A Common Representative Intermediates (CRI) mechanism for VOC degradation. Part 3: Development of a secondary organic aerosol module
A Common Representative Intermediates (CRI) mechanism for VOC degradation. Part 3: Development of a secondary organic aerosol module
复制标题
DOI：
10.1016/j.atmosenv.2009.01.008
复制
发表时间：
2009-04
影响因子：
5
通讯作者：
S. Utembe;L. Watson;D. Shallcross;M. Jenkin
中科院分区：
文献类型：
--
作者：
S. Utembe;L. Watson;D. Shallcross;M. Jenkin
一个光化学轨迹模型（PTM），包含主化学机制版本3.1（MCM v3.1）再加上365含氧产品物种的气体气溶胶吸收分区的优化表示，已被用来模拟质量浓度的二次有机气溶胶（SOA）的条件下的TORCH-2003运动在英国东南部在2003年7月下旬和8月。一个全面的参考数据集的50个案例研究的到来事件（和4750个相关的每小时的空气质量的历史事件）已被编译，它认为是基本情况下的条件和情景中，人为污染的排放量已减少了高达100的因素。SOA来自人为和生物的前体的相对贡献的范围内的条件下，这些模拟组件的组成进行了讨论的平均分子式，原子比（H/C，O/C和N/C）和有机气溶胶质量有机碳质量比（OM/OC），这是比较报告的测量。MCM v3.1数据集已被用作开发和优化简化（14种）SOA模块的参考基准，用于与第2版共同代表性中间体机制（CRI v2）一起使用，在前两篇配套论文的第一篇中描述[Jenkin，M.E.，洛杉矶的沃森Utembe，S.R.，Shallcross，D.E.，2008年a。VOC降解的常见代表性中间体（CRI）机制。第一部分：气相机理的发展。大气环境，42页。7185-7195. doi：10.1016/j.atmosenv.2008.07.028.]。由此产生的版本的PTM包含CRI v2和减少SOA模块已被用来模拟整个TORCH-2003运动在每小时的分辨率，和来自人为和生物的前体SOA的贡献，并进行了讨论。简化的SOA模块还被示出与最简化的CRI变体（CRI v2-R5）兼容，该变体在前两篇配套论文的第二篇中描述[沃森，L.A.，Shallcross，D.E.，Utembe，S.R.，詹金法医2008. VOC降解的常见代表性中间体（CRI）机制。第2部分：气相机理还原。大气环境，42页。7196-7204. doi：10.1016/j.atmosenv.2008.07.034.]，这被认为适合作为全球模拟中的可追踪参考机制。
A Photochemical Trajectory Model (PTM), containing the Master Chemical Mechanism version 3.1 (MCM v3.1) coupled with an optimised representation of gas–aerosol absorptive partitioning of 365 oxygenated product species, has been used to simulate mass concentrations of secondary organic aerosol (SOA) for the conditions of the TORCH-2003 campaign in the south-east UK in late July and August 2003. A comprehensive reference dataset of 50 case study arrival events (and 4750 associated hourly air mass history events) has been compiled, which considers the base case conditions and scenarios in which emissions of anthropogenic pollution have been reduced by factors of up to 100. The relative contributions of SOA derived from anthropogenic and biogenic precursors are presented for the range of conditions, and the composition of these simulated components is discussed in terms of average molecular formulae, atomic ratios (H/C, O/C and N/C) and organic aerosol mass to organic carbon mass ratios (OM/OC), which are compared to reported measurements. The MCM v3.1 dataset has been used as a reference benchmark for development and optimisation of a reduced (14 species) SOA module for use with version 2 the Common Representative Intermediates mechanism (CRI v2), described in the first of two preceding companion papers [Jenkin, M.E., Watson, L.A., Utembe, S.R., Shallcross, D.E., 2008a. A Common Representative Intermediates (CRI) mechanism for VOC degradation. Part 1: gas phase mechanism development. Atmospheric Environment, 42, pp. 7185–7195. doi:10.1016/j.atmosenv.2008.07.028.]. The resultant version of the PTM containing CRI v2 and the reduced SOA module has been used to simulate the entire TORCH-2003 campaign at hourly resolution, and the contributions of SOA derived from anthropogenic and biogenic precursors are presented and discussed. The reduced SOA module is also shown to be compatible with the most reduced CRI variant (CRI v2-R5), described in the second of two preceding companion papers [Watson, L.A., Shallcross, D.E., Utembe, S.R., Jenkin, M.E., 2008. A Common Representative Intermediates (CRI) mechanism for VOC degradation. Part 2: gas phase mechanism reduction. Atmospheric Environment, 42, pp. 7196–7204. doi:10.1016/j.atmosenv.2008.07.034.], which is considered appropriate as a traceable reference mechanism in global simulations.