SOA from limonene: role of NO<sub>3</sub> in its generation and degradation
The formation of organic nitrates and secondary organic aerosol (SOA) were monitored during the NO<sub>3</sub> + limonene reaction in the atmosphere simulation chamber SAPHIR at Research Center Jülich. The 24-h run began in a purged, dry, particle-free chamber and comprised two injection...
| Main Authors: | , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2011-04-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | http://www.atmos-chem-phys.net/11/3879/2011/acp-11-3879-2011.pdf |
| _version_ | 1819160461792247808 |
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| author | R. Tillmann F. Rohrer A. Mensah H. Fuchs H.-P. Dorn W. P. Dubé S. S. Brown T. Brauers A. W. Rollins A. Kiendler-Scharr J. L. Fry A. Wahner P. J. Wooldridge R. C. Cohen |
| author_facet | R. Tillmann F. Rohrer A. Mensah H. Fuchs H.-P. Dorn W. P. Dubé S. S. Brown T. Brauers A. W. Rollins A. Kiendler-Scharr J. L. Fry A. Wahner P. J. Wooldridge R. C. Cohen |
| author_sort | R. Tillmann |
| collection | DOAJ |
| description | The formation of organic nitrates and secondary organic aerosol (SOA) were monitored during the NO<sub>3</sub> + limonene reaction in the atmosphere simulation chamber SAPHIR at Research Center Jülich. The 24-h run began in a purged, dry, particle-free chamber and comprised two injections of limonene and oxidants, such that the first experiment measured SOA yield in the absence of seed aerosol, and the second experiment yields in the presence of 10 μg m<sup>−3</sup> seed organic aerosol. After each injection, two separate increases in aerosol mass were observed, corresponding to sequential oxidation of the two limonene double bonds. Analysis of the measured NO<sub>3</sub>, limonene, product nitrate concentrations, and aerosol properties provides mechanistic insight and constrains rate constants, branching ratios and vapor pressures of the products. The organic nitrate yield from NO<sub>3</sub> + limonene is ≈30%. The SOA mass yield was observed to be 25–40%. The first injection is reproduced by a kinetic model. PMF analysis of the aerosol composition suggests that much of the aerosol mass results from combined oxidation by both O<sub>3</sub> and NO<sub>3</sub>, e.g., oxidation of NO<sub>3</sub> + limonene products by O<sub>3</sub>. Further, later aerosol nitrate mass seems to derive from heterogeneous uptake of NO<sub>3</sub> onto unreacted aerosol alkene. |
| first_indexed | 2024-12-22T16:56:49Z |
| format | Article |
| id | doaj.art-930a7e958f3f49378fbb941979c41634 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-12-22T16:56:49Z |
| publishDate | 2011-04-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-930a7e958f3f49378fbb941979c416342022-12-21T18:19:26ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242011-04-011183879389410.5194/acp-11-3879-2011SOA from limonene: role of NO<sub>3</sub> in its generation and degradationR. TillmannF. RohrerA. MensahH. FuchsH.-P. DornW. P. DubéS. S. BrownT. BrauersA. W. RollinsA. Kiendler-ScharrJ. L. FryA. WahnerP. J. WooldridgeR. C. CohenThe formation of organic nitrates and secondary organic aerosol (SOA) were monitored during the NO<sub>3</sub> + limonene reaction in the atmosphere simulation chamber SAPHIR at Research Center Jülich. The 24-h run began in a purged, dry, particle-free chamber and comprised two injections of limonene and oxidants, such that the first experiment measured SOA yield in the absence of seed aerosol, and the second experiment yields in the presence of 10 μg m<sup>−3</sup> seed organic aerosol. After each injection, two separate increases in aerosol mass were observed, corresponding to sequential oxidation of the two limonene double bonds. Analysis of the measured NO<sub>3</sub>, limonene, product nitrate concentrations, and aerosol properties provides mechanistic insight and constrains rate constants, branching ratios and vapor pressures of the products. The organic nitrate yield from NO<sub>3</sub> + limonene is ≈30%. The SOA mass yield was observed to be 25–40%. The first injection is reproduced by a kinetic model. PMF analysis of the aerosol composition suggests that much of the aerosol mass results from combined oxidation by both O<sub>3</sub> and NO<sub>3</sub>, e.g., oxidation of NO<sub>3</sub> + limonene products by O<sub>3</sub>. Further, later aerosol nitrate mass seems to derive from heterogeneous uptake of NO<sub>3</sub> onto unreacted aerosol alkene.http://www.atmos-chem-phys.net/11/3879/2011/acp-11-3879-2011.pdf |
| spellingShingle | R. Tillmann F. Rohrer A. Mensah H. Fuchs H.-P. Dorn W. P. Dubé S. S. Brown T. Brauers A. W. Rollins A. Kiendler-Scharr J. L. Fry A. Wahner P. J. Wooldridge R. C. Cohen SOA from limonene: role of NO<sub>3</sub> in its generation and degradation Atmospheric Chemistry and Physics |
| title | SOA from limonene: role of NO<sub>3</sub> in its generation and degradation |
| title_full | SOA from limonene: role of NO<sub>3</sub> in its generation and degradation |
| title_fullStr | SOA from limonene: role of NO<sub>3</sub> in its generation and degradation |
| title_full_unstemmed | SOA from limonene: role of NO<sub>3</sub> in its generation and degradation |
| title_short | SOA from limonene: role of NO<sub>3</sub> in its generation and degradation |
| title_sort | soa from limonene role of no sub 3 sub in its generation and degradation |
| url | http://www.atmos-chem-phys.net/11/3879/2011/acp-11-3879-2011.pdf |
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