Simulating secondary organic aerosol in a 3-D Lagrangian chemistry transport model using the reduced Common Representative Intermediates mechanism (CRI v2-R5)
Simulating secondary organic aerosol in a 3-D Lagrangian chemistry transport model using the reduced Common Representative Intermediates mechanism (CRI v2-R5)
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使用简化的通用代表中间体机制 (CRI v2-R5) 在 3-D 拉格朗日化学传输模型中模拟二次有机气溶胶
DOI：
10.1016/j.atmosenv.2010.11.046
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发表时间：
2011
影响因子：
5
通讯作者：
Utembe S
中科院分区：
文献类型：
--
作者：
Utembe S
二次有机气溶胶（SOA）的代码，加上减少共同代表性中间体的化学机制（CRI v2-R5），已被用于全球3-D化学传输模式，STOCHEM，模拟有机气溶胶（OA）的质量负荷的全球分布。SOA代码代表了人为、生物源和生物质燃烧源排放的各种有机前体经过几代氧化形成的产品的气体-气溶胶分配。该模型还包括基于AeroCom清单和全球火灾排放数据库（GFED）的初级有机气溶胶（POA）排放。POA，0.89Tg和SOA，0.23Tg的计算负担，是在以前的建模研究中报告的值的范围内。计算出的SOA年原位产量为22.5Tgyr-1，福尔斯其他模型计算的8- 110 Tgyr-1范围内，但略低于最近报道的观测约束自上而下的估计。研究发现，生物前体的氧化约占全球SOA负担的90%，这对热带森林地区模拟的最高年平均表面OA浓度（高达8μgm−3）做出了重大贡献。模拟的OA质量负荷与来自不同位置的表面观测结果的比较表明OA分布的良好描述，但平均低估了约3倍。持续形成的SOA到自由对流层模拟，在对流层上层的萜烯氧化的第二代和第三代产品的重要贡献。从ACE-亚洲运动的垂直剖面的模拟OA质量负荷的比较表明，OA与海拔高度的相对变化的一个很好的描述，但一致低估约5倍。虽然全球源强度的绝对大小被低估，但这种一致性仍然提供了支持的重要作用，多代氧化化学作为一个大的SOA源在自由对流层，并提供证据的必要性，代表可凝结的材料形成了几代VOC氧化在全球化学传输模型。
A secondary organic aerosol (SOA) code, coupled to the reduced Common Representative Intermediates chemical mechanism (CRI v2-R5), has been used in the global 3-D chemistry-transport model, STOCHEM, to simulate the global distribution of organic aerosol (OA) mass loadings. The SOA code represents the gas-to-aerosol partitioning of products formed over several generations of oxidation of a variety of organic precursors emitted from anthropogenic, biogenic and biomass burning sources. The model also includes emissions of primary organic aerosol (POA), based on the AeroCom inventory and the Global Fire Emissions database (GFED). The calculated burdens for POA, 0.89Tg, and SOA, 0.23Tg, are well within the range of values that have been reported in previous modelling studies. The calculated SOA annual in-situ production of 22.5Tgyr−1also falls within the 8–110Tgyr−1range calculated by other models, but is somewhat lower than observationally-constrained top-down estimates which have been reported recently. The oxidation of biogenic precursors is found to account for about 90% of the global SOA burden, and this makes a substantial contribution to the highest annual mean surface OA concentrations (up to 8μgm−3), which are simulated in tropical forested regions. Comparison of the simulated OA mass loadings with surface observations from a variety of locations indicate a good description of the OA distribution, but with an average underestimation of about a factor of 3. Sustained formation of SOA into the free troposphere is simulated, with important contributions from second and third-generation products of terpene oxidation in the upper troposphere. Comparison of the simulated OA mass loadings with vertical profiles from the ACE-Asia campaign indicates a very good description of the relative variation of OA with altitude, but with consistent underestimation of about a factor of 5. Although the absolute magnitude of the global source strength is underestimated, this consistency nonetheless provides support for an important role for multigenerational oxidation chemistry as a large source of SOA in the free troposphere, and lends credence to the necessity of representing condensable material formed over several generations of VOC oxidation in global chemistry-transport models.
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影响因子：
6.3
作者：
C. Luo
通讯作者：
C. Luo
3-D 拉格朗日化学输运模型中二次颗粒物的全球分布
影响因子：
2
作者：
R. Derwent;W. Collins;Michael E. Jenkin;C. E. Johnson;D. Stevenson
通讯作者：
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影响因子：
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作者：
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通讯作者：
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DOI：
--
发表时间：
1994
期刊：
影响因子：
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作者：
D. Murphy;D. Fahey
通讯作者：
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影响因子：
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作者：
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通讯作者：
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