高等学校化学学报

高等学校化学学报

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SO2与Fe2O3生成Fe(Ⅱ)(aq)和硫酸盐的复相反应机理

张秋菊; 王晓; 陈建民; 庄国顺   

  1. 复旦大学环境科学与工程系, 大气化学研究中心，上海 200433
  • 收稿日期:2005-09-27 修回日期:1900-01-01 出版日期:2006-07-10 发布日期:2006-07-10
  • 通讯作者: 陈建民

Formation of Fe(Ⅱ)(aq) and Sulfate via Heterogeneous Reaction of SO2 with Fe2O3

ZHANG Qiu-Ju, WANG Xiao; CHEN Jian-Min*; ZHUANG Guo-Shun   

  1. Center for the Atmospheric Chemistry Study, Department of Environmental
    Science & Engineering, Fudan University, Shanghai 200433, China
  • Received:2005-09-27 Revised:1900-01-01 Online:2006-07-10 Published:2006-07-10
  • Contact: CHEN Jian-Min

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摘要： 使用DRIFTS, XPS, HPLC和IC考察了常温、常压和氧气存在下SO2与Fe2O3的复相反应，结果表明, SO2在Fe2O3表面的反应活性与Fe2O3表面含水量密切相关, 表面含水量增加有助于Fe(Ⅱ)(aq)和硫酸盐的生成. 室温下(T=291 K, 相对湿度68%), 每毫克Fe2O3在30 min内可消耗53.6 μg SO2, 生成12.6 ng Fe(Ⅱ)(aq)和56.2 μg SO2-4. 反应产物 SO2-4的浓度比Fe(Ⅱ)(aq)的浓度高3个数量级, 表明在生成硫酸盐的复相反应中铁对SO2氧化具有非常高的催化活性. 提出了Fe(Ⅱ)(aq) 和硫酸盐的生成机理.

关键词: 复相反应, Fe2O3, SO2, Fe(Ⅱ)(aq), 硫酸盐

Abstract: The formation mechanism of Fe(Ⅱ)(aq) and sulfate via heterogeneous reaction of SO2 oxidation on the surface of Fe2O3was investigated at the normal temperature, pressure and in the presence of oxygen by DRIFTS, XPS, HPLC and IC. The results revealed that the reaction activity of SO2with Fe2O3 was closely related to the amount of absorbed water on the surface of Fe2O3, which was favorable for the formation of Fe(Ⅱ)(aq) and S(Ⅵ). Under ambient
condition[T=291 K, relative humidity(RH)=68%] within 30 min, for 1 mg Fe2O3 with the exhaustion of 53.6 μg SO2, it could produce 12.6 ng Fe(Ⅱ)(aq) and 56.2 μg SO2-4. The concentration of the product, [SO2-4], was three orders of magnitude higher than that of Fe(Ⅱ)(aq), indicating that large amount of SO2-4 production was formed via catalysis by the transitional metal Fe. The reaction mechanism of SO2 oxidation on Fe2O3 is proposed.

Key words: Heterogeneous reaction, Fe2O3, SO2, Fe(Ⅱ)(aq), Sulfate

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