物理化学学报 >> 2013, Vol. 29 >> Issue (11): 2429-2436.doi: 10.3866/PKU.WHXB201310084

催化和表面科学 上一篇    下一篇

Fe-Al 柱撑膨润土的制备及其非均相Fenton降解橙黄II

万栋, 王光华, 李文兵, 陈坤, 舒广   

  1. 武汉科技大学化学工程与技术学院, 武汉 430081
  • 收稿日期:2013-07-11 修回日期:2013-10-07 发布日期:2013-10-30
  • 通讯作者: 王光华, 李文兵 E-mail:wghuah@21cn.com; liwenbing@126.com
  • 基金资助:

    高等学校博士学科点专项科研基金(20114219110002), 煤转化与新型炭材料湖北省重点实验室开放基金(武汉科技大学) (WKDM201107)和湖北省教育厅重点项目(D20131107)资助

Synthesis of Fe-Al Pillared Bentonite and Heterogeneous Fenton Degradation of Orange Ⅱ

WAN Dong, WANG Guang-Hua, LI Wen-Bing, CHEN Kun, SHU Guang   

  1. College of Chemical Engineering and Technology, Wuhan University of Science and Technology, Wuhan 430081, P. R. China
  • Received:2013-07-11 Revised:2013-10-07 Published:2013-10-30
  • Contact: WANG Guang-Hua, LI Wen-Bing E-mail:wghuah@21cn.com; liwenbing@126.com
  • Supported by:

    The project was supported by the Specialized Research Fund for the Doctoral Program of Higher Education of China (20114219110002), Hubei Key Laboratory of Coal Conversion and New Carbon Materials (Wuhan University of Science and Technology), China (WKDM201107), and Educational Commission of Hubei Province, China (D20131107).

摘要:

通过离子交换方法制备不同Fe 含量的Fe-Al 柱撑膨润土, 并且研究了其作为非均相Fenton 催化剂降解橙黄II 的性能. 通过X射线粉末衍射(XRD), 比表面积(SBET), 傅里叶变换红外(FTIR)光谱, 拉曼(Raman)光谱和扫描电子显微镜(SEM)研究其结构特征. 结果显示, 钠化膨润土的层间距为1.24 nm, 经过柱撑之后, Al 柱撑膨润土的层间距增大到1.77 nm, Fe-Al 柱撑膨润土为1.72 nm左右, 并且比表面积也有明显增大. XRD和Raman结果表明Fe/(Fe+Al)摩尔比达到20%时, 样品中出现α-Fe2O3, 膨润土未能形成柱撑. 在橙黄II 初始浓度为100 mg·L-1, 催化剂用量为1.0 g·L-1, 温度为40 ℃, pH为3.0, H2O2初始浓度为10 mmol·L-1的条件下, 考察了柱撑膨润土的Fenton 催化活性. 结果表明, Fe-Al 柱撑膨润土的催化性能随着Fe 含量的增多先增大后略有降低, 当Fe/(Fe+Al)摩尔比为10%时达到最大, 橙黄II 溶液在4 h内色度去除率和化学需氧量(CODCr)去除率分别达到100%和87.73%, 并且降解反应为非均相Fenton 反应. 研究了Fe-Al 柱撑膨润土的重复使用性. 催化剂循环使用4次, 仍然具有良好的活性.

关键词: Fe-Al柱撑膨润土, 非均相催化剂, 橙黄II, Fenton反应, 降解

Abstract:

A series of Fe-Al pillared bentonites with different Fe contents were synthesized through a simple ion exchange method. The samples were used as catalysts for the heterogeneous Fenton degradation of Orange II. The microstructure of the catalysts was characterized by X-ray diffraction (XRD), specific surface area measurements (SBET), Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, and scanning electron microscopy (SEM). The obtained results showed that the pillaring process increased the basal spacing (d(001)) from 1.24 nm for the Na-bentonite (Bent) to 1.77 nm for the Al-Bent and ~1.72 nm for the Fe-Al pillared bentonites. The SBET values of the samples were increased after pillaring. It was obvious from the XRD and Raman results that intercalation was not achieved and that hematite was formed in the 20Fe-Al-Bent sample. The influence of Fe content on the degradation of Orange II was investigated. The catalytic activity of pillared bentonites increased with Fe content and hardly increased when the molar ratio of Fe/(Al + Fe) in the pillaring solution exceeded 10% . The decolorization efficiency and chemical oxygen demand (CODCr) removal of Orange II reached 100% and 87.73%, respectively, after 4 h oxidation reaction using the 10Fe-Al-Bent sample. It is also proved that the whole decomposition of Orange II by 10Fe-Al-Bent was dominated by heterogeneous Fenton reaction. The catalysts were chemically stable and reusable, with low release of iron.

Key words: Fe-Al pillared bentonite, Heterogeneous catalysis, Orange II, Fenton reaction, Degradation

MSC2000: 

  • O643