化学学报 ›› 2007, Vol. 65 ›› Issue (18): 2007-2013. 上一篇    下一篇

研究论文

预处理条件对Au/ZnO催化剂CO氧化性能的影响

邵建军1,2, 张平1, 宋巍2, 黄秀敏2, 徐奕德2, 申文杰*,2   

  1. (1装甲兵工程学院装备再制造国防科技重点实验室 北京 100072)
    (2中国科学院大连化学物理研究所催化基础国家重点实验室 大连 116023)
  • 投稿日期:2006-11-10 修回日期:2007-03-22 发布日期:2007-09-28
  • 通讯作者: 申文杰

Effects of Pretreatment Conditions on the Catalytic Performance of Au/ZnO Catalysts for CO Oxidation

SHAO Jian-Jun1,2; ZHANG Ping1; SONG Wei2; HUANG Xiu-Min2; XU Yi-De2; SHEN Wen-Jie*,2   

  1. (1 National Key Laboratory for Remanufacturing, Academy of Armored Force Engineering, Beijing 100072)
    (2 State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023)
  • Received:2006-11-10 Revised:2007-03-22 Published:2007-09-28
  • Contact: SHEN Wen-Jie

采用沉积沉淀法制备了用于CO氧化的Au/ZnO催化剂, 并用程序升温还原(TPR), X射线衍射(XRD)和透射电镜(TEM)技术对催化剂进行了表征. 结果表明: 采用沉积沉淀法可制备出高度分散的Au/ZnO催化剂; 提高焙烧温度导致金颗粒聚集长大, 样品经533, 673, 773 K焙烧后金物种的颗粒尺寸分别为2.7, 3.5, 3.7 nm. 催化剂的TPR表征结果中发现部分还原态的金物种在室温就可被氧化, 催化剂预先用流动空气处理可提高其氧化还原性, 样品经多次氧化还原循环后, 其氧化循环性能没有明显下降. CO的氧化反应结果表明, 焙烧温度强烈影响催化剂对CO的氧化活性, 533 K焙烧后的催化剂活性最高. 即使在反应气中含水3.1%(体积比)的湿气条件下, 反应300 h后, CO的转化率仍然保持在95%.

关键词: Au/ZnO, CO氧化, 焙烧温度, 预处理

Au/ZnO catalysts were prepared by the deposition-precipitation (DP) method. Effects of calcination temperature and pretreatment conditions on the structure and the catalytic performance of Au/ZnO catalysts were investigated for CO oxidation. For the samples calcined in 533~773 K, no diffraction peak of gold species could be detected by XRD measurement. Transmission electron microscopy (TEM) observation revealed that the particle sizes of gold were 2.7, 3.5 and 3.7 nm respectively, for the catalysts calcined at 533, 673 and 773 K. Temperature-programmed reduction (H2-TPR) measurements further indicated that the pre-reduced gold species could be reoxidized at room temperature and the redox property of the catalyst could be enhanced through pretreatment with flowing air. However, its high redox properties still remained after several redox cycles. The result of CO oxidation on the catalytic behavior of the Au/ZnO catalysts was strongly influenced by the particle size and the surface area of the catalyst. The highly dispersed Au/ZnO catalyst with larger surface area and the least particle size can be prepared by the deposition-precipitation calcined at 533 K, resulting in the most promising activity and stability for CO oxidation. 95% CO conversion could be achieved after 300 h time-on-stream even though the feed gas contained 3.1 vol.% of water vapor.

Key words: Au/ZnO, CO oxidation, calcination temperature, pretreatment