摘要
用蒙特卡罗方法对水气转移反应两种典型机理的初始反应动力学进行了研究．结果表明，Ｔｅｍｋｉｎ等人的氧化－还原机理中，无论反应物ＣＯ和Ｈ２Ｏ的相对浓度怎样变化，ＣＯ２和Ｈ２的初始生成速率总是相差很大．而在Ｏｋｉ等人的Ｌａｎｇｍｕｉｒ－Ｈｉｎｓｈｅｌｗｏｏｄ机理中，ＣＯ２和Ｈ２的初始生成速率是随反应物浓度的变化而变化的．当Ｈ２Ｏ的浓度大于ＣＯ的浓度时，Ｈ２的初始生成速率比ＣＯ２大；当ＣＯ的浓度大于Ｈ２Ｏ的浓度时，Ｈ２和ＣＯ２的生成速率始终保持相等；引入ＯＨ＊的扩散和Ｈ２Ｏ＊的脱附后。
The initial kinetics of two typical mechanisms for water\|gas shift reaction has been studied by Monte Carlo method. The simulated results show that (1) for oxidation\|reduction mechanism proposed by Temkin, the initial rate of CO2 formation is always much larger than that of H2 no matter what the ratio of CO concentration to H2O concentration is. (2) For L\|H mechanism proposed by Oki , the characteristics of CO2 and H2 initial formation rate changes with the ratio of CO concentration to H2O concentration. When H2O concentration is much higher than that of CO the initial rate of H2 formation is much larger than that of CO2. However, when CO concentration is higher than that of H2O the rate of H2 formation is all the time in step with that of CO2. Finally, when OH* diffusion or H2O* desorption is considered the kinetic characteristics described above are still obvious.
出处
《分子催化》
EI
CAS
CSCD
北大核心
1999年第2期131-136,共6页
Journal of Molecular Catalysis(China)
