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SCIENCE CHINA Earth Sciences, Volume 61 , Issue 1 : 23-32(2018) https://doi.org/10.1007/s11430-017-9104-9

Exploration of the formation mechanism and source attribution of ambient ozone in Chongqing with an observation-based model

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  • ReceivedMar 16, 2017
  • AcceptedAug 28, 2017
  • PublishedOct 12, 2017

Abstract


Funded by

work was supportted by the Environmental Public Welfare Industry in China(201509001)

National Science and Technology Supporting Plan(2014BAC21B01)

and the Chongqing project of the Ozone Source Appointment and its impact on surrounding areas are acknowledged.


Acknowledgment

The support of the Chongqing Environmental Protection Bureau for the integrated field studies is deeply appreciated. The work was supportted by the Environmental Public Welfare Industry in China (Grant No. 201509001), the National Science and Technology Supporting Plan (Grant No. 2014BAC21B01), and the Chongqing Project of the Ozone Source Appointment and its Impact on Surrounding Areas are acknowledged.


Contributions statement

Corresponding author (email: yhzhang@pku.edu.cn)


References

[1] Cardelino C A, Chameides W L. An observation-based model for analyzing ozone precursor relationships in the urban atmosphere. J Air Waste Manage Association, 1995, 45: 161-180 CrossRef Google Scholar

[2] Chameides W, Walker J C G. A photochemical theory of tropospheric ozone. J Geophys Res, 1973, 78: 8751-8760 CrossRef ADS Google Scholar

[3] Geng F H, Zhao C S, Tang X, Lu G L, Tie X X. Analysis of ozone and VOCs measured in Shanghai: A case study. Atmos Environ, 2007, 41: 989-1001 CrossRef ADS Google Scholar

[4] Guttikunda S K, Tang Y, Carmichael G R, Kurata G, Pan L, Streets D G, Woo J H, Thongboonchoo N, Fried A. Impacts of Asian megacity emissions on regional air quality during spring 2001. J Geophys Res, 2005, 110: D20301 CrossRef ADS Google Scholar

[5] Hidy G M. Ozone process insights from field experiments—Part I: Overview. Atmos Environ, 2000, 34: 2001-2022 CrossRef ADS Google Scholar

[6] Huang W, Yu J Y, Tang X, Xu L P, Liu M. 2015. Regional ozone pollution status and causes of Chongqing in summer (in Chinese). Sichuan Environ, 34: 91–96. Google Scholar

[7] Kanaya Y, Fukuda M, Akimoto H, Takegawa N, Komazaki Y, Yokouchi Y, Koike M, Kondo Y. Urban photochemistry in central Tokyo: 2. Rates and regimes of oxidant (O3+NO2) production. J Geophys Res, 2008, 113: D06301 CrossRef ADS Google Scholar

[8] Kanaya Y, Pochanart P, Liu Y, Li J, Tanimoto H, Kato S, Suthawaree J, Inomata S, Taketani F, Okuzawa K, Kawamura K, Akimoto H, Wang Z F. Rates and regimes of photochemical ozone production over Central East China in June 2006: A box model analysis using comprehensive measurements of ozone precursors. Atmos Chem Phys, 2009, 9: 7711-7723 CrossRef Google Scholar

[9] Kleinman L I, Daum P H, Imre D G, Lee J H, Lee Y N, Nunnermacker L J, Springston S R, Weinstein-Lloyd J, Newman L. Ozone production in the New York City urban plume. J Geophys Res, 2000, 105: 14495-14511 CrossRef ADS Google Scholar

[10] Li J F, Lu K D, Lv W, Li J, Zhong L J, Ou Y B, Chen D H, Huang X, Zhang Y H. Fast increasing of surface ozone concentrations in Pearl River Delta characterized by a regional air quality monitoring network during 2006–2011. J Environ Sci, 2014, 26: 23-36 CrossRef Google Scholar

[11] Liu J J, Jiang C T, Song D, An B B. 2014. Analysis of distribution characteristics of surface ozone and its influencing factors in summer in Chongqing (in Chinese). J Chongqing Univ, 37: 91–98. Google Scholar

[12] Liu P, Zhai CZ, Yu JY, Bao L, Huang W, 2013. Correlation analysis on variation characteristics of surface ozone concentration and its precursor compounds in Chongqing (in Chinese). Environ Sci Manage, 38: 40–43. Google Scholar

[13] Liu R L, Zhai C Z, Li L, Yu J Y, Liu M, Xu L P, Feng N. 2017. Concentration characteristics and source analysis of ambient VOCs in summer and autumn in the urban area of Chongqing (in Chinese). Acta Sci Circums, 37: 1260–1267. Google Scholar

[14] Liu Z, Wang Y, Gu D, Zhao C, Huey L G, Stickel R, Liao J, Shao M, Zhu T, Zeng L, Amoroso A, Costabile F, Chang C C, Liu S C. Summertime photochemistry during CAREBeijing-2007: ROx budgets and O3 formation. Atmos Chem Phys, 2012, 12: 7737-7752 CrossRef ADS Google Scholar

[15] Lu K D, Zhang Y H, Su H, Brauers T, Chou C C, Hofzumahaus A, Liu S C, Kita K, Kondo Y, Shao M, Wahner A, Wang J L, Wang X S, Zhu T. Oxidant (O3+NO2) production processes and formation regimes in Beijing. J Geophys Res, 2010a, 115: D07303 CrossRef ADS Google Scholar

[16] Lu K D, Zhang Y H, Su H, Shao M, Zeng L M, Zhong L J, Xiang Y R, Chang C C, Chou C K C, Wahner A. Regional ozone pollution and key controlling factors of photochemical ozone production in Pearl River Delta during summer time. Sci China Chem, 2010b, 53: 651-663 CrossRef Google Scholar

[17] NRC. 1991. Rethinking the ozone problem in urban and regional air pollution. Washington: The National Academies Press. Google Scholar

[18] Qi X, Hao Q J, Ji D S, Zhang J K, Liu Z R, Hu B, Wang Y S, Jiang C S. 2014. Composition characteristics of atmospheric volatile organic compounds in the urban area of Beibei District, Chongqing (in Chinese). Environ Sci, 35: 3293–3301. Google Scholar

[19] Ran L, Zhao C S, Xu W Y, Han M, Lu X Q, Han S Q, Lin W L, Xu X B, Gao W, Yu Q, Geng F H, Ma N, Deng Z Z, Chen J. Ozone production in summer in the megacities of Tianjin and Shanghai, China: A comparative study. Atmos Chem Phys, 2012, 12: 7531-7542 CrossRef ADS Google Scholar

[20] Ren X R, Harder H, Martinez M, Lesher R L, Oliger A, Simpas J B, Brune W H, Schwab J J, Demerjian K L, He Y, Zhou X L, Gao H G. OH and HO2 chemistry in the urban atmosphere of New York City. Atmos Environ, 2003, 37: 3639-3651 CrossRef ADS Google Scholar

[21] Shao M, Tang X Y, Zhang Y H, Li W J. City clusters in China: Air and surface water pollution. Front Ecology Environ, 2006, 4: 353-361 CrossRef Google Scholar

[22] Shao M, Zhang Y, Zeng L, Tang X, Zhang J, Zhong L, Wang B. Ground-level ozone in the Pearl River Delta and the roles of VOC and NOx in its production. J Environ Manage, 2009, 90: 512-518 CrossRef PubMed Google Scholar

[23] Shirley T R, Brune W H, Ren X, Mao J, Lesher R, Cardenas B, Volkamer R, Molina L T, Molina M J, Lamb B, Velasco E, Jobson T, Alexander M. Atmospheric oxidation in the Mexico City Metropolitan Area (MCMA) during April 2003. Atmos Chem Phys, 2006, 6: 2753-2765 CrossRef Google Scholar

[24] Tang X Y, Zhang Y H, Shao M. 2006. Atmosphere Environmental Chemistry. Beijing: Higher Education Press. Google Scholar

[25] Wang T, Ding A, Gao J, Wu W S. Strong ozone production in urban plumes from Beijing, China. Geophys Res Lett, 2006, 33: L21806 CrossRef ADS Google Scholar

[26] Wang T, Xue L, Brimblecombe P, Lam Y F, Li L, Zhang L. Ozone pollution in China: A review of concentrations, meteorological influences, chemical precursors, and effects. Sci Total Environ, 2017, 575: 1582-1596 CrossRef PubMed Google Scholar

[27] Wei W, Lv Z F, Cheng S Y, Wang L L, Ji D S, Zhou Y, Han L H, Wang L T. Characterizing ozone pollution in a petrochemical industrial area in Beijing, China: A case study using a chemical reaction model. Environ Monit Assess, 2015, 187: 377 CrossRef PubMed Google Scholar

[28] Xu P, Hao Q J, Ji D S, Zhang J K, Liu Z R, Hu B, Wang Y S, Jiang C S. 2014. Observation of atmospheric pollutants in the urban area of Beibei District, Chongqing (in Chinese). Environ Sci, 35: 820–829. Google Scholar

[29] Xu X, Lin W, Wang T, Yan P, Tang J, Meng Z, Wang Y. Long-term trend of surface ozone at a regional background station in eastern China 1991–2006: Enhanced variability. Atmos Chem Phys, 2008, 8: 2595-2607 CrossRef Google Scholar

[30] Xu Z, Wang T, Xue L K, Louie P K K, Luk C W Y, Gao J, Wang S L, Chai F H, Wang W X. Evaluating the uncertainties of thermal catalytic conversion in measuring atmospheric nitrogen dioxide at four differently polluted sites in China. Atmos Environ, 2013, 76: 221-226 CrossRef ADS Google Scholar

[31] Xue L, Gu R, Wang T, Wang X, Saunders S, Blake D, Louie P K K, Luk C W Y, Simpson I, Xu Z, Wang Z, Gao Y, Lee S, Mellouki A, Wang W. Oxidative capacity and radical chemistry in the polluted atmosphere of Hong Kong and Pearl River Delta region: Analysis of a severe photochemical smog episode. Atmos Chem Phys Discuss, 2016, 2016: 1-26 CrossRef Google Scholar

[32] Xue L K, Wang T, Louie P K K, Luk C W Y, Blake D R, Xu Z. Increasing external effects negate local efforts to control ozone air pollution: A case study of Hong Kong and implications for other Chinese cities. Environ Sci Technol, 2014, 48: 10769-10775 CrossRef PubMed ADS Google Scholar

[33] Zhang J, Wang T, Chameides W L, Cardelino C, Kwok J, Blake D R, Ding A, So K L. Ozone production and hydrocarbon reactivity in Hong Kong, Southern China. Atmos Chem Phys, 2007, 7: 557-573 CrossRef Google Scholar

[34] Zhang Q, Yuan B, Shao M, Wang X, Lu S, Lu K, Wang M, Chen L, Chang C C, Liu S C. Variations of ground-level O3 and its precursors in Beijing in summertime between 2005 and 2011. Atmos Chem Phys, 2014, 14: 6089-6101 CrossRef ADS Google Scholar

[35] Zhang Y H, Su H, Zhong L J, Cheng Y F, Zeng L M, Wang X S, Xiang Y R, Wang J L, Gao D F, Shao M, Fan S J, Liu S C. Regional ozone pollution and observation-based approach for analyzing ozone-precursor relationship during the PRIDE-PRD2004 campaign. Atmos Environ, 2008a, 42: 6203-6218 CrossRef ADS Google Scholar

[36] Zhang Y H, Hu M, Zhong L J, Wiedensohler A, Liu S C, Andreae M O, Wang W, Fan S J. Regional integrated experiments on air quality over Pearl River Delta 2004 (PRIDE-PRD2004): Overview. Atmos Environ, 2008b, 42: 6157-6173 CrossRef ADS Google Scholar

[37] Zheng Y, Stevenson K J, Barrowcliffe R, Chen S, Wang H, Barnes J D. Ozone levels in Chongqing: A potential threat to crop plants commonly grown in the region?. Environ Pollut, 1998, 99: 299-308 CrossRef Google Scholar

  • Figure 1

    Time series measurements of j(O1D), temperature, concentrations of NO, NO2, O3, Ox, ISO, and AHC for three measurement sites at NQ (blue), CZ (red), and JYS (green).

  • Figure 2

    The location of the measurement sites with the maximum 8-hour ozone concentrations (in 10−9 V/V) for two typical days (red dots: online measurement sites, yellow dots: VOC offline measurement sites, cyan dots: VOC intensive measurement sites. The details are provided in the text). The bar plots surrounding the map show the reactivity of the grouped VOCs (in s−1) for the sites.

  • Figure 3

    Mean diurnal profiles of temperature and concentrations of O3, NO2, Ox, reactivity of AHC, and ISO for pollution days (red) and attainment days (blue) at NQ (left), CZ (middle), and JYS (right).

  • Figure 4

    Ozone budget analysis during ozone non-attainment days at NQ (a), CZ (b), and JYS (c).

  • Figure 5

    Time series of RIR for NOx, AHC, NHC, and CO at NQ (a), CZ (b), and JYS (c).

  • Figure 6

    Analysis of chemical control factors of local ozone in Chongqing. (a) Isopleth diagram of ozone production rate for averaged conditions in Chongqing (the isopleth lines are in 10−9 V/V h−1). The x-axis represents the AHC reactivity and the y-axis represents the NOx reactivity. The circles, squares, and diamonds denote the average AHC and NOx reactivity values for 15 measurement sites. (b)–(d) The average RIR values of NOx, AHC, NHC, and CO for campaign-averaged (b), pollution episode-averaged (c), and attainment days-averaged (d) conditions for NQ, CZ, and JYS.

  • Figure 7

    The RIR of different groups of VOCs during ozone non-attainment and attainment days at NQ, CZ, and JYS.

  • Figure 8

    Sources of VOCs. (a) Composition of VOCs in Chongqing based on the PMF Model. (b) RIR of various VOC emission sources based on the PMF results at NQ, CZ, and JYS.

  • Table 1   Summary of the measured species and instrument performance

    Species

    Instrument

    Accuracy (1σ)

    Limit of Dection (10−9V/V)

    O3

    Thermo Electric 49i

    5%

    0.5

    NO, NO2, NOx

    Thermo Electric 42i

    10%

    0.06, 0.3, 0.05

    VOCs

    GC-FID/MS

    10%

    0.01‒0.07

    CO

    Thermo Electric 48i

    5%

    4

    HONO

    Wet diffusion tube

    15%

    0.05

    PAN

    PAN instrument

    15%

    0.005

    jO1D, jNO2, jHONO

    Spectroradiometer

    10%

    -