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本文在H-Li(100)面吸附扩散的ab initio SCF势能面基础上构造了(H_2H+H)/Li(100)面相互作用的推广LEPS势能面,并用QCT方法研究了该体系的反应动力学行为。分析势能面特征得到:H_2在Li(100)面上的吸附无需活化能,H_2在Li(100)面上的解离吸附与吸附位及吸附模式密切相关,H_2的卧式解离比立式解离要容易得多。分析各种碰撞轨迹得到:低覆盖度下双氢原子的表面复合几率很小,H_2的表面解离几率受到H_2振动量子数的控制。本文构造了一种适合于动力学研究的气体-金属表面相互作用势能面,并且,动力学QCT计算结果能够对H_2表面活化的分子束实验作出合理的解释。
In this paper, an extended LEPS potential surface of (H_2H + H) / Li (100) surface interaction is constructed on the ab initio SCF potential surface of H-Li (100) adsorbed and diffused, and the reaction kinetics of the system is studied by QCT Academic behavior. The analysis of the potential energy surface shows that there is no activation energy required for the adsorption of H_2 on the Li (100) surface, the dissociative adsorption of H_2 on the Li (100) surface is closely related to the adsorption site and adsorption mode, and the H 2 horizontal dissociation ratio Dissociation is much easier. The analysis of various collision trajectories shows that the surface recombination probability of hydrogen atoms in the low coverage is very small and the surface dissociation probability of H 2 is controlled by the H 2 vibration quantum number. In this paper, we construct a gas-metal surface potential energy surface that is suitable for the study of kinetics, and the kinetic QCT calculation results can reasonably explain the H 2 surface activation molecular beam experiment.