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CMAQv4.7 中二次有机气溶胶的模型表示。

Model representation of secondary organic aerosol in CMAQv4.7.

机构信息

U.S. Environmental Protection Agency, Research Triangle Park, North Carolina 27711, USA.

出版信息

Environ Sci Technol. 2010 Nov 15;44(22):8553-60. doi: 10.1021/es100636q.

Abstract

Numerous scientific upgrades to the representation of secondary organic aerosol (SOA) are incorporated into the Community Multiscale Air Quality (CMAQ) modeling system. Additions include several recently identified SOA precursors: benzene, isoprene, and sesquiterpenes; and pathways: in-cloud oxidation of glyoxal and methylglyoxal, particle-phase oligomerization, and acid enhancement of isoprene SOA. NO(x)-dependent aromatic SOA yields are also added along with new empirical measurements of the enthalpies of vaporization and organic mass-to-carbon ratios. For the first time, these SOA precursors, pathways and empirical parameters are included simultaneously in an air quality model for an annual simulation spanning the continental U.S. Comparisons of CMAQ-modeled secondary organic carbon (OC(sec)) with semiempirical estimates screened from 165 routine monitoring sites across the U.S. indicate the new SOA module substantially improves model performance. The most notable improvement occurs in the central and southeastern U.S. where the regionally averaged temporal correlations (r) between modeled and semiempirical OC(sec) increase from 0.5 to 0.8 and 0.3 to 0.8, respectively, when the new SOA module is employed. Wintertime OC(sec) results improve in all regions of the continental U.S. and the seasonal and regional patterns of biogenic SOA are better represented.

摘要

众多科学升级版本的二次有机气溶胶 (SOA) 被纳入到了综合空气质量模型 (CMAQ) 系统中。新增内容包括几种最近被识别的 SOA 前体物:苯、异戊二烯和半萜烯;以及反应途径:包括气溶胶水相氧化过程中的乙二醛和甲基乙二醛、颗粒相中低聚物的形成过程、异戊二烯 SOA 的酸增强过程。还添加了与芳香族 SOA 产率相关的氮氧化物 (NOx),以及蒸发焓和有机碳质量与碳比值的新的经验测量值。这是首次将这些 SOA 前体物、反应途径和经验参数同时应用于涵盖美国大陆的年度空气质量模型模拟中。将 CMAQ 模型模拟的二次有机碳 (OC(sec)) 与从美国各地 165 个常规监测站点筛选出的半经验估算值进行比较表明,新的 SOA 模块大大提高了模型性能。最显著的改进发生在美国中部和东南部地区,当使用新的 SOA 模块时,模型模拟的和半经验估算的 OC(sec)之间的区域平均时间相关性 (r) 分别从 0.5 增加到 0.8 和从 0.3 增加到 0.8。在美国大陆的所有地区,冬季 OC(sec) 的结果都得到了改善,并且更好地体现了生物源 SOA 的季节性和区域性模式。

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