用于烯烃臭氧化反应的快速流动管的设计与动力学研究  

Design and kinetic study of fast flow tube for alkene ozonation reaction

作　　者：王兴[1,2] 施晓雯 周莉 王臻 马嫣 郑军[1,2] WANG Xing;SHI Xiaowen;ZHOU Li;WANG Zhen;MA Yan;ZHENG Jun(School of Environmental Science and Engineering,Nanjing University of Information Science and Technology,Nanjing,210044,China;Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control,Nanjing,210044,China;Jiangsu Provincial Academy of Environmental Sciences,Nanjing,210000,China)

机构地区：[1]南京信息工程大学环境科学与工程学院,南京210044 [2]江苏省大气环境与监测污染控制高技术研究重点实验室,南京210044 [3]江苏省环境科学研究院,南京210000

出　　处：《环境化学》2024年第10期3470-3479,共10页Environmental Chemistry

基　　金：国家自然科学基金(41975172,42275116,41730106)资助.

摘　　要：Criegee中间体是烯烃气相臭氧化反应过程中最重要的中间产物,可以发生单分子分解生成羟基自由基,也可以与大气中的污染成分发生双分子反应,化学性质十分活跃.本文设计了大气压力快速流动反应管用于烯烃臭氧化反应及后续二次反应的研究.该流动管具有良好的温度和流量控制功能;可以同时进行两个独立反应(如烯烃+O_(3)和SCI+SO_(2));可以通过调节长度控制反应时间;易拆卸清洗,最大限度减少可能影响反应的痕量污染物的存在.通过3个流体力学无量纲参数雷诺数、斯托克斯数和理查德森数对流动管进行表征,并利用高分辨率化学电离飞行时间质谱对烯烃臭氧化反应及后续双分子反应进行动力学研究.经验证,新设计的流动管适用于烯烃臭氧化体系的研究,并且能够提供精确的、直接的动力学信息.Criegee intermediate is the most important intermediate product in the process of alkene ozonolysis,which can undergo unimolecular decomposition to form hydroxyl radicals or bimolecular reaction with atmospheric pollutants,and has very active chemical properties.In this paper,atmospheric pressure fast flow reaction tube was designed for the study of alkene ozonation reaction and subsequent secondary reactions.The flow tube has good temperature and flow control;two independent reactions(e.g.,alkene+O_(3)and SCI+SO_(2))can be carried out independently;allows control of the reaction time by adjusting the length;and is easily disassembled for cleaning,minimizing the presence of trace contaminants that may affect the reaction.The flow tube was characterized by three hydrodynamic dimensionless parameters,Reynolds number,Stokes number and Richardson number.Kinetic study of the alkene ozonation reaction and subsequent bimolecular reaction using High Resolution Time-of-Flight Chemical Ionization Mass Spectrometer.The newly designed flow tube was proven to be suitable for the study of alkene ozonation system and to provide accurate and direct kinetic information.

关 键 词：流动管 烯烃臭氧化反应 反应速率 产率. 

分 类 号：X-1[环境科学与工程] O6[理学—化学]