Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing

Daniel J. Bryant; William J. Dixon; James R. Hopkins; Rachel E. Dunmore; Kelly L. Pereira; Marvin Shaw; Freya A. Squires; Thomas J. Bannan; Archit Mehra; Stephen D. Worrall; Asan Bacak; Hugh Coe; Carl J. Percival; Lisa K. Whalley; Dwayne E. Heard; Eloise J. Slater; Bin Ouyang; Tianqu Cui; Jason D. Surratt; Di Liu; Zongbo Shi; Roy Harrison; Yele Sun; Weiqi Xu; Alastair C. Lewis; James D. Lee; Andrew R. Rickard; Jacqueline F. Hamilton

doi:10.5194/acp-2019-929

Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing

Daniel J. Bryant, William J. Dixon, James R. Hopkins, Rachel E. Dunmore, Kelly L. Pereira, Marvin Shaw, Freya A. Squires, Thomas J. Bannan, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Bin Ouyang, Tianqu Cui, Jason D. Surratt, Di LiuZongbo Shi, Roy Harrison, Yele Sun, Weiqi Xu, Alastair C. Lewis, James D. Lee, Andrew R. Rickard, Jacqueline F. Hamilton

Chemical Engineering & Applied Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants is poorly understood. In this study, we examined the formation of anthropogenically influenced iSOA during summer in Beijing, China. Local isoprene emissions and high levels of anthropogenic pollutants, in particular NOx and particulate SO2-4 , led to the formation of iSOA under both high- A nd low-NO oxidation conditions, with significant heterogeneous transformations of isoprene-derived oxidation products to particulate organosulfates (OSs) and nitrooxyorganosulfates (NOSs). Ultra-high-performance liquid chromatography coupled to high-resolution mass spectrometry was combined with a rapid automated data processing technique to quantify 31 proposed iSOA tracers in offline PM2.5 filter extracts. The co-elution of the inorganic ions in the extracts caused matrix effects that impacted two authentic standards differently. The average concentration of iSOA OSs and NOSs was 82.5 ngm-3, which was around 3 times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and the sulfate available for reactive uptake, as shown by a strong correlation with the product of ozone (O3) and particulate sulfate (SO2-4). A greater proportion of high-NO OS products were observed in Beijing compared with previous studies in less polluted environments. The iSOA-derived OSs and NOSs represented 0.62% of the oxidized organic aerosol measured by aerosol mass spectrometry on average, but this increased to ∼ 3% on certain days. These results indicate for the first time that iSOA formation in urban Beijing is strongly controlled by anthropogenic emissions and results in extensive conversion to OS products from heterogenous reactions.

Original language	English
Pages (from-to)	7531-7552
Number of pages	22
Journal	Atmospheric Chemistry and Physics
Volume	20
Issue number	12
DOIs	https://doi.org/10.5194/acp-2019-929 https://doi.org/10.5194/acp-20-7531-2020
Publication status	Published - 30 Jun 2020

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Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing
© Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
Submitted manuscript, 920 KBLicence: CC BY 3.0
VoR. Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing
© Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
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Bryant, D. J., Dixon, W. J., Hopkins, J. R., Dunmore, R. E., Pereira, K. L., Shaw, M., Squires, F. A., Bannan, T. J., Mehra, A., Worrall, S. D., Bacak, A., Coe, H., Percival, C. J., Whalley, L. K., Heard, D. E., Slater, E. J., Ouyang, B., Cui, T., Surratt, J. D., ... Hamilton, J. F. (2020). Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing. Atmospheric Chemistry and Physics, 20(12), 7531-7552. https://doi.org/10.5194/acp-2019-929, https://doi.org/10.5194/acp-20-7531-2020

@article{a6b31cd83eb048be95ceb89acb1fe85c,

title = "Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing",

abstract = "Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants is poorly understood. In this study, we examined the formation of anthropogenically influenced iSOA during summer in Beijing, China. Local isoprene emissions and high levels of anthropogenic pollutants, in particular NOx and particulate SO2-4 , led to the formation of iSOA under both high- A nd low-NO oxidation conditions, with significant heterogeneous transformations of isoprene-derived oxidation products to particulate organosulfates (OSs) and nitrooxyorganosulfates (NOSs). Ultra-high-performance liquid chromatography coupled to high-resolution mass spectrometry was combined with a rapid automated data processing technique to quantify 31 proposed iSOA tracers in offline PM2.5 filter extracts. The co-elution of the inorganic ions in the extracts caused matrix effects that impacted two authentic standards differently. The average concentration of iSOA OSs and NOSs was 82.5 ngm-3, which was around 3 times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and the sulfate available for reactive uptake, as shown by a strong correlation with the product of ozone (O3) and particulate sulfate (SO2-4). A greater proportion of high-NO OS products were observed in Beijing compared with previous studies in less polluted environments. The iSOA-derived OSs and NOSs represented 0.62% of the oxidized organic aerosol measured by aerosol mass spectrometry on average, but this increased to ∼ 3% on certain days. These results indicate for the first time that iSOA formation in urban Beijing is strongly controlled by anthropogenic emissions and results in extensive conversion to OS products from heterogenous reactions.",

author = "Bryant, {Daniel J.} and Dixon, {William J.} and Hopkins, {James R.} and Dunmore, {Rachel E.} and Pereira, {Kelly L.} and Marvin Shaw and Squires, {Freya A.} and Bannan, {Thomas J.} and Archit Mehra and Worrall, {Stephen D.} and Asan Bacak and Hugh Coe and Percival, {Carl J.} and Whalley, {Lisa K.} and Heard, {Dwayne E.} and Slater, {Eloise J.} and Bin Ouyang and Tianqu Cui and Surratt, {Jason D.} and Di Liu and Zongbo Shi and Roy Harrison and Yele Sun and Weiqi Xu and Lewis, {Alastair C.} and Lee, {James D.} and Rickard, {Andrew R.} and Hamilton, {Jacqueline F.}",

note = "{\textcopyright} Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.",

year = "2020",

month = jun,

day = "30",

doi = "10.5194/acp-2019-929",

language = "English",

volume = "20",

pages = "7531--7552",

journal = "Atmospheric Chemistry and Physics",

issn = "1680-7316",

publisher = "European Geosciences Union",

number = "12",

}

Bryant, DJ, Dixon, WJ, Hopkins, JR, Dunmore, RE, Pereira, KL, Shaw, M, Squires, FA, Bannan, TJ, Mehra, A, Worrall, SD, Bacak, A, Coe, H, Percival, CJ, Whalley, LK, Heard, DE, Slater, EJ, Ouyang, B, Cui, T, Surratt, JD, Liu, D, Shi, Z, Harrison, R, Sun, Y, Xu, W, Lewis, AC, Lee, JD, Rickard, AR & Hamilton, JF 2020, 'Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing', Atmospheric Chemistry and Physics, vol. 20, no. 12, pp. 7531-7552. https://doi.org/10.5194/acp-2019-929, https://doi.org/10.5194/acp-20-7531-2020

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T1 - Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing

AU - Bryant, Daniel J.

AU - Dixon, William J.

AU - Hopkins, James R.

AU - Dunmore, Rachel E.

AU - Pereira, Kelly L.

AU - Shaw, Marvin

AU - Squires, Freya A.

AU - Bannan, Thomas J.

AU - Mehra, Archit

AU - Worrall, Stephen D.

AU - Bacak, Asan

AU - Coe, Hugh

AU - Percival, Carl J.

AU - Whalley, Lisa K.

AU - Heard, Dwayne E.

AU - Slater, Eloise J.

AU - Ouyang, Bin

AU - Cui, Tianqu

AU - Surratt, Jason D.

AU - Liu, Di

AU - Shi, Zongbo

AU - Harrison, Roy

AU - Sun, Yele

AU - Xu, Weiqi

AU - Lewis, Alastair C.

AU - Lee, James D.

AU - Rickard, Andrew R.

AU - Hamilton, Jacqueline F.

PY - 2020/6/30

Y1 - 2020/6/30

N2 - Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants is poorly understood. In this study, we examined the formation of anthropogenically influenced iSOA during summer in Beijing, China. Local isoprene emissions and high levels of anthropogenic pollutants, in particular NOx and particulate SO2-4 , led to the formation of iSOA under both high- A nd low-NO oxidation conditions, with significant heterogeneous transformations of isoprene-derived oxidation products to particulate organosulfates (OSs) and nitrooxyorganosulfates (NOSs). Ultra-high-performance liquid chromatography coupled to high-resolution mass spectrometry was combined with a rapid automated data processing technique to quantify 31 proposed iSOA tracers in offline PM2.5 filter extracts. The co-elution of the inorganic ions in the extracts caused matrix effects that impacted two authentic standards differently. The average concentration of iSOA OSs and NOSs was 82.5 ngm-3, which was around 3 times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and the sulfate available for reactive uptake, as shown by a strong correlation with the product of ozone (O3) and particulate sulfate (SO2-4). A greater proportion of high-NO OS products were observed in Beijing compared with previous studies in less polluted environments. The iSOA-derived OSs and NOSs represented 0.62% of the oxidized organic aerosol measured by aerosol mass spectrometry on average, but this increased to ∼ 3% on certain days. These results indicate for the first time that iSOA formation in urban Beijing is strongly controlled by anthropogenic emissions and results in extensive conversion to OS products from heterogenous reactions.

AB - Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants is poorly understood. In this study, we examined the formation of anthropogenically influenced iSOA during summer in Beijing, China. Local isoprene emissions and high levels of anthropogenic pollutants, in particular NOx and particulate SO2-4 , led to the formation of iSOA under both high- A nd low-NO oxidation conditions, with significant heterogeneous transformations of isoprene-derived oxidation products to particulate organosulfates (OSs) and nitrooxyorganosulfates (NOSs). Ultra-high-performance liquid chromatography coupled to high-resolution mass spectrometry was combined with a rapid automated data processing technique to quantify 31 proposed iSOA tracers in offline PM2.5 filter extracts. The co-elution of the inorganic ions in the extracts caused matrix effects that impacted two authentic standards differently. The average concentration of iSOA OSs and NOSs was 82.5 ngm-3, which was around 3 times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and the sulfate available for reactive uptake, as shown by a strong correlation with the product of ozone (O3) and particulate sulfate (SO2-4). A greater proportion of high-NO OS products were observed in Beijing compared with previous studies in less polluted environments. The iSOA-derived OSs and NOSs represented 0.62% of the oxidized organic aerosol measured by aerosol mass spectrometry on average, but this increased to ∼ 3% on certain days. These results indicate for the first time that iSOA formation in urban Beijing is strongly controlled by anthropogenic emissions and results in extensive conversion to OS products from heterogenous reactions.

UR - https://www.atmos-chem-phys.net/20/7531/2020/

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U2 - 10.5194/acp-2019-929

DO - 10.5194/acp-2019-929

M3 - Article

SN - 1680-7316

VL - 20

SP - 7531

EP - 7552

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

IS - 12

ER -

Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing

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