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NO2对SO2/H2O/空气体系气溶胶成核过程的影响
引用本文:温作赢,顾学军,荣华,马乔,唐小锋,胡长进,张为俊.NO2对SO2/H2O/空气体系气溶胶成核过程的影响[J].环境科学研究,2016,29(5):609-616.
作者姓名:温作赢  顾学军  荣华  马乔  唐小锋  胡长进  张为俊
作者单位:1.中国科学院安徽光学精密机械研究所, 中国科学院大气成分与光学重点实验室, 安徽 合肥 230031 ;中国科学技术大学研究生院, 安徽 合肥 230026 ;中国科学院安徽光学精密机械研究所大气物理化学研究室, 安徽 合肥 230031
基金项目:国家自然科学基金项目(41175121,7);国家自然科学基金委员会-中国科学院大科学装置科学研究联合基金项目(U1232209)
摘    要:为研究NO2对SO2/H2O/空气体系气溶胶成核过程的影响,采用纳米扫描迁移率粒子粒径谱仪(Nano-SMPS),对NO2/SO2/H2O/空气混合气体在X-射线作用下生成粒子的粒径和浓度进行测量. 结果表明,粒子的粒径在2.0~63.8 nm之间,最高数浓度可达到1.4×107 cm-3. 成核粒子谱的分布呈双峰模式,其中一个谱峰中心位置在4.0 nm附近,另一个在7.0~14.6 nm之间,分别对应于均相成核和离子诱导成核两种过程. 在均相成核方面,NO2和SO2均能参与气溶胶成核,而对气溶胶的生长没有明显影响,粒子的粒径主要集中在4.0 nm附近. 在离子诱导成核方面,当混合气体中φ(SO2)低于2.12×10-6时,加入NO2可促进粒子生成;而当超过该值时,NO2的加入反而会降低气溶胶成核粒子的总数浓度. 当φ(SO2)为3.61×10-6时,在φ(NO2)分别为0.13×10-6、0.18×10-6和0.84×10-6的条件下,气溶胶成核粒子的总数浓度比不含NO2下分别减少了25.9%、33.1%和49.0%. 研究显示,NO2和SO2对·OH的反应竞争作用是影响NO2/SO2/H2O/空气体系气溶胶成核的重要机制. 

关 键 词:气溶胶    新粒子形成    均相成核    离子诱导成核
收稿时间:2015/11/19 0:00:00
修稿时间:2016/2/5 0:00:00

Effects of NO2 on New Particle Formation in SO2/H2O/Air Mixtures
WEN Zuoying,GU Xuejun,RONG Hu,MA Qiao,TANG Xiaofeng,HU Changjin and ZHANG Weijun.Effects of NO2 on New Particle Formation in SO2/H2O/Air Mixtures[J].Research of Environmental Sciences,2016,29(5):609-616.
Authors:WEN Zuoying  GU Xuejun  RONG Hu  MA Qiao  TANG Xiaofeng  HU Changjin and ZHANG Weijun
Affiliation:Key Laboratory of Atmospheric Composition and Optical Radiation, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;Graduate School, University of Science and Technology of China, Hefei 230026, China ;Laboratory of Atmospheric Physics and Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China,Key Laboratory of Atmospheric Composition and Optical Radiation, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;Laboratory of Atmospheric Physics and Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China,Key Laboratory of Atmospheric Composition and Optical Radiation, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;Laboratory of Atmospheric Physics and Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China, Hefei 230026, China,Key Laboratory of Atmospheric Composition and Optical Radiation, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;Graduate School, University of Science and Technology of China, Hefei 230026, China ;Laboratory of Atmospheric Physics and Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China,Key Laboratory of Atmospheric Composition and Optical Radiation, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;Laboratory of Atmospheric Physics and Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China,Key Laboratory of Atmospheric Composition and Optical Radiation, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;Laboratory of Atmospheric Physics and Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China and Key Laboratory of Atmospheric Composition and Optical Radiation, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;Laboratory of Atmospheric Physics and Chemistry, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031, China ;School of Environmental Science and Optoelectronic Technology, University of Science and Technology of China, Hefei 230026, China
Abstract:New particle formation induced by a soft X-ray radiolysis in NO2/SO2/H2O/air gas mixtures was investigated by using a nanometer scanning mobility particle sizer (Nano-SMPS). The role of NO2 in the formation was especially discussed. The electrical mobility size distribution of the newly formed particles was measured; it exhibited a bimodal shape. The diameter of particles was measured from 2.02 to 63.80 nm. The maximum concentration reached 1.4×107 cm-3. The intensity of the first peak with center at ~4.0 nm could be enhanced with both NO2 and SO2 gases,and its formation mechanism was assigned as homogenous nucleation. The second peak with a bigger center size (7.0-14.6 nm) was mainly from the ion-induced nucleation process,and the addition of NO2 and SO2 gases enhanced both its intensity and center size. In addition,the experimental results also showed that the total particle number was influenced by the concentrations of SO2 and NO2. The total particle number increased with NO2 when the concentration of SO2 was below 2.12×10-6,whereas NO2 exerted a negative effect on the particle number when the concentration of SO2 was high. When the concentration of SO2 was fixed at 3.61×10-6,the concentrations of new particle decreased 25.9%,33.1% and 49.0% after NO2 with concentrations of 0.13×10-6,0.18×10-6 and 0.84×10-6 was added in the reaction chamber. These phenomena can be explained by the competition of NO2 and SO2 in the production channel of ·OH radicals. 
Keywords:aerosol  new particle formation  homogeneous nucleation  ion-induced nucleation
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