments, monoterpene oxidation was dominated by OH oxidation. We found that SO<sub>2</sub> induced nucleation and enhanced SOA mass formation. NO<sub><i>x</i></sub> strongly suppressed not only new particle formation but also SOA mass yield. However, in the presence of SO<sub>2</sub> which induced a high number concentration of particles after oxidation to H<sub>2</sub>SO<sub>4</sub>, the suppression of the mass yield of SOA by NO<sub><i>x</i></sub> was completely or partly compensated for. This indicates that the suppression of SOA yield by NO<sub><i>x</i></sub> 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 NO<sub><i>x</i></sub>, SO<sub>2</sub> also compensated for the suppressing effect on SOA yield. Aerosol mass spectrometer data show that increasing NO<sub><i>x</i></sub> enhanced nitrate formation. The majority of the nitrate was organic nitrate (57–77 %), even in low-NO<sub><i>x</i></sub> conditions (< ∼ 1 ppb). Organic nitrate contributed 7–26 % of total organics assuming a molecular weight of 200 g mol<sup>−1</sup>. SOA from <i>α</i>-pinene photooxidation at high NO<sub><i>x</i></sub> had a generally lower hydrogen to carbon ratio (H ∕ C), compared to low NO<sub><i>x</i></sub>. The NO<sub><i>x</i></sub> dependence of the chemical composition can be attributed to the NO<sub><i>x</i></sub> dependence of the branching ratio of the RO<sub>2</sub> loss reactions, leading to a lower fraction of organic hydroperoxides and higher fractions of organic nitrates at high NO<sub><i>x</i></sub>. While NO<sub><i>x</i></sub> suppressed new particle formation and SOA mass formation, SO<sub>2</sub> can compensate for such effects, and the combining effect of SO<sub>2</sub> and NO<sub><i>x</i></sub> may have an important influence on SOA formation affected by interactions of biogenic volatile organic compounds (VOCs) with anthropogenic emissions.https://www.atmos-chem-phys.net/18/1611/2018/acp-18-1611-2018.pdf |
| spellingShingle | D. Zhao S. H. Schmitt M. Wang M. Wang I.-H. Acir I.-H. Acir R. Tillmann Z. Tan Z. Tan A. Novelli H. Fuchs I. Pullinen I. Pullinen R. Wegener F. Rohrer J. Wildt A. Kiendler-Scharr A. Wahner T. F. Mentel Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limonene Atmospheric Chemistry and Physics |
| title | Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limonene |
| title_full | Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limonene |
| title_fullStr | Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limonene |
| title_full_unstemmed | Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limonene |
| title_short | Effects of NO<sub><i>x</i></sub> and SO<sub>2</sub> on the secondary organic aerosol formation from photooxidation of <i>α</i>-pinene and limonene |
| title_sort | effects of no sub i x i sub and so sub 2 sub on the secondary organic aerosol formation from photooxidation of i α i pinene and limonene |
| url | https://www.atmos-chem-phys.net/18/1611/2018/acp-18-1611-2018.pdf |
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