A Four Carbon Organonitrate as a Significant Product of Secondary Isoprene Chemistry

Epameinondas Tsiligiannis; Rongrong Wu; Ben H. Lee; Christian Mark Salvador; Michael Priestley; Philip T.M. Carlsson; Sungah Kang; Anna Novelli; Luc Vereecken; Hendrik Fuchs; Alfred W. Mayhew; Jacqueline F. Hamilton; Peter M. Edwards; Juliane L. Fry; Bellamy Brownwood; Steven S. Brown; Robert J. Wild; Thomas J. Bannan; Hugh Coe; James Allan; Jason D. Surratt; Asan Bacak; Paul Artaxo; Carl Percival; Song Guo; Min Hu; Tao Wang; Thomas F. Mentel; Joel A. Thornton; Mattias Hallquist

doi:10.1029/2021GL097366

A Four Carbon Organonitrate as a Significant Product of Secondary Isoprene Chemistry

Epameinondas Tsiligiannis
, Rongrong Wu
, Ben H. Lee
, Christian Mark Salvador
, Michael Priestley
, Philip T.M. Carlsson
, Sungah Kang
, Anna Novelli
, Luc Vereecken
, Hendrik Fuchs
, Alfred W. Mayhew
, Jacqueline F. Hamilton
, Peter M. Edwards
, Juliane L. Fry
, Bellamy Brownwood
, Steven S. Brown
, Robert J. Wild
, Thomas J. Bannan
, Hugh Coe
, James Allan

Jason D. Surratt, Asan Bacak, Paul Artaxo, Carl Percival, Song Guo, Min Hu, Tao Wang, Thomas F. Mentel, Joel A. Thornton, Mattias Hallquist

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

16 Scopus citations

Abstract

Oxidation of isoprene by nitrate radicals (NO₃) or by hydroxyl radicals (OH) under high NO_x conditions forms a substantial amount of organonitrates (ONs). ONs impact NO_x concentrations and consequently ozone formation while also contributing to secondary organic aerosol. Here we show that the ONs with the chemical formula C₄H₇NO₅ are a significant fraction of isoprene-derived ONs, based on chamber experiments and ambient measurements from different sites around the globe. From chamber experiments we found that C₄H₇NO₅ isomers contribute 5%–17% of all measured ONs formed during nighttime and constitute more than 40% of the measured ONs after further daytime oxidation. In ambient measurements C₄H₇NO₅ isomers usually dominate both nighttime and daytime, implying a long residence time compared to C₅ ONs which are removed more rapidly. We propose potential nighttime sources and secondary formation pathways, and test them using a box model with an updated isoprene oxidation scheme.

Original language	English
Article number	e2021GL097366
Journal	Geophysical Research Letters
Volume	49
Issue number	11
DOIs	https://doi.org/10.1029/2021GL097366
State	Published - Jun 16 2022
Externally published	Yes

Funding

The authors acknowledge SAPHIR team of the Institute for Energy and Climate (IEK-8), Forschungszentrum Jülich for their support and technical help during the isoprene + NO3 experiments at the SAPHIR chamber, the team of the NO3Isop, JULIAC, Hong Kong, Changping, Amazon, SOAS and Gothenburg campaigns. This research has been supported by the European Research Council (ERC) (SARLEP grant agreement no. 681529), European Commission (EC) under the European Union's Horizon 2020 research and innovation program (Eurochamp 2020 grant agreement no. 730997 and FORCeS grant agreement no. 821205), Vetenskapsrådet (VR, Grant Nos. 2014–05332 and 2018–04430), and Svenska Forskningsrådet Formas (Grant Nos. 2015–1537 and 2019–586). A. Mayhew acknowledges the Natural Environment Research Council for a PhD studentship as part of the PANORAMA DTP. T. Wang is supported by the Hong Kong Research Grants Council (project no. A-PolyU502/16), and he thanks the Hong Kong Environmental Protection for providing access to its air monitoring site. The Amazon deployment was supported by the FAPESP-University of Manchester SPRINT initiative. The authors acknowledge SAPHIR team of the Institute for Energy and Climate (IEK‐8), Forschungszentrum Jülich for their support and technical help during the isoprene + NO experiments at the SAPHIR chamber, the team of the NO3Isop, JULIAC, Hong Kong, Changping, Amazon, SOAS and Gothenburg campaigns. This research has been supported by the European Research Council (ERC) (SARLEP grant agreement no. 681529), European Commission (EC) under the European Union's Horizon 2020 research and innovation program (Eurochamp 2020 grant agreement no. 730997 and FORCeS grant agreement no. 821205), Vetenskapsrådet (VR, Grant Nos. 2014–05332 and 2018–04430), and Svenska Forskningsrådet Formas (Grant Nos. 2015–1537 and 2019–586). A. Mayhew acknowledges the Natural Environment Research Council for a PhD studentship as part of the PANORAMA DTP. T. Wang is supported by the Hong Kong Research Grants Council (project no. A‐PolyU502/16), and he thanks the Hong Kong Environmental Protection for providing access to its air monitoring site. The Amazon deployment was supported by the FAPESP‐University of Manchester SPRINT initiative. 3

Keywords

VOC oxidation
atmospheric chamber
isoprene
organonitrate

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10.1029/2021GL097366

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Tsiligiannis, E., Wu, R., Lee, B. H., Salvador, C. M., Priestley, M., Carlsson, P. T. M., Kang, S., Novelli, A., Vereecken, L., Fuchs, H., Mayhew, A. W., Hamilton, J. F., Edwards, P. M., Fry, J. L., Brownwood, B., Brown, S. S., Wild, R. J., Bannan, T. J., Coe, H., ... Hallquist, M. (2022). A Four Carbon Organonitrate as a Significant Product of Secondary Isoprene Chemistry. Geophysical Research Letters, 49(11), Article e2021GL097366. https://doi.org/10.1029/2021GL097366

@article{f1db4653c0664b8d811396a106f914e7,

title = "A Four Carbon Organonitrate as a Significant Product of Secondary Isoprene Chemistry",

abstract = "Oxidation of isoprene by nitrate radicals (NO3) or by hydroxyl radicals (OH) under high NOx conditions forms a substantial amount of organonitrates (ONs). ONs impact NOx concentrations and consequently ozone formation while also contributing to secondary organic aerosol. Here we show that the ONs with the chemical formula C4H7NO5 are a significant fraction of isoprene-derived ONs, based on chamber experiments and ambient measurements from different sites around the globe. From chamber experiments we found that C4H7NO5 isomers contribute 5\%–17\% of all measured ONs formed during nighttime and constitute more than 40\% of the measured ONs after further daytime oxidation. In ambient measurements C4H7NO5 isomers usually dominate both nighttime and daytime, implying a long residence time compared to C5 ONs which are removed more rapidly. We propose potential nighttime sources and secondary formation pathways, and test them using a box model with an updated isoprene oxidation scheme.",

keywords = "VOC oxidation, atmospheric chamber, isoprene, organonitrate",

author = "Epameinondas Tsiligiannis and Rongrong Wu and Lee, \{Ben H.\} and Salvador, \{Christian Mark\} and Michael Priestley and Carlsson, \{Philip T.M.\} and Sungah Kang and Anna Novelli and Luc Vereecken and Hendrik Fuchs and Mayhew, \{Alfred W.\} and Hamilton, \{Jacqueline F.\} and Edwards, \{Peter M.\} and Fry, \{Juliane L.\} and Bellamy Brownwood and Brown, \{Steven S.\} and Wild, \{Robert J.\} and Bannan, \{Thomas J.\} and Hugh Coe and James Allan and Surratt, \{Jason D.\} and Asan Bacak and Paul Artaxo and Carl Percival and Song Guo and Min Hu and Tao Wang and Mentel, \{Thomas F.\} and Thornton, \{Joel A.\} and Mattias Hallquist",

note = "Publisher Copyright: {\textcopyright} 2022. The Authors.",

year = "2022",

month = jun,

day = "16",

doi = "10.1029/2021GL097366",

language = "English",

volume = "49",

journal = "Geophysical Research Letters",

issn = "0094-8276",

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number = "11",

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Tsiligiannis, E, Wu, R, Lee, BH, Salvador, CM, Priestley, M, Carlsson, PTM, Kang, S, Novelli, A, Vereecken, L, Fuchs, H, Mayhew, AW, Hamilton, JF, Edwards, PM, Fry, JL, Brownwood, B, Brown, SS, Wild, RJ, Bannan, TJ, Coe, H, Allan, J, Surratt, JD, Bacak, A, Artaxo, P, Percival, C, Guo, S, Hu, M, Wang, T, Mentel, TF, Thornton, JA & Hallquist, M 2022, 'A Four Carbon Organonitrate as a Significant Product of Secondary Isoprene Chemistry', Geophysical Research Letters, vol. 49, no. 11, e2021GL097366. https://doi.org/10.1029/2021GL097366

TY - JOUR

T1 - A Four Carbon Organonitrate as a Significant Product of Secondary Isoprene Chemistry

AU - Tsiligiannis, Epameinondas

AU - Wu, Rongrong

AU - Lee, Ben H.

AU - Salvador, Christian Mark

AU - Priestley, Michael

AU - Carlsson, Philip T.M.

AU - Kang, Sungah

AU - Novelli, Anna

AU - Vereecken, Luc

AU - Fuchs, Hendrik

AU - Mayhew, Alfred W.

AU - Hamilton, Jacqueline F.

AU - Edwards, Peter M.

AU - Fry, Juliane L.

AU - Brownwood, Bellamy

AU - Brown, Steven S.

AU - Wild, Robert J.

AU - Bannan, Thomas J.

AU - Coe, Hugh

AU - Allan, James

AU - Surratt, Jason D.

AU - Bacak, Asan

AU - Artaxo, Paul

AU - Percival, Carl

AU - Guo, Song

AU - Hu, Min

AU - Wang, Tao

AU - Mentel, Thomas F.

AU - Thornton, Joel A.

AU - Hallquist, Mattias

PY - 2022/6/16

Y1 - 2022/6/16

N2 - Oxidation of isoprene by nitrate radicals (NO3) or by hydroxyl radicals (OH) under high NOx conditions forms a substantial amount of organonitrates (ONs). ONs impact NOx concentrations and consequently ozone formation while also contributing to secondary organic aerosol. Here we show that the ONs with the chemical formula C4H7NO5 are a significant fraction of isoprene-derived ONs, based on chamber experiments and ambient measurements from different sites around the globe. From chamber experiments we found that C4H7NO5 isomers contribute 5%–17% of all measured ONs formed during nighttime and constitute more than 40% of the measured ONs after further daytime oxidation. In ambient measurements C4H7NO5 isomers usually dominate both nighttime and daytime, implying a long residence time compared to C5 ONs which are removed more rapidly. We propose potential nighttime sources and secondary formation pathways, and test them using a box model with an updated isoprene oxidation scheme.

AB - Oxidation of isoprene by nitrate radicals (NO3) or by hydroxyl radicals (OH) under high NOx conditions forms a substantial amount of organonitrates (ONs). ONs impact NOx concentrations and consequently ozone formation while also contributing to secondary organic aerosol. Here we show that the ONs with the chemical formula C4H7NO5 are a significant fraction of isoprene-derived ONs, based on chamber experiments and ambient measurements from different sites around the globe. From chamber experiments we found that C4H7NO5 isomers contribute 5%–17% of all measured ONs formed during nighttime and constitute more than 40% of the measured ONs after further daytime oxidation. In ambient measurements C4H7NO5 isomers usually dominate both nighttime and daytime, implying a long residence time compared to C5 ONs which are removed more rapidly. We propose potential nighttime sources and secondary formation pathways, and test them using a box model with an updated isoprene oxidation scheme.

KW - VOC oxidation

KW - atmospheric chamber

KW - isoprene

KW - organonitrate

UR - https://www.scopus.com/pages/publications/85132074163

U2 - 10.1029/2021GL097366

DO - 10.1029/2021GL097366

M3 - Article

AN - SCOPUS:85132074163

SN - 0094-8276

VL - 49

JO - Geophysical Research Letters

JF - Geophysical Research Letters

IS - 11

M1 - e2021GL097366

ER -

A Four Carbon Organonitrate as a Significant Product of Secondary Isoprene Chemistry

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Keywords

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