实验室模拟大气中醛类与硫酸铵及胺类的液相反应研究

发布时间：2018-01-04 01:41

本文关键词：实验室模拟大气中醛类与硫酸铵及胺类的液相反应研究　出处：《山东大学》2015年硕士论文　论文类型：学位论文

【摘要】：大气中气溶胶根据来源分为一次气溶胶和二次气溶胶。大气中挥发性有机物可以通过气相反应或者云雾水及颗粒物的液相反应形成二次有机气溶胶。实验选取乙醇醛、苯甲醛及异丁烯醛作为研究对象,分别模拟研究云水或颗粒相中与硫酸铵、甲胺及甘氨酸的液相反应。乙醇醛、苯甲醛及异丁烯醛是大气中挥发性有机物(异戊二烯、甲苯等)光氧化反应的重要产物。硫酸铵是大气环境中含量较大且化学性质稳定的无机盐。甘氨酸是大气气溶胶中含量最多的游离氨基酸。烷基胺是大气中较为普遍的含氮化合物,甲胺是其中最简单的有机含氮化合物。研究乙醇醛、苯甲醛及异丁烯醛与硫酸铵、甲胺及甘氨酸液相反应产生二次有机气溶胶,一方面可以进一步完善液相反应生成二次有机气溶胶过程的相关内容,另一方面可以加深对反应产物的形成过程及产物的光学性质的理解,对于预测大气环境中的二次有机气溶胶的液相形成及研究其对能见度及气候影响具有重要意义。本研究的主要内容为：模拟大气云水或颗粒相中乙醇醛、苯甲醛及异丁烯醛分别与硫酸铵、甲胺及甘氨酸反应产生二次有机气溶胶的过程及产物的光学性质。具体包括：(1)研究不同浓度乙醇醛与硫酸铵、甲胺和甘氨酸的反应,通过紫外-可见吸收谱研究产物的光学性质,通过质谱分析可能的产物。此外,为了研究硫酸铵、甲胺及甘氨酸之间的相互影响,研究了硫酸铵、甲胺及甘氨酸混合后与乙醇醛的反应。(2)研究苯甲醛与硫酸铵、甲胺及甘氨酸的反应。(3)研究异丁烯醛与硫酸铵、甲胺及甘氨酸的反应。结果表明,相同浓度下乙醇醛与甘氨酸反应产生吸光产物的速度最快,且量最大,甲胺次之,硫酸铵最慢,其中主要发生醇醛缩合、缩醛及生成亚胺反应。苯甲醛可以与硫酸铵、甲胺及甘氨酸发生反应,但反应速度较慢,对二次有机气溶胶的贡献较小。异丁烯醛与硫酸铵、甲胺没有反应,与甘氨酸的反应较为缓慢,对二次有机气溶胶的形成贡献很小。
[Abstract]:Aerosols in the atmosphere can be divided into primary aerosol and secondary aerosol according to their source. Volatile organic compounds in the atmosphere can be formed by aerosol reaction or liquid phase reaction of cloud water and particulate matter. Aldehydes. Benzaldehyde and isobutenaldehyde were used to simulate the liquid phase reaction of ammonium sulfate, methylamine and glycine in cloud water or granular phase. Benzaldehyde and isobutenaldehyde are volatile organic compounds (isoprene) in the atmosphere. Toluene et al.). Ammonium sulfate is an inorganic salt with high content and stable chemical properties in the atmospheric environment. Glycine is the most abundant free amino acid in atmospheric aerosol. Alkylamine is the most common amino acid in the atmosphere. Nitrogen compounds. Methylamine is the simplest organic nitrogen-containing compound. The secondary organic aerosol was produced by the reaction of ethanol aldehyde, benzaldehyde and isobutenal with ammonium sulfate, methylamine and glycine in liquid phase. On the one hand, it can further improve the content of the formation of secondary organic aerosol from liquid phase reaction, on the other hand, it can deepen the understanding of the formation process of the reaction products and the optical properties of the products. It is of great significance to predict the formation of secondary organic aerosols in the atmosphere and to study their effects on visibility and climate. The main contents of this study are as follows: modeling glycolaldehyde in cloud water or granular phase. The reaction of benzaldehyde and isobutenaldehyde with ammonium sulfate, methylamine and glycine to produce secondary organic aerosol and the optical properties of the product were studied. The reaction of methylamine with glycine was studied by UV-Vis absorption spectroscopy, and the possible products were analyzed by mass spectrometry. In addition, the interaction among ammonium sulfate, methylamine and glycine was studied. The reaction of ammonium sulfate, methylamine and glycine with ethanol aldehydes was studied. The reaction of benzaldehyde with ammonium sulfate, methylamine and glycine was studied. The reaction of methylamine and glycine. The results showed that the reaction of glycine with glycine at the same concentration had the fastest rate and the largest amount, followed by methylamine and ammonium sulfate, among which the condensation of alcohol and aldehydes occurred mainly. Benzaldehyde can react with ammonium sulfate, methylamine and glycine, but the reaction rate is slower and the contribution to secondary organic aerosol is small. Isobutenal has no reaction with ammonium sulfate and methylamine. The reaction with glycine is slow and has little contribution to the formation of secondary organic aerosols.
【学位授予单位】：山东大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：X513

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