Monte Carlo Simulations of Reaction Kinetics for Ethane Hydrogenolysis over Pt
Monte Carlo Simulations of Reaction Kinetics for Ethane Hydrogenolysis over Pt
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DOI：
10.1021/jp020345z
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发表时间：
2002-08
影响因子：
3.3
通讯作者：
S. Podkolzin;R. Alcalá;J. Pablo;J. Dumesic
中科院分区：
文献类型：
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作者：
S. Podkolzin;R. Alcalá;J. Pablo;J. Dumesic
的Monte Carlo（MC）分子模型，与来自密度泛函理论计算的参数，是用来描述的实验数据的乙烷氢解率的Pt/SiO2催化剂在很宽的范围内的条件。最丰富的稳定物种（氢原子，次乙基物种，和二-σ-键合的乙烯）的表面浓度与MC巨正则系综模拟，乙烷氢解速率通过模拟表面浓度为三种类型的过渡态复合物的C-C键断裂。模拟结果表明，吸附的C2 Hx和H物种之间的排斥作用越大，相对于氢压的反应级数越负。MC模拟的结果表明，该反应主要通过吸附的C2 H5物种中的C-C键断裂进行，吸附的CHCH 3和CHCH 2物种的贡献较小。MC的结果表明，虽然最丰富的表面烃类物种，
A Monte Carlo (MC) molecular model, with parameters derived from density functional theory calculations, is used to describe experimental data for the rate of ethane hydrogenolysis for a Pt/SiO2 catalyst over a wide range of conditions. The surface concentrations of the most abundant stable species (hydrogen atoms, ethylidyne species, and di-σ-bonded ethylene) are simulated with a MC grandcanonical ensemble, and the rate of ethane hydrogenolysis is calculated by simulating surface concentrations for three types of transition state complexes for C−C bond cleavage. The simulation shows that larger repulsive interactions between adsorbed C2Hx and H species lead to more negative reaction orders with respect to the hydrogen pressure. The results of the MC simulation indicate that the reaction proceeds primarily through C−C bond cleavage in adsorbed C2H5 species, with smaller contributions from adsorbed CHCH3 and CHCH2 species. The MC results suggest that although the most abundant surface hydrocarbon species h...