实验室模拟大气中羰基化合物与硫酸铵/胺液相反应形成SOA的研究

项目名称： 实验室模拟大气中羰基化合物与硫酸铵/胺液相反应形成SOA的研究

项目编号： No.21507070

项目类型： 青年科学基金项目

立项/批准年度： 2016

项目学科： 化学工业

项目作者： 周学华

作者单位： 山东大学

项目金额： 20万元

中文摘要： 水相形成SOA由于能够解释传统气-粒分配理论无法解释的野外观测与模型模拟及野外观测与烟雾箱模拟SOA在颗粒大小、分布、浓度及老化程度等方面的差异，成为近年研究的热点。羰基化合物和硫酸铵/胺的液相非自由基反应是水相形成SOA的重要途径，由于其产物具有明显的光学吸收，即形成“棕碳”，在近年引起人们的广泛关注。本项目通过实验室模拟，首次全面系统地研究大气中不同类型典型羰基化合物与硫酸铵/胺液相反应形成SOA的动力学、反应机理、反应产物及产物的光学性质，从分子水平上揭示SOA的形成及吸光物种。在此基础上，归纳不同类型有机物反应规律，探究影响反应的关键因素，揭示该类反应的总反应特征。最后，评估反应产物对大气氧化性的影响及对气溶胶光吸收的贡献。本项目的开展将为研究SOA光吸收对大气辐射平衡的影响及完善当前的气候模型提供有力的基础支撑；同时，也对研究SOA光吸收引起的能见度降低，灰霾频发等具有重要意义。

中文关键词： 水相二次有机气溶胶；羰基化合物；硫酸铵/胺；形成；光学性质

英文摘要： Formation of aqueous SOA has been becoming a research hotspot in recent years due to its important roles in explaining the discrepancies between field observation and model results, field observation and chamber simulation results on size, distribution, concentration and aging degree of SOA, which can’t be understood by the traditional SOA formation through gas phase. It is an important way to form aqueous SOA by the non-radical reactions of aqueous phase carbonyl compounds and ammonium sulfate/amines. This is attaching people’s eyes in the current due to the light absorption of the reaction products, that is “brown carbon”. For the first time, this work comprehensively and systematically studies the kinetics, mechanisms, products and the light absorption characteristics of products in the reactions of aqueous carbonyl compounds and ammonium sulfate/amines in order to reveal the formation of SOA and the products with light absorption in the level of molecules in the lab. On the base, induce the reaction rules for different reactants, probe into the key factors influencing reactions and reveal the total characteristics of reactions. Last, evaluate the influence of light absorption of the products on the oxidability of the atmosphere and the contribution of the light absorption of products to the light absorption of aerosol. These will provide the strongly fundamental support for the study of the influence of SOA light absorption on the radiative balance of atmosphere and improving the current climate model. At the same time, it also has a great significance in studying the visibility degradation and frequent haze.

英文关键词： aqueous SOA;carbonyl compound;ammonium sulfate/amine;formaton;optical characteristics