化学学报 ›› 2004, Vol. 62 ›› Issue (18): 1853-1857. 上一篇    

研究简报

Ir/SiO2上甲烷部分氧化制合成气反应的原位时间分辨红外和原位Raman光谱表征

翁维正, 罗春容, 李建梅, 刘颖, 林海强, 黄传敬, 万惠霖   

  1. 厦门大学化学系, 物理化学研究所, 固体表面物理化学国家重点实验室, 厦门, 361005
  • 投稿日期:2004-04-22 修回日期:2004-06-16 发布日期:2014-02-17
  • 通讯作者: 翁维正,E-mail:wzweng@xmu.edu.cn;万惠霖,E-mail:hlwan@xmu.edu.cn E-mail:wzweng@xmu.edu.cn;hlwan@xmu.edu.cn
  • 基金资助:
    国家重点基础研究发展规划(No.G1999022408)和国家自然科学基金(No.20021002)资助项目

In situ Time-resolved FTIR and Raman Characterizations of the Partial Oxidation of Methane to Synthesis Gas over Ir/SiO2 Catalyst

WENG Wei-Zheng, LUO Chun-Rong, LI Jian-Mei, LIU Ying, LIN Hai-Qiang, HUANG Chuan-Jing, WAN Hui-Lin   

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, Institute of Physical Chemistry, Xiamen University, Xiamen 361005
  • Received:2004-04-22 Revised:2004-06-16 Published:2014-02-17

采用原位时间分辨红外光谱和原位显微Raman光谱技术对Ir/SiO2上甲烷部分氧化(POM)制合成气反应的初级产物和反应条件下催化剂表面物种进行了跟踪考察,实验结果表明,在H2预还原的新鲜Ir/SiO2表面,CO是V(CH4):V(O2):V(Ar)=2:1:45混合气反应的初级产物,因而甲烷的直接氧化过程是CO生成的主要途径;而在稳态反应条件下,CO生成的途径可能主要来自CO2和H2O与催化剂表面积碳物种(CHx)和/或CH4的反应.催化剂上生成的积碳可能是导致稳态条件下Ir/SiO2上POM反应机理不同于H2预还原的新鲜催化剂的主要原因.

关键词: 甲烷部分氧化, 合成气, 铱催化剂, 反应机理

In situ time-resolved FTIR and in situ microprobe Raman spectroscopies were used to follow the primary products as well as the surface and gas phase species formed during the reaction of partial oxidation of methane (POM) to synthesis gas over Ir/SiO2 catalyst. The results suggested that direct oxidation of CH4 to CO is the dominant pathway of POM reaction over the freshly reduced Ir/SiO2 catalyst, while the dominant schemes of CO formation over the catalyst under the steady state reaction condition are probably via the reactions of CO2 and H2O with the deposited carbon species (CHx) and/or CH4. The mechanistic difference between the POM to synthesis gas over freshly reduced Ir/SiO2 catalyst and the catalyst under the steady state reaction may have resulted from the formation of significant amount of deposited carbon species in the latter system.

Key words: partial oxidation of methane(POM), synthesis gas, iridium catalyst, reaction mechanism