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First space-based derivation of the global atmospheric methanol emission fluxes

机译:基于空间的全局大气甲醇排放通量的推导

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This study provides improved methanol emission estimates on the global scale, in particular for the largest methanol source, the terrestrial biosphere, and for biomass burning. To this purpose, one complete year of spaceborne measurements of tropospheric methanol columns retrieved for the first time by the thermal infrared sensor IASI aboard the MetOp satellite are compared with distributions calculated by the IMAGESv2 global chemistry-transport model. Two model simulations are performed using a priori biogenic methanol emissions either from the new MEGANv2.1 emission model, which is fully described in this work and is based on net ecosystem flux measurements, or from a previous parameterization based on net primary production by Jacob et al. (2005). A significantly better model performance in terms of both amplitude and seasonality is achieved through the use of MEGANv2.1 in most world regions, with respect to IASI data, and to surface- and air-based methanol measurements, even though important discrepancies over several regions are still present. As a second step of this study, we combine the MEGANv2.1 and the IASI column abundances over continents in an inverse modelling scheme based on the adjoint of the IMAGESv2 model to generate an improved global methanol emission source. The global optimized source totals 187 Tg yr1 with a contribution of 100 Tg yr1 from plants, only slightly lower than the a priori MEGANv2.1 value of 105 Tg yr1. Large decreases with respect to the MEGANv2.1 biogenic source are inferred over Amazonia (up to 55 %) and Indonesia (up to 58 %), whereas more moderate reductions are recorded in the Eastern US (20–25 %) and Central Africa (25–35 %). On the other hand, the biogenic source is found to strongly increase in the arid and semi-arid regions of Central Asia (up to a factor of 5) and Western US (factor of 2), probably due to a source of methanol specific to these ecosystems which is unaccounted for in the MEGANv2.1 inventory. The most significant error reductions achieved by the optimization concern the derived biogenic emissions over the Amazon and over the Former Soviet Union. The robustness of the derived fluxes to changes in convective updraft fluxes, in methanol removal processes, and in the choice of the biogenic a priori inventory is assessed through sensitivity inversions. Detailed comparisons of the model with a number of aircraft and surface observations of methanol, as well as new methanol measurements in Europe and in the Reunion Island show that the satellite-derived methanol emissions improve significantly the agreement with the independent data, giving thus credence to the IASI dataset.
机译:该研究提供了对全球规模的改善的甲醇排放估计,特别是对于最大的甲醇源,陆地生物圈以及生物量燃烧。为此目的,通过热红外传感器IASI首次检出的对流层甲醇柱的整个星载液的全年空间甲醇柱的乘坐卫星进行了比较了由由ImpliceV2全球化学传输模型计算的分布。使用来自新兆瓦52.1发射模型的先验生物甲醇排放进行了两种模型模拟,该模型在这项工作中完全描述,并且基于净生态系统磁通测量,或根据jacob et的净初级生产的先前参数化。 al。 (2005)。通过在大多数世界地区使用Meganv2.1,在大多数世界地区以及表面和空气基甲醇测量中,实现了幅度和季节性方面的显着更好的模型性能,即使几个地区的重要差异也是如此仍然存在。作为本研究的第二步,我们将梅根夫柱和IASI柱丰度与逆建模方案相结合,基于图像V2模型的伴随,以产生改进的全局甲醇发射源。全球优化的源总计187 TG YR1,源于植物100 TG YR1,仅略低于先验的Meganv2.1值105 Tg YR1。梅亨夫52.1生物源的大幅减少是在亚马逊(高达55%)和印度尼西亚(高达58%)上的(高达58%),而在美国东部(20-25%)和中非录得更温和的减少( 25-35%)。另一方面,生物源被发现在中亚的干旱和半干旱地区(高达5倍)和美国西部(因子2)的生物源强烈增加,可能是由于特异性甲醇的来源这些生态系统在Meganv2.1库存中未占用。优化实现的最显着的错误减少涉及亚马逊和前苏联的源性生物排放。通过灵敏度反转评估甲醇去除过程中的导流助熔剂对对流上升助熔剂变化的稳健性,以及在生物生成的先验清单中进行评估。具有多种飞机和甲醇表面观察的模型的详细比较,以及欧洲和团聚岛的新甲醇测量表明,卫星衍生的甲醇排放与独立数据的协议大大提高了,从而使信任IASI数据集。
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