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化学学报
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化学学报 ›› 2011, Vol. 69 ›› Issue (14): 1593-1600.    下一篇

研究论文

烟雾箱模拟丙烯-NOx的大气光化学反应

胡高硕1,2，徐永福*,1，贾龙1   

  1. (1中国科学院大气物理研究所大气边界层物理和大气化学国家重点实验室 北京 100029)
    (2中国科学院研究生院 北京 100049)
  • 投稿日期:2010-11-15 修回日期:2011-03-22 发布日期:2011-03-28
  • 通讯作者: 徐永福 E-mail:xyf@mail.iap.ac.cn
  • 基金资助:

    不同前体物配比和反应条件下O3的生成和变化规律研究

Smog Chamber Simulation of Atmospheric Photochemical Reactions of Propene and NOx

Hu Gaoshuo1,2 Xu Yongfu*,1 Jia Long1   

  1. (1 State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029)
    (2 Graduate University of Chinese Academy of Sciences, Beijing 100049)
  • Received:2010-11-15 Revised:2011-03-22 Published:2011-03-28

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利用自制烟雾箱对丙烯-NOx的光化学反应进行了一系列模拟实验, 研究了相对湿度及丙烯与NOx的初始浓度比值对丙烯-NOx光化学反应产物如O3和CO的影响. 实验得到了臭氧最大值、CO最大值及反应掉的C3H6均随相对湿度的增加而减少, 丙烯的臭氧生成活性最大值(IRmax)也随着相对湿度的增加而减小, 且两者间存在显著的线性关系. 丙烯与NOx的比值对反应生成臭氧最大值的影响出现两种情况: 当初始浓度比值在1.0～3.4之间时, 臭氧最大值随着该比值的增加而有大幅度提高|而当该比值分别在3.7～7.4之间时, 臭氧最大值随比值的增加而有小幅度的下降. 此外, 本研究还利用丙烯MCMv3.1机理对反应进行了数值模拟.

关键词: 烟雾箱, 光化学反应, 丙烯, 相对湿度, 增量反应活性

A series of experiments was conducted in a self-made photochemical smog chamber in order to simulate atmospheric photochemical reactions of propene and NOx. The effects of both relative humidity (RH) and the initial C3H6 to NOx concentration ([C3H6]0/[NOx]0) ratio on the ozone and CO production in the photochemical reactions were mainly investigated in this paper. Results show that the maximum concentrations of ozone and CO, as well as the concentration of reacted propene linearly decrease with increasing RH. The maximum value of incremental reactivity (IRmax) for propene also declines as RH increases. Their relationships with RH are statistically significant. The effects of [C3H6]0/[NOx]0 on the maximum ozone concentration show two different trends. When the ratio is within 1.0～3.4, the maximum ozone concentration greatly increases with increasing ratio, whereas for the ratio of 3.7 to 7.4, it gradually decreases as the ratio increases. The comparison between smog-chamber data and results from the propene sub-mechanism of MCMv3.1 is also made in this work.

Key words: smog chamber, photochemical reaction, propene, relative humidity, incremental reactivity