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Advanced Chemical process Modelling of aqSOA (ACoMa)

aqSOA 的高级化学过程建模 (ACoMa)

基本信息

批准号：
281607657
负责人：
Dr. Andreas Tilgner
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：
2015
资助国家：
德国
起止时间：
2014-12-31 至 2018-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/281607657?language=en
关键词：
Advanced Chemical process Modelling aqSOA

项目摘要

Organic aerosols (OA) represent an ubiquitous major component of atmospheric aerosols affecting numerous atmospheric processes and environmental issues. The quantitative assessment of, e.g., climate effects remains hampered by a number of factors, including an incomplete understanding of how emitted VOCs contribute to the formation of atmospheric OA. A huge fraction of OA is formed secondarily (secondary organic aerosol (SOA)) in the atmosphere through gas phase chemical processes including subsequent gas-to-particle partitioning (gasSOA) or through aqueous phase chemical processes (aqSOA). However, by means of pure gas phase chemistry approaches, the properties of the ambient SOA cannot be explained. Furthermore, gasSOA approaches tend to underestimate the overall SOA. From several laboratory and field studies, it was concluded that the aqSOA formation might have the same importance than the gasSOA formation. Thus, there is a growing attention on aqueous phase processes contributing to the SOA. But, the chemical aqSOA processing, i.e. secondary formation and aging of aqueous OA, remains poorly understood and considered in current multiphase chemical mechanisms. To further address this scientific issue, further investigations with more detailed multiphase chemistry mechanisms and advanced process models are needed to predict more accurately photochemical processes of organic compounds in the atmospheric aqueous phases.In order to improve the current understanding of the aqSOA processing and their importance for the tropospheric chemistry and its related scientific issues, the present project aims at the development of an advanced aqSOA chemical mechanism and an advanced multiphase model. The model should near-explicitly treat the inorganic/organic chemistry in both the gas phase and aqueous phase including radical and non-radical chemistry of organic compounds. Moreover, the aimed advanced multiphase process model will sufficiently treats complex/salt formation processes and non-ideal solution effects. By means of such an advanced multiphase model the tropospheric chemical aqSOA processing will be investigated in detail by accompanied model studies. The proposed model studies will focus mainly on (i) the identification of the main aqSOA formation pathways, (ii) the importance of radical, non-radical and non-oxidative processes for aqSOA within different environmental regimes and (iii) the importance of interactions of organic compounds with inorganics for their tropospheric resistance time. Overall, by means of the advanced multiphase model framework and the projected model studies, new insights will be provided into aqSOA processing, its importance for the overall particulate OM formation and the link to other important tropospheric chemistry issues such as the tropospheric oxidation capacity.

有机气溶胶是大气气溶胶中普遍存在的主要成分，影响着众多的大气过程和环境问题。定量评估，例如，气候影响仍然受到许多因素的阻碍，包括对排放的VOC如何促进大气OA形成的不完全理解。大部分的OA是通过气相化学过程（包括随后的气体-颗粒分配（gasSOA）或通过水相化学过程（aqSOA））在大气中二次形成的（二次有机气溶胶（SOA））。然而，通过纯气相化学的方法，周围的SOA的属性无法解释。此外，gasSOA方法往往低估了整体SOA。从几个实验室和现场研究，得出的结论是，aqSOA形成可能具有相同的重要性比gasSOA形成。因此，有一个越来越多的关注水相过程有助于SOA。但是，化学aqSOA处理，即水OA的二次形成和老化，仍然很少了解和考虑在当前的多相化学机制。为了进一步解决这一科学问题，需要进一步研究更详细的多相化学机制和先进的过程模型，以更准确地预测大气水相中有机化合物的光化学过程，以提高目前对aqSOA过程及其对对流层化学及其相关科学问题的重要性的认识。本项目旨在开发先进的aqSOA化学机理和先进的多相模型。该模型应接近明确地处理在气相和水相中的无机/有机化学，包括有机化合物的自由基和非自由基化学。此外，目标先进的多相过程模型将充分处理复杂/盐形成过程和非理想溶液效应。通过这种先进的多相模式对流层化学aqSOA处理将详细研究伴随模式研究。拟议的模式研究将主要集中在（一）的主要aqSOA形成途径的识别，（二）的重要性，自由基，非自由基和非氧化过程的aqSOA在不同的环境制度和（iii）的重要性，有机化合物与无机物的相互作用，其对流层阻力时间。总体而言，通过先进的多相模型框架和预测的模型研究，新的见解将提供到aqSOA处理，其整体颗粒OM形成的重要性和其他重要的对流层化学问题，如对流层氧化能力的联系。