Pd/SiO2催化剂上甲烷直接羰基化反应
Studies of Direct Carbonylation of Methane on Pd/SiO2 Catalysts
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摘要: 利用程序升温脉冲反应、恒温脉冲反应技术较系统地考察了Pt/SiO2催化剂上甲烷直接羰基化制乙醛的反应,研究发现通过采用总反应分解法操作后,能够克服甲烷直接羰基化反应的热力学限制,将总反应转化为两个可在较温和条件发生的反应,实现了CH4+CO→CH3CHO的反应。即首先进行甲烷的分解,然后引入CO使其与甲烷分解产生的表面物种直接反应生成乙醛。还探讨了甲烷吸附条件,CO与甲烷分解所产生的表面碳物种间的作用等反应的影响因素。Abstract: Direct carbonylation of methane on silica-supported palladium catalysts was tentatively investigated by using the temperature programmed pulse reaction (TPPR),constant temperature pulse reaction(CTPR).An important approach is to split the overall reaction into two reaction steps occurring under moderate conditions.Methane decomposition on palladium surface was firstly employed to form surface carbonaceous species.Then the CO syn-gas was introduced to interact with surface carbonaceous species to produce aldehyde.In such a two step route the thermodynamic limitations can be overcome and the direct carbonylation of methane may be effectively achieved.This reaction is an attractively novel route for utilization of methane.Optimization of this process would results in a new route for effective ultilization of methane.