物理化学学报 >> 2010, Vol. 26 >> Issue (09): 2443-2448.doi: 10.3866/PKU.WHXB20100840

催化和表面结构 上一篇    下一篇

Fe、Mn掺杂干凝胶的制备、表征及催化臭氧氧化邻二氯苯性能

黄燕, 张兴旺, 雷乐成   

  1. 浙江大学化学工程与生物工程学系,工业生态与环境研究所,杭州310027
  • 收稿日期:2010-02-25 修回日期:2010-05-05 发布日期:2010-09-02
  • 通讯作者: 雷乐成 E-mail:lclei@zju.edu.cn;lablei@zju.edu.cn
  • 基金资助:

    国家自然科学基金(20836008, U0633003), 浙江省科技计划项目(2007C13061)和国家高技术研究发展计划(2007AA06Z339, 2008BAC32B06,2007AA06A409)资助

Preparation, Characterization and Catalytic Activity for ortho- Dichlorobenzene Ozonation of Fe-, Mn-Doped Xerogels

HUANG Yan, ZHANG Xing-Wang, LEI Le-Cheng   

  1. Institute of Industrial Ecology and Environment, Department of Chemical and Biological Engineering,Zhejiang University, Hangzhou 310027, P. R. China
  • Received:2010-02-25 Revised:2010-05-05 Published:2010-09-02
  • Contact: LEI Le-Cheng E-mail:lclei@zju.edu.cn;lablei@zju.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20836008, U0633003), Science and Technology Department of Zhejiang Province, China (2007C13061), and National High Technology Research and Development Programof China (2007AA06Z339, 2008BAC32B06, 2007AA06A409).

摘要:

采用溶胶-凝胶法制备Fe、Mn 掺杂的干凝胶材料(XFe 和XMn), 并对其催化臭氧氧化去除邻二氯苯(o- DCB)的性能进行了研究. 通过X 射线光电子能谱(XPS)、X 射线衍射(XRD)、透射电镜(TEM)、扫描电镜(SEM)、 压汞仪和氮气吸附等技术对Fe、Mn 掺杂的干凝胶材料进行表征. 结果表明: XFe 和XMn 中存在三价金属氧化 物等活性物种, 金属相无明显的衍射峰且金属颗粒的尺寸较小, 表明金属颗粒在干凝胶载体上获得较好的分散 性; 相比于单独臭氧氧化时44%的o-DCB 去除率, XFe 和XMn 的添加使得o-DCB 去除率分别达到58%和 72%, XFe 和XMn 显示了较好的催化活性; XFe 和XMn 的金属溶出状况不同, 在水溶液中浸泡5 h 后它们的金 属溶出率分别为2%和8%左右.

关键词: 溶胶-凝胶法, 干凝胶, 表征, 催化臭氧化, 邻二氯苯

Abstract:

Metal-doped xerogels were synthesized by the sol-gel method and their catalytic performance was evaluated for the catalytic ozonation of simulated micro-polluted water containing ortho-dichlorobenzene (o-DCB). The obtained samples were characterized by X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), X-ray diffraction (XRD), scanning electron microscopy (SEM), mercury porosimetry and nitrogen adsorption. Results show that Fe3+ oxides and Mn3+ oxides are present in the Fe-doped xerogel (XFe) and the Mn-doped xerogel (XMn), respectively. No obvious diffraction peaks corresponding to a metallic phase were present in the XRD patterns of the xerogels. Also, the metallic particles were found to be small; therefore, the metallic particles were well distributed over the xerogel supports. Catalytic ozonation experiments indicated that the removal rate of o-DCB was 44% with single ozonation, and this increased to 58% and 72% with catalytic ozonation using XFe and XMn, respectively, which suggests that metal-doped xerogels are promising catalysts for the ozonation process. We also investigated metal leaching from the metal-doped xerogel to the water solution to test the stability of the catalysts, and about 2%and 8%metal leaching for XFe and XMn was obtained within 5 h.

Key words: Sol-gel method, Xerogel, Characterization, Catalytic ozonation, ortho-Dichlorobenzene