Reactive Monte Carlo and grand-canonical Monte Carlo simulations of the propene metathesis reaction system
Reactive Monte Carlo and grand-canonical Monte Carlo simulations of the propene metathesis reaction system
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DOI：
10.1063/1.1884108
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发表时间：
2005-04-22
影响因子：
4.4
通讯作者：
Keil, FJ
中科院分区：
文献类型：
--
作者：
Hansen, N;Jakobtorweihen, S;Keil, FJ
用分子模拟方法研究了Silicalite-1孔对丙烯歧化反应体系在300~600K和0.5~7bar压力范围内的反应平衡和选择性的影响。用反应蒙特卡罗(RxMC)方法模拟了等压等温系综中的体相和Gibbs系综中的两相体系。此外，在巨正则系综(GCMC)中进行了蒙特卡罗模拟，分别使用和不使用RxMC技术。各种模拟程序与构型偏置蒙特卡罗方法相结合。结果表明，对于体相平衡可以预先计算的反应，GCMC模拟优于Gibbs系综模拟，而不必与孔内分子同时进行模拟。受限环境可以显著提高转化率。体相和孔相之间的选择性有很大的变化。压力和温度对转化率和选择性都有很大影响。在较低的压力和温度下，转化率和选择性都有最高值。禁闭效应随着温度的升高而减小。D 2005年美国物理研究所。
The influence of silicalite-1 pores on the reaction equilibria and the selectivity of the propene metathesis reaction system in the temperature range between 300 and 600 K and the pressure range from 0.5 to 7 bars has been investigated with molecular simulations. The reactive Monte Carlo (RxMC) technique was applied for bulk-phase simulations in the isobaric-isothermal ensemble and for two phase systems in the Gibbs ensemble. Additionally, Monte Carlo simulations in the grand-canonical ensemble (GCMC) have been carried out with and without using the RxMC technique. The various simulation procedures were combined with the configurational-bias Monte Carlo approach. It was found that the GCMC simulations are superior to the Gibbs ensemble simulations for reactions where the bulk-phase equilibrium can be calculated in advance and does not have to be simulated simultaneously with the molecules inside the pore. The confined environment can increase the conversion significantly. A large change in selectivity between the bulk phase and the pore phase is observed. Pressure and temperature have strong influences on both conversion and selectivity. At low pressure and temperature both conversion and selectivity have the highest values. The effect of confinement decreases as the temperature increases. D 2005 American Institute of Physics.