FTIR time series of tropospheric HCN in eastern China: seasonality, interannual variability and source attribution
FTIR time series of tropospheric HCN in eastern China: seasonality, interannual variability and source attribution
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DOI：
10.5194/acp-2019-736
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发表时间：
2020-01
影响因子：
6.3
通讯作者：
Youwen Sun;Cheng Liu;Lin Zhang;M. Palm;J. Notholt;Haoyue Yin;C. Vigouroux;E. Lutsch;Wei Wang;Changong Shan;T. Blumenstock;T. Nagahama;I. Morino;E. Mahieu;K. Strong;B. Langerock;M. D. De Mazière;Q. Hu;Huifang Zhang;Christoph Petri;Jianguo Liu
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文献类型：
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作者：
Youwen Sun;Cheng Liu;Lin Zhang;M. Palm;J. Notholt;Haoyue Yin;C. Vigouroux;E. Lutsch;Wei Wang;Changong Shan;T. Blumenstock;T. Nagahama;I. Morino;E. Mahieu;K. Strong;B. Langerock;M. D. De Mazière;Q. Hu;Huifang Zhang;Christoph Petri;Jianguo Liu
抽象的。首次分析了中国东部地区对流层HCN柱量的季节变化和年际变化。结果来自2015年至2018年期间在合肥（117°10′ E，31°54′ N）使用地基高光谱分辨率傅里叶变换红外（FTIR）光谱仪记录的太阳吸收光谱。合肥地区对流层HCN柱的季节变化显著，全年有三个月平均峰值。对流层HCN柱峰值大小5月> 9月> 12月。对流层HCN柱在5月达到最大值（9.8 ± 0.78）× 1015 molecules/cm ~ 2，在11月达到最小值（7.16 ± 0.75）× 1015 molecules/cm ~ 2。在大多数情况下，合肥（32° N）的对流层HCN柱高于Ny Alesund（79° N），基律纳（68° N），不莱梅（53° N），少女峰（47° N），多伦多（44° N），陆别（43° N），Izana（28° N），Mauna Loa（20° N），La Reunion Maido（21° S），Lauder（45° S），和到达高度（78° S），隶属于大气成分变化探测网络（NDACC）。与其他年份的对应测量相比，2015年9月至2016年7月期间观察到对流层HCN柱的增强。增强幅度为5%~ 46%，平均22%。对流层HCN（ΔHCN）的增强与对流层CO（ΔCO）的同步增强相关，表明对流层CO和HCN的增强是由同一源引起的。GEOS-Chem标记的CO模拟，全球火灾地图和使用后向轨迹计算的PSCF（潜在源贡献函数）显示，5月份的季节性最大值主要是由于东南亚（SEAS）（41 ± 13.1%），欧洲和北亚（尤巴）（21 ± 9.3%）和非洲（AF）（22 ± 4.7%）的生物质燃烧的影响。9月份的季节性最大值主要是由于尤巴（38 ± 11.3%）、AF（26 ± 6.7%）、SEAS（14 ± 3.3%）和北方美洲（NA）（13.8 ± 8.4%）的生物量燃烧的影响。对于12月的季节最大值，主要贡献来自AF（36 ± 7.1%），尤巴（21 ± 5.2%）和NA（18.7 ± 5.2%）。2015年9月至2016年7月合肥（32° N）对流层HCN的增强归因于在此期间SEAS，尤巴和大洋洲（OCE）生物质燃烧的影响。特别是，2015年下半年OCE的火灾数量增加主导了2015年9月至12月对流层HCN的增强。2016年上半年，东南亚的火灾数量增加，主导了2016年1月至7月对流层HCN的增强。
Abstract. We analyzed seasonality and interannual variability of tropospheric HCN column amounts in densely populated eastern China for the first time. The results were derived from solar absorption spectra recorded with ground-based high spectral resolution Fourier transform infrared (FTIR) spectrometer at Hefei (117°10′ E, 31°54′ N) between 2015 and 2018. The tropospheric HCN columns over Hefei, China showed significant seasonal variations with three monthly mean peaks throughout the year. The magnitude of the tropospheric HCN column peak in May > September > December. The tropospheric HCN column reached a maximum of (9.8 ± 0.78) × 1015 molecules/cm2 in May and a minimum of (7.16 ± 0.75) × 1015 molecules/cm2 in November. In most cases, the tropospheric HCN columns at Hefei (32° N) are higher than the FTIR observations at Ny Alesund (79° N), Kiruna (68° N), Bremen (53° N), Jungfraujoch (47° N), Toronto (44° N), Rikubetsu (43° N), Izana (28° N), Mauna Loa (20° N), La Reunion Maido (21° S), Lauder (45° S), and Arrival Heights (78° S) that are affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Enhancements of the tropospheric HCN columns were observed between September 2015 and July 2016 compared to the counterpart measurements in other years. The magnitude of the enhancement ranges from 5 to 46 % with an average of 22 %. Enhancement of tropospheric HCN (ΔHCN) is correlated with the coincident enhancement of tropospheric CO (ΔCO), indicating that enhancements of tropospheric CO and HCN were due to the same sources. The GEOS-Chem tagged CO simulation, the global fire maps and the PSCFs (Potential Source Contribution Function) calculated using back trajectories revealed that the seasonal maxima in May is largely due to the influence of biomass burning in South Eastern Asia (SEAS) (41 ± 13.1 %), Europe and Boreal Asia (EUBA) (21 ± 9.3 %) and Africa (AF) (22 ± 4.7 %). The seasonal maxima in September is largely due to the influence of biomass burnings in EUBA (38 ± 11.3 %), AF (26 ± 6.7 %), SEAS (14 ± 3.3 %), and Northern America (NA) (13.8 ± 8.4 %). For the seasonal maxima in December, dominant contributions are from AF (36 ± 7.1 %), EUBA (21 ± 5.2 %), and NA (18.7 ± 5.2 %). The tropospheric HCN enhancement between September 2015 and July 2016 at Hefei (32° N) were attributed to an elevated influence of biomass burnings in SEAS, EUBA, and Oceania (OCE) in this period. Particularly, an elevated fire number in OCE in the second half of 2015 dominated the tropospheric HCN enhancement in September–December 2015. An elevated fire number in SEAS in the first half of 2016 dominated the tropospheric HCN enhancement in January–July 2016.