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Oscillations during partial oxidation of methane to synthesis gas over Ru/Al_2O_3 catalyst

查看全文 作  者:Meiliu Wang Weizheng Weng Haozhuan Zheng Xiaodong Yi Chuanjing Huang Huilin [1,2]Wan 高影响力作者 机构地区:[1]State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters and Department of Chemistry College of Chemistry and Chemical Engineering, Xiamen UniversiO;[2] Xiamen 361005, Fujian, China;高影响力机构 出  处:《Journal of Natural Gas Chemistry》索引2009年第18卷第3期,共6页高影响力期刊 基  金:supported by the Ministry of Science and Technology of China (2005CB221401);the National Natural Science Foundation of China(20873111);the Key Science & Technology Specific Projects of Fujian Province (2009HZ10102) 摘  要:Oscillations in temperatures of catalyst bed as well as concentrations of gas phase species at the exit of reactor were observed during the partial oxidation of methane to synthesis gas over Ru/Al2O3 in the temperature range of 600 to 850 ℃.XRD,H2-TPR and in situ Raman techniques was used to characterize the catalyst.Two types of ruthenium species,i.e.the ruthenium species weakly interacted with Al2O3 and that strongly interacted with the support,were identified by H2-TPR experiment.These species are responsible for two types of oscillation profiles observed during the reaction.The oscillations were the result of these ruthenium species switching cyclically between the oxidized state and the reduced state under the reaction condition.These cyclic transformations,in turn,were the result of temperature variations caused by the varying levels of the strongly exothermic CH4 combustion and the highly endothermic CH4 reforming(with H2O and CO2) reactions(or the less exothermic direct partial oxidation of methane to CO and H2),which were favored by the oxidized and the metallic sites,respectively.The major pathway of synthesis gas formation over the catalyst was via the combustion-reforming mechanism. 关 键 词:Ru/Al2O3催化剂 甲烷部分氧化 合成气 部分氧化反应 振动 拉曼光谱技术 温度范围 甲烷燃烧
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