浏览全部资源
扫码关注微信
Received：20 December 2017，
Accepted：20 April 2018，
Published：2019-01
移动端阅览
利用Aura/OMI月均甲醛对流层垂直柱浓度数据对2005年—2016年中国广东省和江苏省的大气甲醛的时空变化规律、不同排放源的前体物的潜在贡献进行了分析。甲醛在广东省主要集中在珠三角地区，在江苏省分布则相对较为均匀。2005年—2010年，随着经济发展，在两省都发现了大面积的甲醛增加趋势；相应的，在2011年—2016年，由于减排等治理措施的实施，在两省都有大面积的甲醛减少现象。广东省的甲醛主要呈现出春季、秋季高于冬季再高于夏季的特征；而江苏地区夏季甲醛浓度远高于其他季节，并与光照强度的季节性特征较为一致。此外，由于广东省甲醛分布的均一性较差，因此区域性因素(如地形等)对广东省甲醛分布可能有着较大的影响。各个排放源中，工业源、交通源对珠三角潜在贡献可能较大；自然源对梅州等林地覆盖地区可能有相对较高的影响；在江苏省，各个排放源对甲醛的贡献相对均衡，但夏季较为频繁的生物质燃烧可能对夏季高值甲醛有着相对较高的贡献。
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.
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
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
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
Choi Y, Kim H, Tong D and Lee P. 2012. Summertime weekly cycles of observed and modeled NO x and O 3 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
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
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
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
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
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
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 NO x and VOC controls on surface ozone formation. Atmospheric Environment, 44(18): 2213–2223
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
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
高文康, 唐贵谦, 辛金元, 王莉莉, 王跃思. 2016. 京津冀地区严重光化学污染时段O 3 的时空分布特征. 环境科学研究, 29(5): 654–663
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 (
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
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
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
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
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
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
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
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
Kaczorowski J and Perelli A. 2004. Inversion of CO and NO x emissions using the adjoint of the IMAGES model. Atmospheric Chemistry and Physics Discussions, 4(6): 7985–8068
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
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
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
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
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
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
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
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
Sillman S. 1995. The use of NO y , H 2 O 2 , and HNO 3 as indicators for ozone‐NO x ‐hydrocarbon sensitivity in urban locations. Journal of Geophysical Research: Atmospheres, 100(D7): 14175–14188
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
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
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
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
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
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
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
张红旗, 许尔琪, 朱会义. 2015. 中国“三生用地”分类及其空间格局. 资源科学, 37(7): 1332–1338
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 (
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
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
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
张玉洁, 庞小兵, 牟玉静. 2009. 北京市植物排放的异戊二烯对大气中甲醛的贡献. 环境科学, 30(4): 976–981
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 (
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
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
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
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
相关文章
相关作者
相关机构
京公网安备11010802024621