Production of Aerosol paRticle orgAnic Matter in ClOUds: chamber and laboratory studies, mechanisms, modelling and iNTegration

云中气溶胶颗粒有机物质的产生：室和实验室研究、机制、建模和集成

• 批准号: 407135662
• 负责人: Professor Dr. Hartmut Herrmann
• 金额: --
• 依托单位: Leibniz-Institut für Troposphärenforschung e.V. (TROPOS)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2018
• 资助国家: 德国
• 起止时间: 2017-12-31 至 2022-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/407135662?language=en
• 关键词: Production; Aerosol; paRticle; orgAnic; Matter

Recently, chemical processes in clouds have been suggested to contribute substantially to organic aerosol particle mass. Recent evidence from the HCCT-2010 field study and the CUMULUS chamber study suggest that this organic mass production can be substantial and depends on the concentration of available organic precursor compounds in the gas phase. However, considerable uncertainties exist, e.g. with regards to the nature of the resulting aerosol particles which might be metastable and loose at least part of their OM content during the cloud droplet evaporation. Hence, PARAMOUNT is aimed at the investigation of cloud processes which are able to process organic constituents and produce organic aerosol particle mass. The project will focus on the multiphase chemistry of very relevant polyfunctional precursors such as polyfunctional carbonyls and acids. With these precursors, a combination of aqueous-phase laboratory and CESAM chamber studies will be undertaken to examine the multiphase cloud processing. Firstly, aqueous-phase laboratory studies will lay the groundwork with regard to kinetics and mechanisms of the multiphase processing of the mentioned compounds. Then, the suggested CESAM chamber experiments, which are central in PARAMOUNT, will focus on studying the organic mass production by the chemical in-cloud processing of these compounds one by one, grouped or with mixtures with all of them. The planned chamber studies will use different seeds and oxidant precursors to examine the organic mass production under different environmental and diurnal conditions. The organic mass increase during the cloud episodes will be investigated. Besides the organic mass formation, the partitioning of organic compounds under cloud conditions should be studied to evaluate possible enrichments of organic carbonyl compounds observed during the cloud field campaign HCCT-2010. The organic aerosol fraction will be analysed on-line by two Aerosol Mass Spectrometer instruments and the processing of the interstitial gas phase and the phase partitioning will be investigated by PTR-MS and the use of a mini CVI (counter virtual impactor) followed by off-line analysis. Finally, the performed CESAM experiments are being modelled with the complex multiphase chemistry mechanism MCM/CAPRAM. The multiphase modelling will be performed to both validate the mechanism and support the interpretation of the chamber experiments. Overall, the proposed project PARAMOUNT will be a scientific breakthrough for understanding of in-cloud processes clarifying the role of clouds for atmospheric organic aerosol mass production.

最近，已经提出云中的化学过程对有机气溶胶颗粒质量产生了重大贡献。 HCCT-2010现场研究和积云室研究的最新证据表明，这种有机质量产生可能是实质的，并且取决于气相中可用的有机前体化合物的浓度。但是，存在相当大的不确定性，例如关于所得的气溶胶颗粒的性质，在云滴蒸发过程中可能是可稳定且至少一部分OM含量的情况下。因此，派拉蒙旨在研究能够处理有机成分并产生有机气溶胶颗粒质量的云过程。该项目将集中于非常相关的多功能前体（例如多功能羰基和酸）的多相化学。对于这些前体，将进行水相实验室和CESAM腔室研究的结合，以检查多相云处理。首先，水相实验室研究将基于上述化合物的多相处理的动力学和机制奠定基础。然后，建议的CESAM腔室实验是尤其是派拉蒙的中心，将重点介绍通过对这些化合物的化学云中的加工来研究有机质量的产生，一一分组或与所有这些化合物一起进行分组或混合物。计划的腔室研究将使用不同的种子和氧化剂前体来检查不同环境和昼夜条件下的有机质量产生。将研究云发作期间的有机质量增加。除了有机质量形成外，还应研究有机化合物在云条件下的分配，以评估在2010年云现场活动期间观察到的有机羰基化合物的可能富集。有机气雾分数将通过两种气溶胶质谱仪仪器在线分析，并且将通过PTR-MS研究间质气相和相分配的处理，并使用Mini CVI（计数器虚拟撞击器），然后使用。 - 线分析。最后，用复杂的多相化学机制MCM/CAPRAM对执行的CESAM实验进行了建模。将进行多相建模，以验证机制并支持腔室实验的解释。总体而言，拟议的项目至高无上将是理解云端过程的科学突破，阐明了云在大气有机气雾剂质量生产中的作用。