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采用原位时间分辨红外光谱(in situ TR-FTIR)技术, 在500~600℃、时间分辨率优于0.3 s的条件下, 对CH4/O2/He (2/1/45, 摩尔比)混合气在不同预处理后的Rh/SiO2, Ru/?-Al2O3和Ru/SiO2上的反应及其与催化剂上吸附CO物种的作用情况进行了跟踪、考察. 实验结果表明, 在还原态和工作态Rh/SiO2上, CO是POM反应的初级产物. 由甲烷直接脱氢生成表面吸附氢和CHx (x = 1~3)物种, 后者再进一步氧化生成CO是Rh/SiO2上POM反应的主要途径. 在Ru/?-Al2O3, Ru/SiO2和氧化态的Rh/SiO2上, CO2是CH4/O2/He混合气反应的初级产物. CH4与CO2和H2O的重整反应是Ru/?-Al2O3和Ru/SiO2上CO和H2生成的主要途径. 在Rh/SiO2和Ru/?-Al2O3上, 催化剂表面吸附CO物种的进一步氧化是POM反应中CO2生成的重要途径之一.
Using in situ TR-FTIR technique, CH4 / O2 / He (2/1/45, molar ratio) was mixed under the conditions of 500-600 ℃ and time resolution better than 0.3 s The reaction of gas on Rh / SiO2, Ru /? - Al2O3 and Ru / SiO2 after different pretreatment and its effect on the adsorption of CO species on the catalyst were investigated and investigated. The experimental results show that in the reduced state and working state Rh / SiO2, CO is the primary product of POM reaction.Direct hydrogenation of methane to form surface-adsorbed hydrogen and CHx (x = 1 ~ 3) species, which is further oxidized to CO, is the main pathway of POM reaction on Rh / SiO2 In Ru /? - Al2O3, Ru / SiO2 and oxidation state Rh / SiO2, CO2 is the primary product of the reaction of CH4 / O2 / He.The reforming reaction between CH4 and CO2 and H2O is Ru /? - Al2O3 and The main pathway for the formation of CO and H2 on Ru / SiO2. On Rh / SiO2 and Ru /? - Al2O3, further oxidation of CO species adsorbed on the catalyst surface is one of the important ways of CO2 generation in POM reaction.