Using a reduced Common Representative Intermediates (CRIv2-R5) mechanism to simulate tropospheric ozone in a 3-D Lagrangian chemistry transport model
Using a reduced Common Representative Intermediates (CRIv2-R5) mechanism to simulate tropospheric ozone in a 3-D Lagrangian chemistry transport model
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DOI：
10.1016/j.atmosenv.2010.01.044
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发表时间：
2010-04
影响因子：
5
通讯作者：
S. Utembe;M. Cooke;A. Archibald;M. Jenkin;R. Derwent;D. Shallcross
中科院分区：
文献类型：
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作者：
S. Utembe;M. Cooke;A. Archibald;M. Jenkin;R. Derwent;D. Shallcross
一个描述甲烷和22种排放的非甲烷碳氢化合物和含氧挥发性有机化合物在对流层降解形成臭氧的简化化学方案（CRIv2-R5）已被应用于全球三维化学传输模型（STOCHEM）中。该方案包含609种反应中的220种，已用于模拟1998年气象年的臭氧及其前体，并将结果与STOCHEM用原始化学方法运行的结果进行了比较。与最初的化学方案相比，CRI方案中更多活性voc的降解导致了更多nox活性储层的形成（及其随后的运输），从而导致了更多远离陆源的臭氧的形成。相反，反应性越强的挥发性有机化合物也会导致大陆地区对OH的去除越多，海洋环境中OH的形成越多。STOCHEM与CRI方案一起运行，模拟了更多的臭氧（高达10 ppb），结果与观测到的垂直臭氧分布更好地吻合。CRI方案将STOCHEM所考虑的年份的全球和年度综合臭氧预算从- 55 Tg /年的净损失转换为+50 Tg /年的净收益。
A reduced chemical scheme (CRIv2-R5) which describes ozone formation from the tropospheric degradation of methane and 22 emitted non-methane hydrocarbons and oxygenated volatile organic compounds has been applied in a global-3D chemistry transport model (STOCHEM). The scheme, which contains 220 species in 609 reactions, has been used to simulate ozone and its precursors for the meteorological year of 1998 and the results have been compared with those from STOCHEM runs with its original chemistry. Compared with the original chemistry scheme, the degradation of a larger number of more reactive VOCs in the CRI scheme results in the formation (and their consequent transportation) of more NOxactive reservoirs thus leading to formation of more ozone away from land-based sources. Conversely, the more reactive VOCs also lead to greater removal of OH in continental areas and greater formation of OH in marine environments. STOCHEM run with the CRI scheme simulates more ozone (by up to 10 ppb), which results in better agreement with observed vertical ozone profiles. The CRI scheme transforms the globally and annually integrated ozone budget for the considered year in STOCHEM from a net loss of −55 Tg yr−1to a net gain of +50 Tg yr−1.