Atmospheric fate of peroxyacetyl nitrate in suburban Hong Kong and its impact on local ozone pollution

Lewei Zeng; Gang-Jie Fan; Xiaopu Lyu; Hai Guo; Jia-Lin Wang; Dawen Yao

doi:10.1016/j.envpol.2019.06.004

Atmospheric fate of peroxyacetyl nitrate in suburban Hong Kong and its impact on local ozone pollution

Lewei Zeng
, Gang-Jie Fan
, Xiaopu Lyu
, Hai Guo^*
, Jia-Lin Wang
, Dawen Yao

^*Corresponding author for this work

Academy of Geography, Sociology and International Studies

Research output: Contribution to journal › Journal article › peer-review

59 Citations (Scopus)

Abstract

Peroxyacetyl nitrate (PAN) is an important reservoir ofatmospheric nitrogen, modulating reactive nitrogen cycle and ozone (O₃)formation. To understand the origins of PAN, a field measurement was conductedat Tung Chung site (TC) in suburban Hong Kong from October to November 2016.The average level of PAN was 0.63 ± 0.05 ppbv, with a maximum of 7.30 ppbv.Higher PAN/O₃ ratio (0.043–0.058) was captured on episodes, i.e. when hourly maximum O₃exceeded 80 ppbv, than on non-episodes (0.01), since O₃ productionwas less efficient than PAN when there was an elevation of precursors (i.e. volatile organic compounds(VOCs) and nitrogen oxide (NO_x)). Model simulations revealed thatoxidations of acetaldehyde (65.3 ± 2.3%), methylglyoxal (MGLY, 12.7 ± 1.2%) andother oxygenated VOCs (OVOCs) (8.0 ± 0.6%), and radical cycling (12.2 ± 0.8%)were the major production pathways of peroxyacetyl (PA) radical, while localPAN formation was controlled by both VOCs and nitrogen dioxide (NO₂).Among all VOC species, carbonyls made the highest contribution (59%) to PANformation, followed by aromatics (26%) and biogenic VOCs (BVOCs) (10%) throughdirect oxidation/decomposition. Besides, active VOCs (i.e. carbonyls, aromatics, BVOCsand alkenes/alkynes) could stimulate hydroxyl (OH) production, thus indirectlyfacilitating the PAN formation. Apart from primary emissions, carbonyls werealso generated from oxidation of first-generation precursors, i.e., hydrocarbons, of whichxylenes contributed the most to PAN production. Furthermore, PAN formationsuppressed local O₃ formation at a rate of 2.84 ppbv/ppbv, when NO₂,OH and hydroperoxy (HO₂) levels decreased and nitrogen monoxide (NO)value enhanced. Namely, O₃ was reduced by 2.84 ppbv per ppbv PANformation. Net O₃ production rate was weakened (∼36%)due to PAN photochemistry, so as each individual production and loss pathway.The findings advanced our knowledge of atmospheric PAN and its impact on O₃production.

Original language	English
Pages (from-to)	1910-1919
Number of pages	10
Journal	Environmental Pollution
Volume	252, Part B
Early online date	6 Jun 2019
DOIs	https://doi.org/10.1016/j.envpol.2019.06.004
Publication status	Published - Sept 2019

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User-Defined Keywords

Formation pathways
Master chemical mechanism (MCM)
O formation
Photochemical smog
Precursors

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10.1016/j.envpol.2019.06.004

Cite this

@article{3c9470aeec9a49c98d5ff24841269288,

title = "Atmospheric fate of peroxyacetyl nitrate in suburban Hong Kong and its impact on local ozone pollution",

abstract = "Peroxyacetyl nitrate (PAN) is an important reservoir ofatmospheric nitrogen, modulating reactive nitrogen cycle and ozone (O3)formation. To understand the origins of PAN, a field measurement was conductedat Tung Chung site (TC) in suburban Hong Kong from October to November 2016.The average level of PAN was 0.63 ± 0.05 ppbv, with a maximum of 7.30 ppbv.Higher PAN/O3 ratio (0.043–0.058) was captured on episodes, i.e. when hourly maximum O3exceeded 80 ppbv, than on non-episodes (0.01), since O3 productionwas less efficient than PAN when there was an elevation of precursors (i.e. volatile organic compounds(VOCs) and nitrogen oxide (NOx)). Model simulations revealed thatoxidations of acetaldehyde (65.3 ± 2.3\%), methylglyoxal (MGLY, 12.7 ± 1.2\%) andother oxygenated VOCs (OVOCs) (8.0 ± 0.6\%), and radical cycling (12.2 ± 0.8\%)were the major production pathways of peroxyacetyl (PA) radical, while localPAN formation was controlled by both VOCs and nitrogen dioxide (NO2).Among all VOC species, carbonyls made the highest contribution (59\%) to PANformation, followed by aromatics (26\%) and biogenic VOCs (BVOCs) (10\%) throughdirect oxidation/decomposition. Besides, active VOCs (i.e. carbonyls, aromatics, BVOCsand alkenes/alkynes) could stimulate hydroxyl (OH) production, thus indirectlyfacilitating the PAN formation. Apart from primary emissions, carbonyls werealso generated from oxidation of first-generation precursors, i.e., hydrocarbons, of whichxylenes contributed the most to PAN production. Furthermore, PAN formationsuppressed local O3 formation at a rate of 2.84 ppbv/ppbv, when NO2,OH and hydroperoxy (HO2) levels decreased and nitrogen monoxide (NO)value enhanced. Namely, O3 was reduced by 2.84 ppbv per ppbv PANformation. Net O3 production rate was weakened (∼36\%)due to PAN photochemistry, so as each individual production and loss pathway.The findings advanced our knowledge of atmospheric PAN and its impact on O3production.",

keywords = "Formation pathways, Master chemical mechanism (MCM), O formation, Photochemical smog, Precursors",

author = "Lewei Zeng and Gang-Jie Fan and Xiaopu Lyu and Hai Guo and Jia-Lin Wang and Dawen Yao",

note = "Funding Information: This study was supported by the Research Grants Council of the Hong Kong Special Administrative Region via Grants PolyU5154/13E , PolyU152052 / 14E, PolyU152052/16E , CRF/C5004-15E , and CRF/C5022-14G and by the Research Institute for Sustainable Urban Development, Hong Kong Polytechnic University ( 1-BBW4 \& 1-BBW9 ). This study was partially supported by Hong Kong PolyU internal grants ( G-YBUQ , 1-ZVJT , and 4-BCF6 ) and the National Key R\&D Program of China supported by Ministry of Science and Technology of the People's Republic of China ( 2017YFC0212001 ). Publisher Copyright: {\textcopyright} 2019 Elsevier Ltd",

year = "2019",

month = sep,

doi = "10.1016/j.envpol.2019.06.004",

language = "English",

volume = "252, Part B",

pages = "1910--1919",

journal = "Environmental Pollution",

issn = "0269-7491",

publisher = "Elsevier Ltd.",

}

TY - JOUR

T1 - Atmospheric fate of peroxyacetyl nitrate in suburban Hong Kong and its impact on local ozone pollution

AU - Zeng, Lewei

AU - Fan, Gang-Jie

AU - Lyu, Xiaopu

AU - Guo, Hai

AU - Wang, Jia-Lin

AU - Yao, Dawen

N1 - Funding Information: This study was supported by the Research Grants Council of the Hong Kong Special Administrative Region via Grants PolyU5154/13E , PolyU152052 / 14E, PolyU152052/16E , CRF/C5004-15E , and CRF/C5022-14G and by the Research Institute for Sustainable Urban Development, Hong Kong Polytechnic University ( 1-BBW4 & 1-BBW9 ). This study was partially supported by Hong Kong PolyU internal grants ( G-YBUQ , 1-ZVJT , and 4-BCF6 ) and the National Key R&D Program of China supported by Ministry of Science and Technology of the People's Republic of China ( 2017YFC0212001 ). Publisher Copyright: © 2019 Elsevier Ltd

PY - 2019/9

Y1 - 2019/9

N2 - Peroxyacetyl nitrate (PAN) is an important reservoir ofatmospheric nitrogen, modulating reactive nitrogen cycle and ozone (O3)formation. To understand the origins of PAN, a field measurement was conductedat Tung Chung site (TC) in suburban Hong Kong from October to November 2016.The average level of PAN was 0.63 ± 0.05 ppbv, with a maximum of 7.30 ppbv.Higher PAN/O3 ratio (0.043–0.058) was captured on episodes, i.e. when hourly maximum O3exceeded 80 ppbv, than on non-episodes (0.01), since O3 productionwas less efficient than PAN when there was an elevation of precursors (i.e. volatile organic compounds(VOCs) and nitrogen oxide (NOx)). Model simulations revealed thatoxidations of acetaldehyde (65.3 ± 2.3%), methylglyoxal (MGLY, 12.7 ± 1.2%) andother oxygenated VOCs (OVOCs) (8.0 ± 0.6%), and radical cycling (12.2 ± 0.8%)were the major production pathways of peroxyacetyl (PA) radical, while localPAN formation was controlled by both VOCs and nitrogen dioxide (NO2).Among all VOC species, carbonyls made the highest contribution (59%) to PANformation, followed by aromatics (26%) and biogenic VOCs (BVOCs) (10%) throughdirect oxidation/decomposition. Besides, active VOCs (i.e. carbonyls, aromatics, BVOCsand alkenes/alkynes) could stimulate hydroxyl (OH) production, thus indirectlyfacilitating the PAN formation. Apart from primary emissions, carbonyls werealso generated from oxidation of first-generation precursors, i.e., hydrocarbons, of whichxylenes contributed the most to PAN production. Furthermore, PAN formationsuppressed local O3 formation at a rate of 2.84 ppbv/ppbv, when NO2,OH and hydroperoxy (HO2) levels decreased and nitrogen monoxide (NO)value enhanced. Namely, O3 was reduced by 2.84 ppbv per ppbv PANformation. Net O3 production rate was weakened (∼36%)due to PAN photochemistry, so as each individual production and loss pathway.The findings advanced our knowledge of atmospheric PAN and its impact on O3production.

AB - Peroxyacetyl nitrate (PAN) is an important reservoir ofatmospheric nitrogen, modulating reactive nitrogen cycle and ozone (O3)formation. To understand the origins of PAN, a field measurement was conductedat Tung Chung site (TC) in suburban Hong Kong from October to November 2016.The average level of PAN was 0.63 ± 0.05 ppbv, with a maximum of 7.30 ppbv.Higher PAN/O3 ratio (0.043–0.058) was captured on episodes, i.e. when hourly maximum O3exceeded 80 ppbv, than on non-episodes (0.01), since O3 productionwas less efficient than PAN when there was an elevation of precursors (i.e. volatile organic compounds(VOCs) and nitrogen oxide (NOx)). Model simulations revealed thatoxidations of acetaldehyde (65.3 ± 2.3%), methylglyoxal (MGLY, 12.7 ± 1.2%) andother oxygenated VOCs (OVOCs) (8.0 ± 0.6%), and radical cycling (12.2 ± 0.8%)were the major production pathways of peroxyacetyl (PA) radical, while localPAN formation was controlled by both VOCs and nitrogen dioxide (NO2).Among all VOC species, carbonyls made the highest contribution (59%) to PANformation, followed by aromatics (26%) and biogenic VOCs (BVOCs) (10%) throughdirect oxidation/decomposition. Besides, active VOCs (i.e. carbonyls, aromatics, BVOCsand alkenes/alkynes) could stimulate hydroxyl (OH) production, thus indirectlyfacilitating the PAN formation. Apart from primary emissions, carbonyls werealso generated from oxidation of first-generation precursors, i.e., hydrocarbons, of whichxylenes contributed the most to PAN production. Furthermore, PAN formationsuppressed local O3 formation at a rate of 2.84 ppbv/ppbv, when NO2,OH and hydroperoxy (HO2) levels decreased and nitrogen monoxide (NO)value enhanced. Namely, O3 was reduced by 2.84 ppbv per ppbv PANformation. Net O3 production rate was weakened (∼36%)due to PAN photochemistry, so as each individual production and loss pathway.The findings advanced our knowledge of atmospheric PAN and its impact on O3production.

KW - Formation pathways

KW - Master chemical mechanism (MCM)

KW - O formation

KW - Photochemical smog

KW - Precursors

UR - https://www.scopus.com/pages/publications/85070494854

U2 - 10.1016/j.envpol.2019.06.004

DO - 10.1016/j.envpol.2019.06.004

M3 - Journal article

C2 - 31227349

AN - SCOPUS:85070494854

SN - 0269-7491

VL - 252, Part B

SP - 1910

EP - 1919

JO - Environmental Pollution

JF - Environmental Pollution

ER -

Atmospheric fate of peroxyacetyl nitrate in suburban Hong Kong and its impact on local ozone pollution

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