The CRI v2.2 reduced degradation scheme for isoprene
The CRI v2.2 reduced degradation scheme for isoprene
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DOI：
10.1016/j.atmosenv.2019.05.055
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发表时间：
2019-09-01
影响因子：
5
通讯作者：
Rickard, A. R.
中科院分区：
文献类型：
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作者：
Jenkin, M. E.;Khan, M. A. H.;Rickard, A. R.
使用主化学机制（MCM v3.3.1）作为参考基准，系统地更新了通用代表性中间体（CRI）机制中异戊二烯降解的简化表示，更新后的机制将作为CRI v2.2发布。在CRI v2.2中，异戊二烯的完全降解机制包括56种封闭壳和自由基的186个反应，与MCM v3.3.1相比，这在尺寸上减小了一个数量级。处理了OH自由基、NO3自由基和臭氧（O-3）反应引发的化学反应。在报告的动力学和机械信息的背景下，提供了更新的概述。这些修订主要涉及oh引发的化学，它往往在大气条件下占主导地位，尽管这些修订包括对O-3（-）和no3引发氧化产生的产物化学的更新。这些修订对一些关键领域产生了影响，包括HOx和NOx的回收。在一系列相关条件下，利用热带森林边界层的箱形模型，将CRI v2.2异戊二烯机制的性能与之前版本（CRI v2.1）和参考MCM v3.3.1进行了比较。此外，还进行了测试，以确保MCM v3.3.1的性能对最近报告的信息保持稳定。CRI v2.2也已被实现到STOCHEM化学输运模型中，并在EMEP MSC-W化学输运模型中实现了CRI v2.2的定制版本。这些研究的结果被用来说明HOx自由基浓度的机制更新在全球范围内的影响。
The reduced representation of isoprene degradation in the Common Representative Intermediates (CRI) mechanism has been systematically updated, using the Master Chemical Mechanism (MCM v3.3.1) as a reference benchmark, with the updated mechanism being released as CRI v2.2. The complete isoprene degradation mechanism in CRI v2.2 consists of 186 reactions of 56 closed shell and free radical species, this being an order of magnitude reduction in size compared with MCM v3.3.1. The chemistry initiated by reaction with OH radicals, NO3 radicals and ozone (O-3) is treated. An overview of the updates is provided, within the context of reported kinetic and mechanistic information. The revisions mainly relate to the OH-initiated chemistry, which tends to dominate under atmospheric conditions, although these include updates to the chemistry of products that are also generated from the O-3(-) and NO3-initiated oxidation. The revisions have impacts in a number of key areas, including recycling of HOx and NOx. The performance of the CRI v2.2 isoprene mechanism has been compared with those of the preceding version (CRI v2.1) and the reference MCM v3.3.1 over a range of relevant conditions, using a box model of the tropical forested boundary layer. In addition, tests are carried out to ensure that the performance of MCM v3.3.1 remains robust to more recently reported information. CRI v2.2 has also been implemented into the STOCHEM chemistry-transport model, with a customized close-variant of CRI v2.2 implemented into the EMEP MSC-W chemistry-transport model. The results of these studies are presented and used to illustrate the global-scale impacts of the mechanistic updates on HOx radical concentrations.