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Quantifying global terrestrial methanol emissions using observations from the TES satellite sensor

机译:使用来自TES卫星传感器的观测定量全球陆地甲醇排放

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We employ new global space-based measurements of atmospheric methanol from the Tropospheric Emission Spectrometer (TES) with the adjoint of the GEOS-Chem chemical transport model to quantify terrestrial emissions of methanol to the atmosphere. Biogenic methanol emissions in the model are based on version 2.1 of the Model of Emissions of Gases and Aerosols from Nature (MEGANv2.1), using leaf area data from NASA's Moderate Resolution Imaging Spectroradiometer (MODIS) and GEOS-5 assimilated meteorological fields. We first carry out a pseudo observation test to validate the overall approach, and find that the TES sampling density is sufficient to accurately quantify regional- to continental-scale methanol emissions using this method. A global inversion of two years of TES data yields an optimized annual global surface flux of 122 Tg yr?1 (including biogenic, pyrogenic, and anthropogenic sources), an increase of 60% from the a priori global flux of 76 Tg yr?1. Global terrestrial methanol emissions are thus nearly 25% those of isoprene (~540 Tg yr?1), and are comparable to the combined emissions of all anthropogenic volatile organic compounds (~100–200 Tg yr?1). Our a posteriori terrestrial methanol source leads to a strong improvement of the simulation relative to an ensemble of airborne observations, and corroborates two other recent top-down estimates (114–120 Tg yr1) derived using in situ and space-based measurements. Inversions testing the sensitivity of optimized fluxes to model errors in OH, dry deposition, and oceanic uptake of methanol, as well as to the assumed a priori constraint, lead to global fluxes ranging from 118 to 126 Tg yr?1. The TES data imply a relatively modest revision of model emissions over most of the tropics, but a significant upward revision in midlatitudes, particularly over Europe and North America. We interpret the inversion results in terms of specific source types using the methanol : CO correlations measured by TES, and find that biogenic emissions are overestimated relative to biomass burning and anthropogenic emissions in central Africa and southeastern China, while they are underestimated in regions such as Brazil and the US. Based on our optimized emissions, methanol accounts for 25% of the photochemical source of CO and HCHO over many parts of the northern extratropics during springtime, and contributes ~6% of the global secondary source of those compounds annually.
机译:我们采用从对流层发射光谱仪(TES)的大气甲醇的新的全球性的空间探测与GEOS-CHEM化学输送模式的伴随量化甲醇的陆地排放到大气中。在模型中的生物甲醇的排放是基于气体和气溶胶的排放从自然(MEGANv2.1)模型的2.1版本,使用来自NASA的中分辨率成像光谱仪(MODIS)叶面积数据和GEOS-5同化气象字段。我们首先进行的伪观察试验,以验证整体方法,并且发现该TES抽样密度足够准确量化区域到使用这种方法大陆尺度甲醇的排放。两年TES数据率122的Tg年的优化每年全球表面的磁通的全局反演?1(包括生物,热解,和人为来源),从76的Tg年的先验全球通量增加60%?1 。全球陆地甲醇排放因此近25%的那些异戊二烯(〜540的Tg年?1)的,并且是可比较的所有的人为的挥发性有机化合物的组合发射(〜100-200的Tg年?1)。我们的后验地面甲醇源引线相对于机载观测的集合的模拟的强改善,证实了其他两个最近自上而下估计(114-120的Tg YR1)使用原位和基于空间的测量中导出。反转测试优化的通量,以OH模型误差,干燥沉积,和甲醇的海洋摄取的敏感性,以及对假定先验约束,导致全球通量范围从118到126的Tg年?1。该TES的数据暗示模型排放量在大部分热带地区的相对温和的调整,但在中纬度地区一个显著上调,特别是在欧洲和北美。我们解释在使用甲醇特定源类型方面反演结果:由TES测量CO的相关性,并且发现,生物排放相对于生物质燃烧和在非洲中部和中国东南部人为排放高估,而它们在区域如低估巴西和美国。根据我们的优化排放,甲醇在春天占CO和HCHO的在北温带的许多部分光化学源的> 25%,并且有助于〜6的那些化合物的全球辅助源的每年%。

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