Is atmospheric oxidation capacity better in indicating tropospheric O₃ formation?

Abstract

● This study summarizes and evaluates different approaches that indicate O₃ formation.

● Isopleth and sensitivity methods are useful but have many prerequisites.

● AOC is a better indicator of photochemical reactions leading to O₃ formation.

Tropospheric ozone (O₃) concentration is increasing in China along with dramatic changes in precursor emissions and meteorological conditions, adversely affecting human health and ecosystems. O₃ is formed from the complex nonlinear photochemical reactions from nitrogen oxides (NO_x = NO + NO₂) and volatile organic compounds (VOCs). Although the mechanism of O₃ formation is rather clear, describing and analyzing its changes and formation potential at fine spatial and temporal resolution is still a challenge today. In this study, we briefly summarized and evaluated different approaches that indicate O₃ formation regimes. We identify that atmospheric oxidation capacity (AOC) is a better indicator of photochemical reactions leading to the formation of O₃ and other secondary pollutants. Results show that AOC has a prominent positive relationship to O₃ in the major city clusters in China, with a goodness of fit (R²) up to 0.6. This outcome provides a novel perspective in characterizing O₃ formation and has significant implications for formulating control strategies of secondary pollutants.

Graphical abstract

Keywords

O ₃ / AOC / O ₃ formation regime

References

[1] Chen S , Wang H , Lu K , Zeng L , Hu M , Zhang Y . (2020). The trend of surface ozone in Beijing from 2013 to 2019: Indications of the persisting strong atmospheric oxidation capacity. Atmospheric Environment, 242 : 117801

[2] Chen T M , Kuschner W G , Gokhale J , Shofer S . (2007). Outdoor air pollution: Ozone health effects. American Journal of the Medical Sciences, 333( 4): 244– 248

[3] Clarke J F , Ching J K S . (1983). Aircraft observations of regional transport of ozone in the northeastern United States. Atmospheric Environment (1967), 17( 9): 1703– 1712

[4] Ding D , Xing J , Wang S , Dong Z , Zhang F , Liu S , Hao J . (2022). Optimization of a NO_x and VOC cooperative control strategy based on clean air benefits. Environmental Science & Technology, 56( 2): 739– 749

[5] Dodge M ( 1977). Combined Use of Modeling Techniques and Smog Chamber Data to Derive Ozone-precursor Relationships, US Environmental Protection Agency. Research Triangle Park, North Carolina: US Environmental Protection Agency, 881– 889

[6] Elshorbany Y F , Kurtenbach R , Wiesen P , Lissi E , Rubio M , Villena G , Gramsch E , Rickard A R , Pilling M J , Kleffmann J . (2009). Oxidation capacity of the city air of Santiago, Chile. Atmospheric Chemistry and Physics, 9( 6): 2257– 2273

[7] Feng T , Bei N , Huang R J , Cao J , Zhang Q , Zhou W , Tie X , Liu S , Zhang T , Su X , Lei W , Molina L T , Li G . (2016). Summertime ozone formation in Xi’an and surrounding areas, China. Atmospheric Chemistry and Physics, 16( 7): 4323– 4342

[8] Feng Z , Kobayashi K . (2009). Assessing the impacts of current and future concentrations of surface ozone on crop yield with meta-analysis. Atmospheric Environment, 43( 8): 1510– 1519

[9] Gaubert B , Bouarar I , Doumbia T , Liu Y , Stavrakou T , Deroubaix A , Darras S , Elguindi N , Granier C , Lacey F , Müller J F , Shi X , Tilmes S , Wang T , Brasseur G P . (2021). Global changes in secondary atmospheric pollutants during the 2020 COVID-19 pandemic. Journal of Geophysical Research: Atmospheres, 126( 8): e2020JD034213

[10] Husain L , Coffey P E , Meyers R E , Cederwall R T . (1977). Ozone transport from stratosphere to troposphere. Geophysical Research Letters, 4( 9): 363– 365

[11] Jacob D J . (2000). Heterogeneous chemistry and tropospheric ozone. Atmospheric Environment, 34( 12): 2131– 2159

[12] Jin S Demerjian K ( 1993). A photochemical box model for urban air quality study. Atmospheric Environment. Part B, Urban Atmosphere, 27( 4): 371− 387

[13] Jin X , Holloway T . (2015). Spatial and temporal variability of ozone sensitivity over China observed from the ozone monitoring instrument. Journal of Geophysical Research. Atmospheres, 120( 14): 7229– 7246

[14] Kentarchos A S , Roelofs G J . (2003). A model study of stratospheric ozone in the troposphere and its contribution to tropospheric OH formation. Journal of Geophysical Research, 108( D12): 8517

[15] Lelieveld J , Hoor P , Jöckel P , Pozzer A , Hadjinicolaou P , Cammas J P , Beirle S . (2009). Severe ozone air pollution in the Persian Gulf region. Atmospheric Chemistry and Physics, 9( 4): 1393– 1406

[16] Li K , Jacob D J , Liao H , Shen L , Zhang Q , Bates K H . (2019a). Anthropogenic drivers of 2013–2017 trends in summer surface ozone in China. Proceedings of the National Academy of Sciences of the United States of America, 116( 2): 422– 427

[17] Li K , Jacob D J , Liao H , Zhu J , Shah V , Shen L , Bates K H , Zhang Q , Zhai S . (2019b). A two-pollutant strategy for improving ozone and particulate air quality in China. Nature Geoscience, 12( 11): 906– 910

[18] Lippmann M . (1989). Health effects of ozone a critical review. JAPCA, 39( 5): 672– 695

[19] Liu Z , Wang Y , Hu B , Lu K , Tang G , Ji D , Yang X , Gao W , Xie Y , Liu J , Yao D , Yang Y , Zhang Y . (2021). Elucidating the quantitative characterization of atmospheric oxidation capacity in Beijing, China. Science of the Total Environment, 771 : 145306

[20] Lu H , Lyu X , Cheng H , Ling Z , Guo H . (2019). Overview on the spatial-temporal characteristics of the ozone formation regime in China. Environmental Science. Processes & Impacts, 21( 6): 916– 929

[21] Ma M , Gao Y , Ding A , Su H , Liao H , Wang S , Wang X , Zhao B , Zhang S , Fu P , Guenther A B , Wang M , Li S , Chu B , Yao X , Gao H . (2022). Development and assessment of a high-resolution biogenic emission inventory from urban green spaces in China. Environmental Science & Technology, 56( 1): 175– 184

[22] Ma M , Gao Y , Wang Y , Zhang S , Leung L R , Liu C , Wang S , Zhao B , Chang X , Su H , Zhang T , Sheng L , Yao X , Gao H . (2019). Substantial ozone enhancement over the North China Plain from increased biogenic emissions due to heat waves and land cover in summer 2017. Atmospheric Chemistry and Physics, 19( 19): 12195– 12207

[23] Menut L , Vautard R , Beekmann M , Honoré C . (2000). Sensitivity of photochemical pollution using the adjoint of a simplified chemistry-transport model. Journal of Geophysical Research, 105( D12): 15379– 15402

[24] Milford J B , Russell A G , Mcrae G J . (1989). A new approach to photochemical pollution control: Implications of spatial patterns in pollutant responses to reductions in nitrogen oxides and reactive organic gas emissions. Environmental Science & Technology, 23( 10): 1290– 1301

[25] Monks P S . (2005). Gas-phase radical chemistry in the troposphere. Chemical Society Reviews, 34( 5): 376– 395

[26] Pollack I B , Ryerson T B , Trainer M , Neuman J A , Roberts J M , Parrish D D . (2013). Trends in ozone, its precursors, and related secondary oxidation products in Los Angeles, California: A synthesis of measurements from 1960 to 2010. Journal of Geophysical Research. Atmospheres, 118( 11): 5893– 5911

[27] Porter W C , Safieddine S A , Heald C L . (2017). Impact of aromatics and monoterpenes on simulated tropospheric ozone and total OH reactivity. Atmospheric Environment, 169 : 250– 257

[28] Prinn R G . (2003). The cleansing capacity of the atmosphere. Annual Review of Environment and Resources, 28( 1): 29– 57

[29] Qian Y , Henneman L R F , Mulholland J A , Russell A G . (2019). Empirical development of ozone isopleths: Applications to Los Angeles. Environmental Science & Technology Letters, 6( 5): 294– 299

[30] Qin M Hu A Mao J Li X Sheng L Sun J Li J Wang X Zhang Y Hu J (2022). PM_2.5 and O₃ relationships affected by the atmospheric oxidizing capacity in the Yangtze River Delta, China . Science of the Total Environment, 810: 152268

[31] Ren X , Van Duin D , Cazorla M , Chen S , Mao J , Zhang L , Brune W H , Flynn J H , Grossberg N , Lefer B L , Rappenglück B , Wong K W , Tsai C , Stutz J , Dibb J E , Thomas Jobson B , Luke W T , Kelley P . (2013). Atmospheric oxidation chemistry and ozone production: Results from SHARP 2009 in Houston, Texas. Journal of Geophysical Research. Atmospheres, 118( 11): 5770– 5780

[32] Sillman S . (1995). The use of NO_y, H₂O₂, and HNO₃ as indicators for ozone-NO_x-hydrocarbon sensitivity in urban locations. Journal of Geophysical Research, 100( D7): 14175– 14188

[33] Sillman S . (1999). The relation between ozone, NO_x and hydrocarbons in urban and polluted rural environments. Atmospheric Environment, 33( 12): 1821– 1845

[34] Sillman S He D ( 2002). Some theoretical results concerning O₃-NO _x-VOC chemistry and NO _x-VOC indicators . Journal of Geophysical Research: Atmospheres, 107(D22): ACH 26– 21-ACH 26– 21

[35] Sillman S , Logan J A , Wofsy S C . (1990). The sensitivity of ozone to nitrogen oxides and hydrocarbons in regional ozone episodes. Journal of Geophysical Research, 95( D2): 1837– 1851

[36] Steinfeld J I . (1998). Atmospheric chemistry and physics: from air pollution to climate change. Environment, 40( 7): 26

[37] Tan Z , Lu K , Jiang M , Su R , Dong H , Zeng L , Xie S , Tan Q , Zhang Y . (2018). Exploring ozone pollution in Chengdu, southwestern China: A case study from radical chemistry to O₃-VOC-NO_x sensitivity. Science of the Total Environment, 636 : 775– 786

[38] Van Dingenen R , Dentener F J , Raes F , Krol M C , Emberson L , Cofala J . (2009). The global impact of ozone on agricultural crop yields under current and future air quality legislation. Atmospheric Environment, 43( 3): 604– 618

[39] Wang N , Lyu X , Deng X , Huang X , Jiang F , Ding A . (2019a). Aggravating O₃ pollution due to NO_x emission control in eastern China. Science of the Total Environment, 677 : 732– 744

[40] Wang P , Chen Y , Hu J , Zhang H , Ying Q . (2019b). Attribution of tropospheric ozone to NO_x and VOC emissions: Considering ozone formation in the transition regime. Environmental Science & Technology, 53( 3): 1404– 1412

[41] Wang S , Zhang Y , Ma J , Zhu S , Shen J , Wang P , Zhang H . (2021a). Responses of decline in air pollution and recovery associated with COVID-19 lockdown in the Pearl River Delta. Science of the Total Environment, 756 : 143868

[42] Wang W , Van Der A R , Ding J , Van Weele M , Cheng T . (2021b). Spatial and temporal changes of the ozone sensitivity in China based on satellite and ground-based observations. Atmospheric Chemistry and Physics, 21( 9): 7253– 7269

[43] Wang Y , Zhu S , Ma J , Shen J , Wang P , Wang P , Zhang H . (2021c). Enhanced atmospheric oxidation capacity and associated ozone increases during COVID-19 lockdown in the Yangtze River Delta. Science of the Total Environment, 768 : 144796

[44] Xing J , Wang S X , Jang C , Zhu Y , Hao J M . (2011). Nonlinear response of ozone to precursor emission changes in China: A modeling study using response surface methodology. Atmospheric Chemistry and Physics, 11( 10): 5027– 5044

[45] Ye L , Wang X , Fan S , Chen W , Chang M , Zhou S , Wu Z , Fan Q . (2016). Photochemical indicators of ozone sensitivity: Application in the Pearl River Delta, China. Frontiers of Environmental Science & Engineering, 10( 6): 15

[46] Zhao K , Luo H , Yuan Z , Xu D , Du Y , Zhang S , Hao Y , Wu Y , Huang J , Wang Y , Jiang R . (2021). Identification of close relationship between atmospheric oxidation and ozone formation regimes in a photochemically active region. Journal of Environmental Sciences-China, 102 : 373– 383

[47] Zhu J , Wang S , Wang H , Jing S , Lou S , Saiz-Lopez A , Zhou B . (2020). Observationally constrained modeling of atmospheric oxidation capacity and photochemical reactivity in Shanghai, China. Atmospheric Chemistry and Physics, 20( 3): 1217– 1232

[48] Zhu S , Poetzscher J , Shen J , Wang S , Wang P , Zhang H . (2021). Comprehensive insights into O₃ changes during the COVID-19 from O₃ formation regime and atmospheric oxidation capacity. Geophysical Research Letters, 48( 10): e2021GL093668

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