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In situ time-resolved FTIR investigation on the reaction mechanism of partial oxidation of methane to syngas over supported Rh and Ru catalysts
Authors:Weizheng Weng  Mingshu Chen  Qiangu Yan  Tinghua Wu  Zisheng Chao  Yuanyan Liao  Huilin Wan
Institution:(1) Department of Chemistry, State Key Laboratory for Physical Chemistry of Solid Surfaces, and Institute of Physical Chemistry, Xiamen University, 361005 Xiamen, China;(2) Department of Chemistry, Zhejiang Normal University, 321004 Jinhua, China
Abstract: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.
Keywords:partial oxidation of methane  synthesis gas  reaction mechanism            in situ time-resolved FTIR  ruthenium  rhodium  supported metal catalyst
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