Global Stratospheric Fluorine Inventory for 2004-2009 From Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) Measurements and SLIMCAT Model Simulations
Global Stratospheric Fluorine Inventory for 2004-2009 From Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) Measurements and SLIMCAT Model Simulations
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DOI：
10.5194/acp-14-267-2014
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发表时间：
2014-01
影响因子：
6.3
通讯作者：
Alexander Brown;M. Chipperfield;N. Richards;C. Boone;P. Bernath
中科院分区：
文献类型：
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作者：
Alexander Brown;M. Chipperfield;N. Richards;C. Boone;P. Bernath
抽象。含氟物质可能是极其有效的大气温室气体。我们目前的氟预算使用的ACE-FTS卫星仪器检索的有机和无机物种补充从SLIMCAT 3-D化学输运模型的输出。计算了2004年至2009年期间若干纬度带的预算：70-30° N、30-00° N、00° N-30° S和30-70° S。在较低的海拔高度，总氟含量主要来自CFC-12，在热带以外的海拔高度为20公里，在热带地区为29公里;在这些海拔高度以上，总氟含量主要由氟化氢（HF）组成。我们的数据显示，所有地点的总氟分布随海拔高度呈负斜率，这证明氟的总排放量（以氟含量衡量）一直在随时间增加。在热带地区，平流层总氟含量也以类似的速度增加：北方半球（NH）为32.5 ± 4.9 ppt yr−1（每年1.31 ± 0.20%），南半球（SH）为29.8 ± 5.3 ppt yr−1（每年1.21 ± 0.22%）。北半球和南半球的热带外平流层氟总量也以相似的速度增加：北半球每年28.3 ± 2.7 ppt（每年1.12 ± 0.11%），南半球每年24.3 ± 3.1 ppt（每年0.96 ± 0.12%）。辐射效率加权总氟的计算允许计算2004年和2009年之间的辐射强迫的变化。这些结果表明，由于在此期间含氟物质的增加，辐射强迫每年增加0.23 ± 0.11%至0.45 ± 0.11%。由于《蒙特利尔议定书》禁止使用哈龙和氯氟化碳，因此其混合比例呈下降趋势，从而抑制了氢氟碳化合物混合比例增加所导致的氟总量增加。这减少了含氟物种对全球变暖的影响。
Abstract. Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70–30° N, 30–00° N, 00° N–30° S, and 30–70° S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show that total fluorine profiles at all locations have a negative slope with altitude, providing evidence that overall fluorine emissions (measured by their F content) have been increasing with time. Total stratospheric fluorine is increasing at a similar rate in the tropics: 32.5 ± 4.9 ppt yr−1 (1.31 ± 0.20% per year) in the Northern Hemisphere (NH) and 29.8 ± 5.3 ppt yr−1 (1.21 ± 0.22% per year) in the Southern Hemisphere (SH). Extra-tropical total stratospheric fluorine is also increasing at a similar rate in both the NH and SH: 28.3 ± 2.7 ppt per year (1.12 ± 0.11% per year) in the NH and 24.3 ± 3.1 ppt per year (0.96 ± 0.12% per year) in the SH. The calculation of radiative efficiency-weighted total fluorine allows the changes in radiative forcing between 2004 and 2009 to be calculated. These results show an increase in radiative forcing of between 0.23 ± 0.11% per year and 0.45 ± 0.11% per year, due to the increase in fluorine-containing species during this time. The decreasing trends in the mixing ratios of halons and chlorofluorocarbons (CFCs), due to their prohibition under the Montreal Protocol, have suppressed an increase in total fluorine caused by increasing mixing ratios of hydrofluorocarbons (HFCs). This has reduced the impact of fluorine-containing species on global warming.