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Title: Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)

Abstract

Isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA) can contribute substantially to organic aerosol (OA) concentrations in forested areas under low NO conditions, hence significantly influencing the regional and global OA budgets, accounting, for example, for 16–36 % of the submicron OA in the southeastern United States (SE US) summer. Particle evaporation measurements from a thermodenuder show that the volatility of ambient IEPOX-SOA is lower than that of bulk OA and also much lower than that of known monomer IEPOX-SOA tracer species, indicating that IEPOX-SOA likely exists mostly as oligomers in the aerosol phase. The OH aging process of ambient IEPOX-SOA was investigated with an oxidation flow reactor (OFR). New IEPOX-SOA formation in the reactor was negligible, as the OFR does not accelerate processes such as aerosol uptake and reactions that do not scale with OH. Simulation results indicate that adding  ∼  100 µg m −3 of pure H 2SO 4 to the ambient air allows IEPOX-SOA to be efficiently formed in the reactor. The heterogeneous reaction rate coefficient of ambient IEPOX-SOA with OH radical ( k OH) was estimated as 4.0 ± 2.0  ×  10 −13 cm 3 molec −1 s −1, which is equivalent to more than a 2-week lifetime. A similar k OH was found for measurements of OH oxidation ofmore » ambient Amazon forest air in an OFR. At higher OH exposures in the reactor (>  1  ×  10 12 molec cm −3 s), the mass loss of IEPOX-SOA due to heterogeneous reaction was mainly due to revolatilization of fragmented reaction products. We report, for the first time, OH reactive uptake coefficients ( γ OH =  0.59 ± 0.33 in SE US and γ OH =  0.68 ± 0.38 in Amazon) for SOA under ambient conditions. A relative humidity dependence of k OH and γ OH was observed, consistent with surface-area-limited OH uptake. No decrease of k OH was observed as OH concentrations increased. These observations of physicochemical properties of IEPOX-SOA can help to constrain OA impact on air quality and climate.« less

Authors:
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Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1328474
Grant/Contract Number:
SC0011105
Resource Type:
Journal Article: Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 16; Journal Issue: 18; Related Information: CHORUS Timestamp: 2016-09-19 04:28:23; Journal ID: ISSN 1680-7324
Publisher:
Copernicus GmbH
Country of Publication:
Germany
Language:
English

Citation Formats

Hu, Weiwei, Palm, Brett B., Day, Douglas A., Campuzano-Jost, Pedro, Krechmer, Jordan E., Peng, Zhe, de Sá, Suzane S., Martin, Scot T., Alexander, M. Lizabeth, Baumann, Karsten, Hacker, Lina, Kiendler-Scharr, Astrid, Koss, Abigail R., de Gouw, Joost A., Goldstein, Allen H., Seco, Roger, Sjostedt, Steven J., Park, Jeong-Hoo, Guenther, Alex B., Kim, Saewung, Canonaco, Francesco, Prévôt, André S. H., Brune, William H., and Jimenez, Jose L. Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA). Germany: N. p., 2016. Web. doi:10.5194/acp-16-11563-2016.
Hu, Weiwei, Palm, Brett B., Day, Douglas A., Campuzano-Jost, Pedro, Krechmer, Jordan E., Peng, Zhe, de Sá, Suzane S., Martin, Scot T., Alexander, M. Lizabeth, Baumann, Karsten, Hacker, Lina, Kiendler-Scharr, Astrid, Koss, Abigail R., de Gouw, Joost A., Goldstein, Allen H., Seco, Roger, Sjostedt, Steven J., Park, Jeong-Hoo, Guenther, Alex B., Kim, Saewung, Canonaco, Francesco, Prévôt, André S. H., Brune, William H., & Jimenez, Jose L. Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA). Germany. doi:10.5194/acp-16-11563-2016.
Hu, Weiwei, Palm, Brett B., Day, Douglas A., Campuzano-Jost, Pedro, Krechmer, Jordan E., Peng, Zhe, de Sá, Suzane S., Martin, Scot T., Alexander, M. Lizabeth, Baumann, Karsten, Hacker, Lina, Kiendler-Scharr, Astrid, Koss, Abigail R., de Gouw, Joost A., Goldstein, Allen H., Seco, Roger, Sjostedt, Steven J., Park, Jeong-Hoo, Guenther, Alex B., Kim, Saewung, Canonaco, Francesco, Prévôt, André S. H., Brune, William H., and Jimenez, Jose L. Mon . "Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)". Germany. doi:10.5194/acp-16-11563-2016.
@article{osti_1328474,
title = {Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)},
author = {Hu, Weiwei and Palm, Brett B. and Day, Douglas A. and Campuzano-Jost, Pedro and Krechmer, Jordan E. and Peng, Zhe and de Sá, Suzane S. and Martin, Scot T. and Alexander, M. Lizabeth and Baumann, Karsten and Hacker, Lina and Kiendler-Scharr, Astrid and Koss, Abigail R. and de Gouw, Joost A. and Goldstein, Allen H. and Seco, Roger and Sjostedt, Steven J. and Park, Jeong-Hoo and Guenther, Alex B. and Kim, Saewung and Canonaco, Francesco and Prévôt, André S. H. and Brune, William H. and Jimenez, Jose L.},
abstractNote = {Isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA) can contribute substantially to organic aerosol (OA) concentrations in forested areas under low NO conditions, hence significantly influencing the regional and global OA budgets, accounting, for example, for 16–36 % of the submicron OA in the southeastern United States (SE US) summer. Particle evaporation measurements from a thermodenuder show that the volatility of ambient IEPOX-SOA is lower than that of bulk OA and also much lower than that of known monomer IEPOX-SOA tracer species, indicating that IEPOX-SOA likely exists mostly as oligomers in the aerosol phase. The OH aging process of ambient IEPOX-SOA was investigated with an oxidation flow reactor (OFR). New IEPOX-SOA formation in the reactor was negligible, as the OFR does not accelerate processes such as aerosol uptake and reactions that do not scale with OH. Simulation results indicate that adding  ∼  100 µg m−3 of pure H2SO4 to the ambient air allows IEPOX-SOA to be efficiently formed in the reactor. The heterogeneous reaction rate coefficient of ambient IEPOX-SOA with OH radical (kOH) was estimated as 4.0 ± 2.0  ×  10−13 cm3 molec−1 s−1, which is equivalent to more than a 2-week lifetime. A similar kOH was found for measurements of OH oxidation of ambient Amazon forest air in an OFR. At higher OH exposures in the reactor (>  1  ×  1012 molec cm−3 s), the mass loss of IEPOX-SOA due to heterogeneous reaction was mainly due to revolatilization of fragmented reaction products. We report, for the first time, OH reactive uptake coefficients (γOH =  0.59 ± 0.33 in SE US and γOH =  0.68 ± 0.38 in Amazon) for SOA under ambient conditions. A relative humidity dependence of kOH and γOH was observed, consistent with surface-area-limited OH uptake. No decrease of kOH was observed as OH concentrations increased. These observations of physicochemical properties of IEPOX-SOA can help to constrain OA impact on air quality and climate.},
doi = {10.5194/acp-16-11563-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 18,
volume = 16,
place = {Germany},
year = {Mon Sep 19 00:00:00 EDT 2016},
month = {Mon Sep 19 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.5194/acp-16-11563-2016

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