化学学报 ›› 2007, Vol. 65 ›› Issue (24): 2965-2970. 上一篇    下一篇

研究论文

Pt/CNTs催化剂的制备及其催化臭氧化活性研究

刘正乾, 马军*   

  1. (哈尔滨工业大学市政环境工程学院 哈尔滨 150090)
  • 投稿日期:2006-10-16 修回日期:2007-08-06 发布日期:2007-12-28
  • 通讯作者: 马军

Preparation and Catalytic Ozonation Activity of Pt/CNTs Catalyst

LIU Zheng-Qian; MA Jun*   

  1. (School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150090)
  • Received:2006-10-16 Revised:2007-08-06 Published:2007-12-28
  • Contact: MA Jun

以碳纳米管(CNTs)为催化剂载体, 以H2PtCl6•6H2O为贵金属活性组分前驱物, 采用等体积浸渍法制备了Pt/CNTs催化剂. 以草酸为目标污染物, 考察了所制备催化剂的催化活性, 并采用SEM, XRD和XPS等分析方法对催化剂进行表征. 对活性组分Pt的负载量、氢还原温度和热处理方式进行了研究, 确定了适宜的制备条件为Pt负载量1.0%、氢还原温度350 ℃. 研究表明, 在本实验条件下, 单独臭氧氧化、碳纳米管载体催化臭氧化和Pt/CNTs催化臭氧化分别能去除溶液中3.0%, 72.9%和97.9%的草酸. Pt的负载明显地提高碳纳米管催化臭氧化的效果. XRD分析显示催化剂的活性组分Pt以单质Pt0的形式存在; 与氢还原过程相比, 在空气气氛中焙烧制备的Pt/CNTs催化剂表面Pt的结晶度过高, 而且XPS结果表明此催化剂表面的Pt有化学吸附氧存在, 导致催化活性降低.

关键词: 碳纳米管, 催化臭氧化, 草酸

Pt/carbon nanotube (CNTs) catalyst was prepared by incipient wetness impregnation using H2PtCl6•6H2O as precursor. The catalyst was characterized by SEM, XRD, XPS and its degradation ability for oxalic acid was evaluated. The preparation conditions, including the reduction temperature, Pt loading and pyrolysis were studied. The optimal preparation parameters are obtained to be 350 ℃ with Pt loading of 1.0%. It was found that the removal efficiency of oxalic acid in ozonation alone, CNTs support and Pt/CNTs catalyzed ozonation was 3.0%, 72.9% and 97.9% respectively under the present experimental conditions. The loading of Pt can enhance catalytic activity of CNTs obviously. The XRD results indicate that the active phases of catalysts are in the form of Pt0. Compared with that prepared by reduction process in hydrogen, Pt/CNTs catalyst prepared by pyrolysis in air showed lower activity due to the over crystallization of Pt and the existence of chemisorbed oxygen with Pt on CNTs surface.

Key words: carbon nanotube, catalytic ozonation, oxalic acid