In situ time-resolved FTIR investigation on the reaction mechanism of partial oxidation of methane to syngas over supported Rh and Ru catalysts  

作　　者：WENG Weizheng CHEN Mingshu YAN Qiangu WU Tinghua CHAO Zisheng LIAO Yuanyan WAN Huilin 

机构地区：[1]Department of Chemistry,State Key Laboratory for Physical Chemistry of Solid Surfaces,and Institute of Physical Chemistry,Xiamen University,Xiamen 361005,China [2]Department of Chemistry,Zhejiang Normal University,Jinhua 321004,China

出　　处：《Chinese Science Bulletin》2000年第24期2236-2240,共5页

摘　　要：In situ time-resolved FTIR spectroscopy was used to study the reaction mechanism of partial oxidation of methane (POM) to synthesis gas and the reaction of CH4/O2/He (2/1/45, molar ratio) gas mixture with adsorbed CO species over Rh/SiO2, Ru/γ-Al2O3 and Ru/SiO2 catalysts at 500-600℃. It was found that CO is the primary product of POM reaction over reduced and working state Rh/SiO2 catalysts. Direct oxidation of CH4 is the main pathway of synthesis gas formation over Rh/SiO2 catalyst. CO2 is the primary product of POM over Ru/γ-Al2O3 and Ru/SiO2 catalysts. The dominant reaction pathway for synthesis gas formation over Ru/γ-Al2O3 catalyst is via the reforming reactions of CH4 with CO2 and H2O. For the POM reaction over Rh/SiO2 and Ru/γ-Al2O3 catalysts, consecutive oxidation of surface CO species is an important pathway of CO2 formation.In situ time-resolved FTIR spectroscopy was used to study the reaction mechanism of partial oxidation of methane (POM) to synthesis gas and the reaction of CH4/O2/He (2/1/45, molar ratio) gas mixture with adsorbed CO species over Rh/SiO2, Ruγ-Al2O3 and Ru/SiO2 catalysts at 500–600°C. It was found that CO is the primary product of POM reaction over reduced and working state Rh/SiO2 catalysts. Direct oxidation of CH4 is the main pathway of synthesis gas formation over Rh/SiO2 catalyst. CO2 is the primary product of POM over Ru/gg-Al2O3 and Ru/SiO2 catalysts. The dominant reaction pathway for synthesis gas formation over Ruγ-Al2O3 catalyst is via the reforming reactions of CH4 with CO2 and H2O. For the POM reaction over Rh/SiO2 and Ru/gg-Al2O2 catalysts, consecutive oxidation of surface CO species is an important pathway of CO2 formation.

关 键 词：partial oxidation of methane synthesis gas reaction mechanism in SITU TIME-RESOLVED FTIR ruthenium RHODIUM SUPPORTED metal catalyst. 

分 类 号：O657.33[理学—分析化学]