物理化学学报 >> 2001, Vol. 17 >> Issue (08): 733-738.doi: 10.3866/PKU.WHXB20010813

研究论文 上一篇    下一篇

甲烷在Ni/TiO2催化剂表面的活化

严前古;罗春容;翁维正;杨乐夫;万惠霖;吴廷华   

  1. 厦门大学化学系 固体表面物理化学国家重点实验室 物理化学研究所,厦门 361005;浙江师范大学物理化学研究所,金华 321004
  • 收稿日期:2000-10-16 修回日期:2001-04-23 发布日期:2001-08-15
  • 通讯作者: 万惠霖

Activation of Methane over Ni/TiO2 Catalyst

Yan Qian-Gu;Luo Chun-Rong;Weng Wei-Zheng;Yang Le-Fu;Wan Hui-Lin;Wu Ting-Hua   

  1. State Key Laboratory for Physical Chemistry of Solid Surfaces,Department of Chemistry and Institute of Physical Chemistry,Xiamen University,Xiamen 361005;Institute of Physical Chemistry,Zhejiang Normal University,Jinhua 321004
  • Received:2000-10-16 Revised:2001-04-23 Published:2001-08-15
  • Contact: Wan Hui-Lin

摘要: 考察了Ni/TiO2催化剂甲烷部分氧化和二氧化碳重整制合成气的反应活性,实验表明,以TiO2为载体的镍系催化剂对于甲烷部分氧化制合成气反应具有较好的活性,尤其对H2的选择性较高,对二氧化碳重整制合成气反应具有较好的低温反应活性.采用脉冲-质谱在线分析等技术,在无气相氧条件下向Ni/TiO2催化剂脉冲CH4,发现甲烷在催化剂表面的活化(转化)及其氧化产物的选择性与金属催化剂表面氧的浓度密切相关.CH4与Ni/TiO2催化剂作用过程中存在明显的氢溢流和氧溢流现象,可能是这种溢流效应使得Ni/TiO2催化剂具有良好的反应活性和抗积碳性能.

关键词: 甲烷, Ni/TiO2催化剂, 活化, 表面氧浓度, 溢流现象

Abstract: The reactions of methane partial oxidation (POM) and methane reforming with CO2 to produce synthetic gas over Ni/TiO2 catalyst were studied.The catalyst shows good catalytic performance with high H2 selectivity for the POM reaction and good low temperature activity for the reaction of methane reforming with CO2.The activation of methane over Ni/TiO2 catalysts was investigated using MS-pulse technique in the absence of gaseous oxygen.It was found that methane activation and its oxidation products were determined by the concentration of surface oxygen species of the catalyst.Both oxygen and hydrogen spillover phenomena were observed during the interaction of methane with Ni/TiO2.The spillover oxygen and hydrogen species over the catalyst may be responsible for the good activity and carbon resistance ability of the Ni/TiO2 catalyst.

Key words: Methane, Ni/TiO2 catalyst, Activation, Surface oxygen concentration, Spillover