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化学学报
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化学学报 ›› 2011, Vol. 69 ›› Issue (04): 452-458. 上一篇    下一篇

研究论文

酸性Fe-SiO2催化剂制备及其photo-Fenton催化性能

刘良军1，张国亮*,1，黄涛1，王玲1，孟琴2   

  1. (a浙江工业大学生物与环境工程学院 杭州 310014)
    (b浙江大学材料与化学工程学院 杭州 310027)
  • 投稿日期:2010-09-16 修回日期:2010-10-19 发布日期:2010-10-25
  • 通讯作者: 张国亮 E-mail:guoliangz@zjut.edu.cn
  • 基金资助:

    高效抗污染中空纤维膜光催化反应器的构建及性能研究

Preparation of Acidic Fe-SiO2 Catalyst and Its Catalytic Reactivity in Photo-Fenton Reaction

Liu Liangjun1 Zhang Guoliang*,1 Huang Tao1 Wang Ling1 Meng Qin2   

  1. (1 College of Biological and Environmental Engineering, Zhejiang University of Technology, Hangzhou 310014)
     (2 College of Material & Chemical Engineering, Zhejiang University, Hangzhou 310027)
  • Received:2010-09-16 Revised:2010-10-19 Published:2010-10-25
  • Contact: Guo-Liang ZHANG E-mail:guoliangz@zjut.edu.cn

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以正硅酸乙酯为硅源, 十二烷基三甲基溴化铵为模板剂, 在不同铁源和酸激活条件下合成Fe-SiO2复合氧化物. 采用扫描电镜(SEM)、X射线衍射仪(XRD)和傅里叶转换红外光谱仪(FT-IR)对催化剂表面形貌、活性组分分散性和表面基团进行分析. 研究了不同酸性Fe-SiO2催化剂(FS)在可见光照射下photo-Fenton降解直接大红4BS的活性. 结果表明: 以硫酸亚铁为铁源制备的催化剂所含骨架Fe的分散性能优于硝酸铁为铁源获得的催化剂, 但后者表面活性位数和酸量却高于前者. 在初始pH＝6.0时, FS/1和FS/6两种Fe-SiO2催化剂均能在120 min使100 mg/L直接大红4BS几乎完全脱色, 且矿化程度分别高达79%与99%. 动力学拟合证明, 该酸催化过程可以看作一级与二级反应联合作用的结果. 对上述两种催化剂的溶剂浸取稳定性和铁离子泄漏测试显示, 催化剂可能实现较长时间稳定运行.

关键词: Fe-SiO2, 可见光, photo-Fenton, 直接大红4BS, 酸催化

The acid-activated Fe-SiO2 composites were synthesized using tetraethyl orthosilicate (TEOS) as the silica source, cetyltrimethylammonium bromide (CTAB) as the template and salts of Fe as the iron sources. After finishing the preparation, these samples were characterized using scanning electron microscopy for the morphology of the catalysts, X-ray diffractometer for the dispersibility of Fe, and Fourier transform infrared spectrometer for the surface groups. To investigate catalytic activities, various photo-Fenton reactions have been conducted to decontaminate the direct red 4BS simulated wastewater under visible light irradiation. The results indicated that the sample possessing its iron source from FeSO4 had better dispersibility, but lower activities and stability than that from Fe(NO3)3. At initial pH of 6.0, both FS/1 and FS/6 not only led to 100% decolorization of a solution containing 100 mg/L direct red, but also about 79% and 99% total organic carbon were removed in respective system after reaction for 120 min. The kinetics study showed that a model in combination of first order and second order reactions was suitable for this acid-catalyzed process. Analyses of solvent-leaching stability and iron leaching demonstrated these catalysts may have long-term stability.

Key words: Fe-SiO2, visible light, photo-Fenton, direct red 4BS, acid-catalysis