Comparative analysis of long-term (2005—2016) spatiotemporal variations in high-level tropospheric formaldehyde (HCHO) in Guangdong and Jiangsu Provinces in China

  • role: First author第一作者
  • Affiliation:

    State Key Laboratory of Remote Sensing Science, Jointly Sponsored by the Institute of Remote Sensing Applications of Chinese Academy of Sciences and Beijing Normal University, Beijing 100101, China

    University of Chinese Academy of Sciences, Beijing 100049, China

  • Email:soonyenju@foxmail.com
  • Introduction:朱松岩,1993年生,男,硕士研究生,研究方向为大气痕量气体反演、污染治理。E-mail:soonyenju@foxmail.com
Songyan ZHU13,  
  • role: Corresponding author通信作者
  • Affiliation:

    State Key Laboratory of Remote Sensing Science, Jointly Sponsored by the Institute of Remote Sensing Applications of Chinese Academy of Sciences and Beijing Normal University, Beijing 100101, China

  • Email:lixy01@radi.ac.cn
  • Introduction:李小英,1975年生,女,副研究员,研究方向为中高空大气临边探测。E-mail:lixy01@radi.ac.cn
Xiaoying LI1*,  
  • Affiliation:

    State Key Laboratory of Remote Sensing Science, Jointly Sponsored by the Institute of Remote Sensing Applications of Chinese Academy of Sciences and Beijing Normal University, Beijing 100101, China

Tianhai CHENG1,  
  • Affiliation:

    State Key Laboratory of Remote Sensing Science, Jointly Sponsored by the Institute of Remote Sensing Applications of Chinese Academy of Sciences and Beijing Normal University, Beijing 100101, China

    State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China

Chao YU12,  
  • Affiliation:

    Beijing Municipal Environmental Monitoring Center, Beijing 100048, China

Xinhui WANG4,  
  • Affiliation:

    State Key Laboratory of Remote Sensing Science, Jointly Sponsored by the Institute of Remote Sensing Applications of Chinese Academy of Sciences and Beijing Normal University, Beijing 100101, China

    University of Chinese Academy of Sciences, Beijing 100049, China

Jing MIAO13,  
  • Affiliation:

    Key Laboratory of Meteorological Disaster, Ministry of Education, Nanjing University of Information Science &Technology, Nanjing 210044, China

Can HOU5

реферат

High-level tropospheric formaldehyde (HCHO) columns were observed in Guangdong and Jiangsu Provinces in China by using the long-term records (2005–2016) of Aura OMI measurements. Given the socioeconomic status of Guangdong and Jiangsu Provinces, research concerning the widespread air pollution issues throughout these regions was imperative. Hence, the spatiotemporal variations in HCHO and the potential contributors were analyzed accordingly. We evaluated the spatiotemporal characteristics of HCHO columns in province- and prefecture-level cites to investigate the region of interest in various spatial resolutions. Hence, administrative shapefiles were used to clip the HCHO distributions to represent various sample regions. The spatial resolution of the OMI monthly gridded HCHO columns was 0.25° × 0.25°, but some ancillary data have finer resolutions than that of the level-3 gridded HCHO columns. Accordingly, the inverse distance-weighted interpolation algorithm and KD-Tree method were adopted for re-sampling fine spatial resolutions into 0.25° × 0.25°. The linear least square regression adopted in this study was the approach used to infer the potential trends exhibited in the HCHO images. The trends were fitted pixel by pixel, and the regional trends were calculated via zonal averaging of the administrative regions selected in the previously mentioned shapefiles. The Spearman correlation coefficients were employed to evaluate the similarity of the HCHO distribution and multitude sources (e.g., isoprene and anthropogenic VOCs). In Guangdong Province, HCHO columns concentrated in the Pearl River Delta (PRD), but an increasingly widespread distribution was observed in Jiangsu Province. An upward trend was found in both provinces from 2005 to 2010 that may be closely related to the rapid economy development in that period. Meanwhile, from 2011 to 2016, an overall downward trend was observed in these two regions, given the enacted multitude controls. With regard to seasonality, the highest HCHO columns were observed in spring and autumn, whereas the HCHO during summertime had the lowest concentration in Guangdong. The HCHO seasonal patterns corresponded to the seasonal patterns of sunlight intensity. Among all source sectors, industrial and transportation may contribute the most in the PRD, but all sectors may also contribute in the same order of magnitude in Jiangsu. In addition, biogenic sources may have a comparatively large contribution in the Northeastern Guangdong, and the biomass burning in summertime possibly played a substantial role in the summertime HCHO concentration in Jiangsu Province. Although isoprene plays significant role in HCHO concentration in global scale, the anthropogenic impact cannot be neglected as well. According to previous studies, anthropogenic sources have more than 40% influence. In addition, in comparison with isoprene, the Spearman correlation coefficients were high for anthropogenic VOCs with HCHO columns. Given the relatively large amount of emissions, industrial sources may be influential for more than 40%. Biomass burning sources cannot be ignored in woodlands, such as in Northeastern Guangdong. Transportation sources exhibited the most similar Spearman correlation coefficients in Guangdong, especially in PRD. Therefore, even a downward trend of transportation emissions was observed in PRD. They may account for a large amount of HCHO concentration. After a comparison, power-based emissions only took a small fraction of approximately 1% for Guangdong and Jiangsu.

ключеви́че слова́

HCHO;OMI;VOC;photochemical reaction;anthropogenic emissions;trend analysis

References

  1. 1.
    Barkley M P, Smedt I D, Van Roozendael M, Kurosu T P, Chance K, Arneth A, Hagberg D, Guenther A, Paulot F, Marais E and Mao J Q. 2013. Top-down isoprene emissions over tropical South America inferred from SCIAMACHY and OMI formaldehyde columns. Journal of Geophysical Research: Atmospheres, 118(12): 6849–6868
  2. 2.
    Bauwens M, Stavrakou T, Müller J F, De Smedt I, Van Roozendael M, Van Der Werf G R, Wiedinmyer C, Kaiser J W, Sindelarova K and Guenther A. 2016. Nine years of global hydrocarbon emissions based on source inversion of OMI formaldehyde observations. Atmospheric Chemistry and Physics, 16(15): 10133–10158
  3. 3.
    Bo Y, Cai H and Xie S D. 2008. Spatial and temporal variation of historical anthropogenic NMVOCs emission inventories in China. Atmospheric Chemistry and Physics, 8(23): 7297–7316
  4. 4.
    Choi Y, Kim H, Tong D and Lee P. 2012. Summertime weekly cycles of observed and modeled NOx and O3 concentrations as a function of satellite-derived ozone production sensitivity and land use types over the Continental United States. Atmospheric Chemistry and Physics, 12(14): 6291–6307
  5. 5.
    De Smedt I, Müller J F, Stavrakou T, Van Der A R, Eskes H and Van Roozendael M. 2008. Twelve years of global observations of formaldehyde in the troposphere using GOME and SCIAMACHY sensors. Atmospheric Chemistry and Physics, 8(16): 4947–4963
  6. 6.
    De Smedt I, Roozendael M V, Stavrakou T, Müller J F, Lerot C, Theys N, Valks P, Hao N and Van Der A R. 2012. Improved retrieval of global tropospheric formaldehyde columns from GOME-2/MetOp-A addressing noise reduction and instrumental degradation issues. Atmospheric Measurement Techniques, 5(11): 2933–2949
  7. 7.
    De Smedt I, Stavrakou T, Hendrick F, Danckaert T, Vlemmix T, Pinardi G, Theys N, Lerot C, Gielen C, Vigouroux C, Hermans C, Fayt C, Veefkind P, Müller J F and Van Roozendael M. 2015. Diurnal, seasonal and long-term variations of global formaldehyde columns inferred from combined OMI and GOME-2 observations. Atmospheric Chemistry and Physics Discussions, 15(8): 12241–12300
  8. 8.
    De Smedt I, Stavrakou T, Müller J F, Van Der A R J and Van Roozendael M. 2010. Trend detection in satellite observations of formaldehyde tropospheric columns. Geophysical Research Letters, 37(18): L18808
  9. 9.
    Duncan B N, Yoshida Y, Damon M R, Douglass A R and Witte J C. 2009. Temperature dependence of factors controlling isoprene emissions. Geophysical Research Letters, 36(5): L05813
  10. 10.
    Duncan B N, Yoshida Y, Olson J R, Sillman S, Martin R V, Lamsal L, Hu Y T, Pickering K E, Retscher C, Allen D J and Crawford J H. 2010. Application of OMI observations to a space-based indicator of NOx and VOC controls on surface ozone formation. Atmospheric Environment, 44(18): 2213–2223
  11. 11.
    Friedfeld S, Fraser M, Ensor K, Tribble S, Rehle D, Leleux D and Tittel F. 2002. Statistical analysis of primary and secondary atmospheric formaldehyde. Atmospheric Environment, 36(30): 4767–4775
  12. 12.
    Fu T M, Jacob D J, Palmer P I, Chance K, Wang Y X, Barletta B. Blake D R, Stanton J C and Pilling M J 2007. Space‐based formaldehyde measurements as constraints on volatile organic compound emissions in east and south Asia and implications for ozone. Journal of Geophysical Research: Atmospheres, 112(D6): D06312
  13. 13.
    Gao W K, Tang G Q, Xin J Y, Wang L L and Wang Y S. 2016. Spatial-temporal variations of ozone during severe photochemical pollution over the Beijing-Tianjin-Hebei region. Research of Environmental Sciences, 29(5): 654–663 (
  14. 14.
    Giglio L, Loboda T, Roy D P, Quayle B and Justiceb C O. 2009. An active-fire based burned area mapping algorithm for the MODIS sensor. Remote Sensing of Environment, 113(2): 408–420
  15. 15.
    González Abad G, Liu X, Chance K, H. Wang1, Kurosu T P and Suleiman R 2015. Updated smithsonian astrophysical observatory ozone monitoring instrument (SAO OMI) formaldehyde retrieval. Atmospheric Measurement Techniques, 8(1): 19–32
  16. 16.
    Guenther A, Karl T, Harley P, Wiedinmyer C, Palmer P I and Geron C. 2006. Estimates of global terrestrial isoprene emissions using MEGAN (model of emissions of gases and aerosols from nature). Atmospheric Chemistry and Physics, 6(11): 3181–3210
  17. 17.
    Guenther A B, Jiang X, Heald C L, Sakulyanontvittaya T, Duhl T, Emmons L K and Wang X. 2012. The model of emissions of gases and aerosols from nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions. Geoscientific Model Development, 5(6): 1471–1492
  18. 18.
    Hao J M, He D Q, Wu Y, Fu L X and He K B. 2000. A study of the emission and concentration distribution of vehicular pollutants in the urban area of Beijing. Atmospheric Environment, 34(3): 453–465
  19. 19.
    He K. 2012. Multi-resolution Emission Inventory for China (MEIC): model framework and 1990-2010 anthropogenic emissions[C]//Proceedings of 2012 AGU Fall Meeting. Beijing, China: School of Environment, Tsinghua University
  20. 20.
    Huo H, Zhang Q, Guan D B, Su X, Zhao H Y and He K B. 2014. Examining air pollution in China using production- and consumption-based emissions accounting approaches. Environmental Science and Technology, 48(24): 14139–14147
  21. 21.
    Jin X M and 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
  22. 22.
    Kaczorowski J and Perelli A. 2004. Inversion of CO and NOx emissions using the adjoint of the IMAGES model. Atmospheric Chemistry and Physics Discussions, 4(6): 7985–8068
  23. 23.
    Li M, Zhang Q, Kurokawa J I, Woo J H, He K B, Lu Z F, Ohara T, Song Y, Streets D G, Carmichael G R, Cheng Y F, Hong C P, Huo H, Jiang X J, Kang S C, Liu F, Su H and Zheng B. 2017. MIX: a mosaic Asian anthropogenic emission inventory under the international collaboration framework of the MICS-Asia and HTAP. Atmospheric Chemistry and Physics, 17(2): 935–963
  24. 24.
    Li M, Zhang Q, Streets D G, He K B, Cheng Y F, Emmons L K, Huo H, Kang S C, Lu Z, Shao M, Su H, Yu X and Zhang Y. 2014. Mapping Asian anthropogenic emissions of non-methane volatile organic compounds to multiple chemical mechanisms. Atmospheric Chemistry and Physics, 14(11): 5617–5638
  25. 25.
    Liu F, Zhang Q, Tong D, Zheng B, Li M, Huo H and He K B. 2015. High-resolution inventory of technologies, activities, and emissions of coal-fired power plants in China from 1990 to 2010. Atmospheric Chemistry and Physics, 15(23): 13299–13317
  26. 26.
    Marais E A, Jacob D J, Kurosu T P, Chance K V, Murphy J G, Reeves C, Mills G, Casadio S, Millet D B, Barkley M P, Paulot F and Mao J Q. 2012. Isoprene emissions in Africa inferred from OMI observations of formaldehyde columns. Atmospheric Chemistry and Physics Discussions, 12(3): 7475–7520
  27. 27.
    Müller J F, Stavrakou T, Wallens S, De Smedt I, Van Roozendael M, Potosnak M J, Rinne J, Munger B, Goldstein A and Guenther A B. 2007. Global isoprene emissions estimated using MEGAN, ECMWF analyses and a detailed canopy environment model. Atmospheric Chemistry and Physics, 8(5): 1329–1341
  28. 28.
    Pang X B and Mu Y J. 2006. Seasonal and diurnal variations of carbonyl compounds in Beijing ambient air. Atmospheric Environment, 40(33): 6313–6320
  29. 29.
    Peters E, Wittrock F, K. Großmann, Frieß U, Richter A and Burrows J P 2012. Formaldehyde and nitrogen dioxide over the remote western Pacific Ocean: SCIAMACHY and GOME-2 validation using ship-based MAX-DOAS observations. Atmospheric Chemistry and Physics, 12(22): 11179–11197
  30. 30.
    Roy D P, Boschetti L, Justice C O and Ju J. 2008. The collection 5 MODIS burned area product — Global evaluation by comparison with the MODIS active fire product. Remote Sensing of Environment, 112(9): 3690–3707
  31. 31.
    Sillman S. 1995. The use of NOy, H2O2, and HNO3 as indicators for ozone‐NOx‐hydrocarbon sensitivity in urban locations. Journal of Geophysical Research: Atmospheres, 100(D7): 14175–14188
  32. 32.
    Souri A H, Choi Y, Jeon W, Woo J H and Zhang Q. 2017. Remote sensing evidence of decadal changes in major tropospheric ozone precursors over East Asia. Journal of Geophysical Research: Atmospheres, 122(4): 2474–2492
  33. 33.
    Stavrakou T, Müller J F, Bauwens M, De Smedt I, Van Roozendael M, Guenther A, Wild M and Xia, X. 2013. Isoprene emissions over Asia 1979-2012: impact of climate and land-use changes. Atmospheric Chemistry and Physics Discussions, 13(11): 29551–29592
  34. 34.
    Vrekoussis M, Wittrock F, Richter A and Burrows J P. 2010. GOME-2 observations of oxygenated VOCs: what can we learn from the ratio glyoxal to formaldehyde on a global scale?. Atmospheric Chemistry and Physics Discussions, 10(8): 19031–19069
  35. 35.
    Wang Y, Zhang Y, Hao J and Luo M. 2010. Seasonal and spatial variability of surface ozone over China: contributions from background and domestic pollution. Atmospheric Chemistry and Physics, 11(7): 3511–3525
  36. 36.
    Wang Z H, Bai Y H and Zhang S Y. 2003. A biogenic volatile organic compounds emission inventory for Beijing. Atmospheric Environment, 37(27): 3771–3782
  37. 37.
    Wei W, Wang S X, Chatani S, Klimont Z, Cofala J and Hao J M. 2008. Emission and speciation of non-methane volatile organic compounds from anthropogenic sources in China. Atmospheric Environment, 42(20): 4976–4988
  38. 38.
    Wei X L, Li Y S, Lam K S, Wang A Y and Wang T J. 2007. Impact of biogenic VOC emissions on a tropical cyclone-related ozone episode in the Pearl River Delta region, China. Atmospheric Environment, 41(36): 7851–7864
  39. 39.
    Zhang H Q, Xu E Q and Zhu H Y. 2015. An ecological-living-industrial land classification system and its spatial distribution in China. Resources Science, 37(7): 1332–1338 (
  40. 40.
    Zhang Q, Shao M, Li Y, Lu S H, Yuan B and Chen W T. 2012. Increase of ambient formaldehyde in Beijing and its implication for VOC reactivity. Chinese Chemical Letters, 23(9): 1059–1062
  41. 41.
    Zhang Q, Streets D G, Carmichael G R, He K B, Huo H, Kannari A, Klimont Z, Park I S, Reddy S, Fu J S, Chen D, Duan L, Lei Y, Wang L T and Yao Z L. 2009. Asian emissions in 2006 for the NASA INTEX-B mission. Atmospheric Chemistry and Physics, 9(14): 5131–5153
  42. 42.
    Zhang X S, Mu Y J, Song W Z and Zhang Y H. 2000. Seasonal variations of isoprene emissions from deciduous trees. Atmospheric Environment, 34(18): 3027–3032
  43. 43.
    Zhang Y J, Pang X B and Mu Y J. 2009. Contribution of isoprene emitted from vegetable to atmospheric formaldehyde in the ambient air of Beijing city. Environmental Science, 30(4): 976–981 (
  44. 44.
    Zheng B, Huo H, Zhang Q, Yao Z L, Wang X T, Yang X F, Liu H and He K B. 2014. High-resolution mapping of vehicle emissions in China in 2008. Atmospheric Chemistry and Physics, 14(18): 9787–9805
  45. 45.
    Zhu L, Jacob D J, Kim P S, Fisher J A, Yu K, Travis K R, Mickley L J, Yantosca R M, Sulprizio M P, De Smedt I, Abad G G, Chance K, Li C, Ferrare R, Fried A, Hair J W, Hanisco T F, Richter D, Scarino A J, Walega J, Weibring P and Wolfe G M. 2016. Observing atmospheric formaldehyde (HCHO) from space: validation and intercomparison of six retrievals from four satellites (OMI, GOME2A, GOME2B, OMPS) with SEAC4RS aircraft observations over the Southeast US. Atmospheric Chemistry and Physics, 16(21): 13477–13490
  46. 46.
    Zhu L, Mickley L J, Jacob D J, Marais E A, Sheng J X, Hu L, González Abad G and Chance K. 2017. Long‐term (2005-2014) trends in formaldehyde (HCHO) columns across North America as seen by the OMI satellite instrument: evidence of changing emissions of volatile organic compounds. Geophysical Research Letters, 44(13): 7079–7086
  47. 47.
    Zhu S Y, Li X Y, Yu C, Wang H, Wang Y and Miao J. 2018. Spatiotemporal variations in satellite-based formaldehyde (HCHO) in the Beijing-Tianjin-Hebei region in China from 2005 to 2015. Atmosphere, 9(1): 5

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