本文以探明Pt/Al2O3、Ir/SiO2和Ru/SiO2等催化剂上甲烷部分氧化（POM）制合成气反应机理为目的，首先采用原位显微Raman光谱技术，对POM反应起燃前后催化剂床层前部贵金属物种的化学态以及由甲烷解离所生成的碳物种进行了详细的表征。在此基础上采用脉冲实验技术在POM反应条件下对Ar稀释的CH4/O2，CH4/H2O，CH4/CO2和CH4/H2O/CO2等混合气在相关催化剂床层前部（氧化区）和后部（重整区）的反应情况进行了考察，并将实验结果与Raman光谱的表征结果进行了关联，最后采用CD4，D2O和18O2同位素示踪技术，进一步考察了Ir/SiO2催化剂氧化区上氢气和一氧化碳...In this study, we report a mechanistic study on the partial oxidation of methane (POM) to synthesis gas over Ru/SiO2, Pt/Al2O3 and Ir/SiO2 catalysts by using in situ microprobe Raman spectroscopy to probe the catalyst located at the entrance of the catalyst bed during the catalytic ignition process (rt ~ 700 C) of the POM reaction for chemical state of the metals as well as the carbon species that...学位：理学博士院系专业：化学化工学院化学系_物理化学(含化学物理)学号：2052008015019
