甲烷部分氧化反应机理的键级守恒研究

A Study on the Bond-Order-Conservation Model of the Mechanism of Methane Partial Oxidation to Syngas on Ni(111)

用键级守恒－Ｍｏｒｓｅ势方法（ＢＯＣ－ＭＰ）研究了甲烷部分氧化制合成气的反应机理．以Ｎｉ（１１１）晶面为模型催化剂，应用ＢＯＣ－ＭＰ方法计算了甲烷在有氧与无氧参与下的解离反应及ＣＯ和ＣＯ２生成反应中各基无反应的活化能垒和反应热焓．计算结果表明：无表面氧参与下的ＣＨ４直接解离途径更可能发生；由ＣＨ（ｓ）生成ＣＯ比由Ｃ（ｓ）更易进行．

The approach of the bond-order-conservation Morse-potential is introduced to study themechanism of methane partial oxidation to syngas on Ni (111). Calculation results indicate: (1)thedirect eissociation of CH4 without the involvement of sruface oxygen is more likely to occur; (2)the formation of CO from CH(s) occurs more readily than from C(s).