化学学报 ›› 2005, Vol. 63 ›› Issue (18): 1651-1655. 上一篇    下一篇

研究论文

整体式Co3O4/YSZ- -Al2O3+CYZ催化剂上的甲烷催化燃烧

杜小春,刘志敏,罗勇悦,陈耀强,龚茂初*   

  1. (四川大学化学学院 成都 610064)
  • 收稿日期:2004-09-20 修回日期:2005-05-30 出版日期:2005-09-28 发布日期:2010-12-10
  • 通讯作者: 龚茂初

Methane Combustion over Co3O4/YSZ- -Al2O3+CYZ Monolithic Catalysts

DU Xiao-Chun, LIU Zhi-Min, LUO Yong-Yue, CHEN Yao-Qiang, GONG Mao-Chu*   

  1. (College of Chemistry, Sichuan University, Chengdu 610064)
  • Received:2004-09-20 Revised:2005-05-30 Online:2005-09-28 Published:2010-12-10
  • Contact: GONG Mao-Chu

用质量比为3∶2的YSZ-γ-Al2O3和CeO2-Y2O3-ZrO2的混合物(以YSZA+CYZ表示)作载体, 制备了不同Co3O4含量的整体式甲烷燃烧催化剂, 同时制备了分别以YSZA和CYZ为载体的催化剂作为对比, 研究了它们老化前后的反应性能, 并用BET, XPS, XRD, TPR等研究了催化剂的比表面、表面状态、晶相结构和还原性能. 结果表明, YSZ- -Al2O3和CeO2-Y2O3-ZrO2混合载体能有效地抑制CoAl2O4的生成, 并能充分发挥各自的优点, 因此负载一定量的钴后表现出很高的甲烷催化燃烧活性和抗老化性, 尤其是含8 wt% Co3O4的样品性能最佳, 有望成为实用的甲烷燃烧催化剂之一.

关键词: 甲烷催化燃烧, 整体式催化剂, Co3O4, YSZ-γ-Al2O3, CeO2-Y2O3-ZrO2

A series of cobalt-based monolithic catalysts supported on mixture of YSZ-γ-Al2O3 and CeO2-Y2O3-ZrO2 were prepared by impregnation method, and characterized by XRD, XPS, BET and H2-TPR. Contrasting with the 8 wt% Co3O4-based monolithic catalyst supported on YSZ-γ-Al2O3 or CeO2-Y2O3-ZrO2, the catalytic activities for methane combustion were assessed in a micro-reactor. All the mixture supported monolithic catalysts had higher activity for methane combustion than the contrast catalysts. After calcination at 1000 ℃ for 5 h, the monolithic catalysts remained highly active and very stable, especially the catalyst containing 8 wt% of Co3O4 had the highest activity and methane was completely converted to CO2 at ca. 514 ℃. The results showed that the mixture had the advantage of CeO2-Y2O3-ZrO2 and YSZ-γ-Al2O3 (γ-Al2O3 modified by Y2O3 and ZrO2) and can resist forming the crystal of CoAl2O4 effectively.

Key words: methane catalytic combustion, monolithic catalyst, Co3O4, YSZ-γ-Al2O3, CeO2-Y2O3-ZrO2