高等学校化学学报

高等学校化学学报 ›› 2002, Vol. 23 ›› Issue (9): 1738.

• 研究论文 • 上一篇    下一篇

大气颗粒物对CS2催化氧化反应动力学研究

王琳, 宋国新, 张峰, 陈建民   

  1. 复旦大学环境科学与工程系, 上海 200433
  • 收稿日期:2001-09-29 出版日期:2002-09-24 发布日期:2002-09-24
  • 通讯作者: 陈建民(1964年出生),男,博士,教授,博士生导师,从事环境化学研究.E-mail:jmchen@fudan.ac.cn E-mail:jmchen@fudan.ac.cn
  • 基金资助:

    国家教育部归国留学人员基金资助

Kinetic Studies on Catalytic Oxidation of CS2 over Atmospheric Particles

WANG Lin, SONG Guo-Xin, ZHANG Feng, CHEN Jian-Min   

  1. Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, China
  • Received:2001-09-29 Online:2002-09-24 Published:2002-09-24

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摘要： 使用FTIR,XPS,BET,TG-DTG-DTA及原位XRD等方法研究了二硫化碳(CS2)在大气颗粒物表面多相催化反应历程及硫物种的转化过程.结果表明,在常温下,CS2能与大气颗粒物反应,主要产物有羰基硫(COS)和正交α-S8,少量硫物种被深度氧化,在大气颗粒物表面形成正六价态硫.反应体系中当氧气过量时,CS2在大气颗粒物表面多相催化反应遵循假二级反应动力学规律.在296K下,该反应的表观速率常数为6.98×10-22cm3·mol-1·s-1,表观活化能为34.6kJ/mol,揭示了大气颗粒物具有消除CS2的重要作用以及深度氧化使颗粒物表面形成SO42-的现象.

关键词: 大气颗粒物, 二硫化碳, 羰基硫, 多相催化

Abstract: Heterogeneous interaction between carbon disulphide and atmospheric particles was investigated by means of FTIR, XPS, TG-DTG-DTAand in situ XRDanalysis. COSand orthorhombic α-S8 were the main products at ambient temperature. And SO42- was identified on the surface of atmospheric due to the further oxidation of sulfur species. Based on the static-state FTIRstudy and the analysis of sulphur species on the surface of atmospheric particles by XPS, a model of mechanism on heterogeneous interaction between the surface of atmospheric particles and CS2 was given. The reaction is confirmed to be a pseudo-secondary one when O2 is overloaded. The apparent rate constant is 6.98×10-22 cm3·mol-1·s-1 at 296 K, and apparent activation energy is 34.6 kJ/mol. In an industrial zone with CS2 exhaust emission standard of 10 mg/m3(GB 3095), the CS2 wastage of the heterogeneous interaction is 41% of that of the reaction between CS2 and OH·, which confirms the significance of the heterogeneous interaction in developing countries.

Key words: Atmospheric particles, Carbon disulphide, Carbonyl sulphide, Heterogeneous interaction

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