The continental source of glyoxal estimated by the synergistic use of spaceborne measurements and inverse modelling
The continental source of glyoxal estimated by the synergistic use of spaceborne measurements and inverse modelling
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DOI：
10.5194/acp-9-8431-2009
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发表时间：
2009-11
影响因子：
6.3
通讯作者：
T. Stavrakou;J.‐F. Müller;I. D. Smedt;M. Roozendael;M. Kanakidou;M. Vrekoussis;F. Wittrock;A. Richter;J. Burrows
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文献类型：
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作者：
T. Stavrakou;J.‐F. Müller;I. D. Smedt;M. Roozendael;M. Kanakidou;M. Vrekoussis;F. Wittrock;A. Richter;J. Burrows
抽象的。2005年从SCIAMACHY卫星仪器中检索到的对流层乙二醛和甲醛柱与IMAGESv 2全球化学传输模型及其伴随模型一起用于双化合物反演方案，旨在估计乙二醛的大陆来源。甲醛的观察结果提供了一个重要的约束生产乙二醛从异戊二烯的模型中，因为异戊二烯的降解构成了乙二醛和甲醛的重要来源。目前的模拟研究在很大程度上低估了观测到的乙二醛卫星柱，指出存在一个额外的陆地生物源乙二醛源。我们在模型中包括一个额外的乙二醛源，我们通过两个反演实验探索其可能的分布和大小。在第一种情况下，额外的来源表示为直接乙二醛排放，在第二种情况下，作为通过氧化未指定的乙二醛前体的二次形成。除了这个额外的来源，反演方案优化的主要乙二醛和甲醛的排放量，以及他们的二次生产从其他确定的非甲烷挥发性有机前体的人为，热解和生物起源。在第一次反演实验中，额外的直接来源，估计为36 Tg/年，占全球大陆源的38%，而异戊二烯的贡献同样重要（30%），其余的人为（20%）和热通量占。反演成功地减少了低估的乙二醛柱的模型，但它导致了严重高估的乙二醛表面浓度与原位测量相比。在第二种情况下，推断的全球大陆乙二醛总来源估计为108 Tg/年，几乎是全球先验来源的两倍。额外的次级来源是全球乙二醛预算的最大贡献（50%），其次是异戊二烯（26%）和人为NMVOC前体（14%）。在这种情况下，实现了更好的性能，因为更新的排放量允许一个令人满意的协议的模型与卫星和现场乙二醛观测。
Abstract. Tropospheric glyoxal and formaldehyde columns retrieved from the SCIAMACHY satellite instrument in 2005 are used with the IMAGESv2 global chemistry-transport model and its adjoint in a two-compound inversion scheme designed to estimate the continental source of glyoxal. The formaldehyde observations provide an important constraint on the production of glyoxal from isoprene in the model, since the degradation of isoprene constitutes an important source of both glyoxal and formaldehyde. Current modelling studies underestimate largely the observed glyoxal satellite columns, pointing to the existence of an additional land glyoxal source of biogenic origin. We include an extra glyoxal source in the model and we explore its possible distribution and magnitude through two inversion experiments. In the first case, the additional source is represented as a direct glyoxal emission, and in the second, as a secondary formation through the oxidation of an unspecified glyoxal precursor. Besides this extra source, the inversion scheme optimizes the primary glyoxal and formaldehyde emissions, as well as their secondary production from other identified non-methane volatile organic precursors of anthropogenic, pyrogenic and biogenic origin. In the first inversion experiment, the additional direct source, estimated at 36 Tg/yr, represents 38% of the global continental source, whereas the contribution of isoprene is equally important (30%), the remainder being accounted for by anthropogenic (20%) and pyrogenic fluxes. The inversion succeeds in reducing the underestimation of the glyoxal columns by the model, but it leads to a severe overestimation of glyoxal surface concentrations in comparison with in situ measurements. In the second scenario, the inferred total global continental glyoxal source is estimated at 108 Tg/yr, almost two times higher than the global a priori source. The extra secondary source is the largest contribution to the global glyoxal budget (50%), followed by the production from isoprene (26%) and from anthropogenic NMVOC precursors (14%). A better performance is achieved in this case, as the updated emissions allow for a satisfactory agreement of the model with both satellite and in situ glyoxal observations.