Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub>
Sulfur dioxide (SO<sub>2</sub>) can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs), but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline ve...
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2016-01-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://www.atmos-chem-phys.net/16/675/2016/acp-16-675-2016.pdf |
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doaj-e5842d739cfb46cfa49827abc672c2a7 |
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Article |
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DOAJ |
| language |
English |
| format |
Article |
| sources |
DOAJ |
| author |
T. Liu T. Liu X. Wang Q. Hu W. Deng W. Deng Y. Zhang X. Ding X. Fu X. Fu F. Bernard F. Bernard Z. Zhang Z. Zhang S. Lü S. Lü Q. He Q. He X. Bi J. Chen Y. Sun J. Yu P. Peng G. Sheng J. Fu |
| spellingShingle |
T. Liu T. Liu X. Wang Q. Hu W. Deng W. Deng Y. Zhang X. Ding X. Fu X. Fu F. Bernard F. Bernard Z. Zhang Z. Zhang S. Lü S. Lü Q. He Q. He X. Bi J. Chen Y. Sun J. Yu P. Peng G. Sheng J. Fu Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub> Atmospheric Chemistry and Physics |
| author_facet |
T. Liu T. Liu X. Wang Q. Hu W. Deng W. Deng Y. Zhang X. Ding X. Fu X. Fu F. Bernard F. Bernard Z. Zhang Z. Zhang S. Lü S. Lü Q. He Q. He X. Bi J. Chen Y. Sun J. Yu P. Peng G. Sheng J. Fu |
| author_sort |
T. Liu |
| title |
Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub> |
| title_short |
Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub> |
| title_full |
Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub> |
| title_fullStr |
Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub> |
| title_full_unstemmed |
Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub> |
| title_sort |
formation of secondary aerosols from gasoline vehicle exhaust when mixing with so<sub>2</sub> |
| publisher |
Copernicus Publications |
| series |
Atmospheric Chemistry and Physics |
| issn |
1680-7316 1680-7324 |
| publishDate |
2016-01-01 |
| description |
Sulfur dioxide (SO<sub>2</sub>) can enhance the formation of secondary aerosols
from biogenic volatile organic compounds (VOCs), but its influence on
secondary aerosol formation from anthropogenic VOCs, particularly complex
mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust
(GVE) and SO<sub>2</sub>, a typical pollutant from coal burning, are directly
co-introduced into a smog chamber, in this study, to investigate the
formation of secondary organic aerosols (SOA) and sulfate aerosols through
photooxidation. New particle formation was enhanced, while substantial
sulfate was formed through the oxidation of SO<sub>2</sub> in the presence of high concentration of SO<sub>2</sub>. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO<sub>2</sub> to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs), formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO<sub>2</sub>. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60–200 % in the presence of high concentration of SO<sub>2</sub>. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (<i>R</i><sup>2</sup> = 0.97) between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) resolved OA's relatively lower oxygen-to-carbon (O : C) (0.44 ± 0.02) and higher hydrogen-to-carbon (H : C) (1.40 ± 0.03) molar ratios for the GVE / SO<sub>2</sub> mixture, with a significantly lower estimated average carbon oxidation state (OS<sub>c</sub>) of −0.51 ± 0.06 than −0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO<sub>2</sub> might be a significant explanation for the lower SOA oxidation degree. |
| url |
https://www.atmos-chem-phys.net/16/675/2016/acp-16-675-2016.pdf |
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doaj-e5842d739cfb46cfa49827abc672c2a72020-11-24T20:40:22ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-01-011667568910.5194/acp-16-675-2016Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO<sub>2</sub>T. Liu0T. Liu1X. Wang2Q. Hu3W. Deng4W. Deng5Y. Zhang6X. Ding7X. Fu8X. Fu9F. Bernard10F. Bernard11Z. Zhang12Z. Zhang13S. Lü14S. Lü15Q. He16Q. He17X. Bi18J. Chen19Y. Sun20J. Yu21P. Peng22G. Sheng23J. Fu24State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaChemical Sciences Division, NOAA Earth System Research Laboratory, Boulder, Colorado 80305, USAState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaUniversity of Chinese Academy of Sciences, Beijing 100049, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaShanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, ChinaInstitute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, ChinaDivision of Environment, Hong Kong University of Science & Technology, Clear Water Bay, Kowloon, Hong Kong, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaState Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaSulfur dioxide (SO<sub>2</sub>) can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs), but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust (GVE) and SO<sub>2</sub>, a typical pollutant from coal burning, are directly co-introduced into a smog chamber, in this study, to investigate the formation of secondary organic aerosols (SOA) and sulfate aerosols through photooxidation. New particle formation was enhanced, while substantial sulfate was formed through the oxidation of SO<sub>2</sub> in the presence of high concentration of SO<sub>2</sub>. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO<sub>2</sub> to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs), formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO<sub>2</sub>. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60–200 % in the presence of high concentration of SO<sub>2</sub>. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (<i>R</i><sup>2</sup> = 0.97) between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) resolved OA's relatively lower oxygen-to-carbon (O : C) (0.44 ± 0.02) and higher hydrogen-to-carbon (H : C) (1.40 ± 0.03) molar ratios for the GVE / SO<sub>2</sub> mixture, with a significantly lower estimated average carbon oxidation state (OS<sub>c</sub>) of −0.51 ± 0.06 than −0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO<sub>2</sub> might be a significant explanation for the lower SOA oxidation degree.https://www.atmos-chem-phys.net/16/675/2016/acp-16-675-2016.pdf |