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

Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, S. De Sa Suzane, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. De Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong Hoo Park, Alex B. Guenther, Saewung KimFrancesco Canonaco, André S.H. Prévôt, William H. Brune, Jose L. Jimenez

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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 ∼ 100μgm-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 × 10-13cm3molec-1s-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 × 1012molec cm-3s), 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.

Original languageEnglish (US)
Pages (from-to)11563-11580
Number of pages18
JournalAtmospheric Chemistry and Physics
Volume16
Issue number18
DOIs
StatePublished - Sep 19 2016

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isoprene
aerosol
oxidation
volatility
aerosol formation
physicochemical property
reaction rate
ambient air

All Science Journal Classification (ASJC) codes

  • Atmospheric Science

Cite this

Hu, Weiwei ; Palm, Brett B. ; Day, Douglas A. ; Campuzano-Jost, Pedro ; Krechmer, Jordan E. ; Peng, Zhe ; De Sa 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). In: Atmospheric Chemistry and Physics. 2016 ; Vol. 16, No. 18. pp. 11563-11580.
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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 ∼ 100μgm-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 × 10-13cm3molec-1s-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 × 1012molec cm-3s), 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.",
author = "Weiwei Hu and Palm, {Brett B.} and Day, {Douglas A.} and Pedro Campuzano-Jost and Krechmer, {Jordan E.} and Zhe Peng and {De Sa Suzane}, S. and Martin, {Scot T.} and Alexander, {M. Lizabeth} and Karsten Baumann and Lina Hacker and Astrid Kiendler-Scharr and Koss, {Abigail R.} and {De Gouw}, {Joost A.} and Goldstein, {Allen H.} and Roger Seco and Sjostedt, {Steven J.} and Park, {Jeong Hoo} and Guenther, {Alex B.} and Saewung Kim and Francesco Canonaco and Pr{\'e}v{\^o}t, {Andr{\'e} S.H.} and Brune, {William H.} and Jimenez, {Jose L.}",
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language = "English (US)",
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Hu, W, Palm, BB, Day, DA, Campuzano-Jost, P, Krechmer, JE, Peng, Z, De Sa Suzane, S, Martin, ST, Alexander, ML, Baumann, K, Hacker, L, Kiendler-Scharr, A, Koss, AR, De Gouw, JA, Goldstein, AH, Seco, R, Sjostedt, SJ, Park, JH, Guenther, AB, Kim, S, Canonaco, F, Prévôt, ASH, Brune, WH & Jimenez, JL 2016, 'Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)', Atmospheric Chemistry and Physics, vol. 16, no. 18, pp. 11563-11580. https://doi.org/10.5194/acp-16-11563-2016

Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA). / Hu, Weiwei; Palm, Brett B.; Day, Douglas A.; Campuzano-Jost, Pedro; Krechmer, Jordan E.; Peng, Zhe; De Sa 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.

In: Atmospheric Chemistry and Physics, Vol. 16, No. 18, 19.09.2016, p. 11563-11580.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)

AU - Hu, Weiwei

AU - Palm, Brett B.

AU - Day, Douglas A.

AU - Campuzano-Jost, Pedro

AU - Krechmer, Jordan E.

AU - Peng, Zhe

AU - De Sa Suzane, S.

AU - Martin, Scot T.

AU - Alexander, M. Lizabeth

AU - Baumann, Karsten

AU - Hacker, Lina

AU - Kiendler-Scharr, Astrid

AU - Koss, Abigail R.

AU - De Gouw, Joost A.

AU - Goldstein, Allen H.

AU - Seco, Roger

AU - Sjostedt, Steven J.

AU - Park, Jeong Hoo

AU - Guenther, Alex B.

AU - Kim, Saewung

AU - Canonaco, Francesco

AU - Prévôt, André S.H.

AU - Brune, William H.

AU - Jimenez, Jose L.

PY - 2016/9/19

Y1 - 2016/9/19

N2 - 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 ∼ 100μgm-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 × 10-13cm3molec-1s-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 × 1012molec cm-3s), 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.

AB - 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 ∼ 100μgm-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 × 10-13cm3molec-1s-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 × 1012molec cm-3s), 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.

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