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氨与甲苯SOA形成含氮有机物的影响因素研究

Study on the factors affecting the formation of nitrogen-containing organic compounds formed from ammonia and toluene secondary organic aerosol

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【作者】 徐俊黄明强冯状状蔡顺有赵卫雄胡长进顾学军张为俊

【Author】 XU Jun;HUANG Ming-qiang;FENG Zhuang-zhuang;CAI Shun-you;ZHAO Wei-xiong;HU Chang-jin;GU Xue-jun;ZHANG Wei-jun;College of Chemistry & Chemical Engineering and Environment, Minnan Normal University, Fujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology;Laboratory of Atmospheric Physico-Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences;

【通讯作者】 黄明强;

【机构】 闽南师范大学化学化工与环境学院福建省现代分离分析科学与技术重点实验室中国科学院安徽光学精密机械研究所大气物理化学实验室

【摘要】 利用自制的烟雾腔系统使臭氧光解产生OH自由基,启动甲苯光氧化产生二次有机气溶胶(SOA)粒子,在不同的实验条件下研究甲苯SOA与氨反应形成的含氮有机物,并采用紫外-可见分光光度计测量反应产物溶液在205和270nm处的吸光度,探究光照时间、甲苯、氨、臭氧浓度和相对湿度等环境因素对含氮有机物形成的影响规律.结果表明,有机酸铵和咪唑类产物的生成浓度随着紫外光照时间的延长,甲苯、氨和臭氧的浓度的增加而逐渐增大.但是当臭氧浓度超过一定值后,光解生成的高浓度OH自由基能够使甲苯光氧化产物变成更多的挥发性化合物,从而不利于含氮有机物的生成.水分子的增加会使臭氧光解产生的OH自由基浓度减少,从而导致有机酸铵和咪唑类产物的生成浓度随着相对湿度的增大而降低.这为研究人为源SOA颗粒中含氮有机物棕色碳的形成提供了实验依据.

【Abstract】 Ozone was photolyzed to produce OH radicals, and photooxidation of toluene is initiated to generate secondary organicaerosol(SOA) particles in home-made smog chamber, nitrogen-containing organic compounds formed from toluene SOA reactionwith ammonia were studied under different experimental conditions. The absorbance at 205 and 270 nm of the reaction productsolution measured by UV-visible spectrophotometer was used to study the influence of environmental factors such as irradiationtime, the concentration of toluene, ammonia, ozone, and relative humidity on the formation of nitrogen-containing organiccompounds. The experimental results demonstrated that the concentration of organic acid ammonium and imidazole productsgradually increases with the increase of ultraviolet irradiation time and the concentrations of toluene, ammonia and ozone.However, when the concentration of ozone exceeds a certain value, the high concentration of OH radicals generated by photolysisof ozone can oxidize the photooxidation product of toluene into more volatile compounds, which is not conducive to theformation of nitrogen-containing organic compounds. Also, the increase of water molecules would reduce the concentration ofOH radicals, resulting in the decrease of the concentration of organic acid ammonium and imidazole products as the relativehumidity increases. These would provide the experimental basis for studying the formation of the nitrogen-containing organicbrown carbon of anthropogenic SOA particles.

【基金】 国家自然科学基金资助项目(41575118,41305109);福建省自然科学基金资助杰青项目(2015J06009)
  • 【文献出处】 中国环境科学 ,China Environmental Science , 编辑部邮箱 ,2019年02期
  • 【分类号】X513
  • 【被引频次】8
  • 【下载频次】123
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