Zhang Bin, Yang Kun, Liu Danyang, Xiao Yiwen, Zhang Kaining, Yang Tuo, Lu Jianying, Wu Junying, Chen Lang
State Key Laboratory of Explosion Science and Safety Protection, Beijing Institute of Technology, Beijing 100081, China.
ACS Omega. 2024 Sep 18;9(39):40446-40455. doi: 10.1021/acsomega.4c02889. eCollection 2024 Oct 1.
The reaction of gaseous hydrogen halides with alkali metals provides a new pathway for producing hydrogen. The structure and reactivity of alkali metals are crucial for the reduction of gaseous halides. However, traditional gas-phase reaction models fail to provide insights into the dynamic processes occurring during alkali metal reactions. In this paper, based on the reaction between Hydrogen fluoride (HF) and alkali metal sodium (Na), we have established a metallic Na slab. HF molecules were randomly inserted above the surface of the Na slab, creating a reaction model for the reduction of HF by metallic Na. The reaction of HF on the Na surface was calculated using first-principles molecular dynamics. The configuration and reaction of the Na surface and HF molecules at different times were judged by analyzing the radial distribution function and mean squared displacement. Na atoms reacted with HF to produce intermediate NaFH, and then the F-H bond broke to form NaF and H. The F-H bond breaking of intermediate NaFH was the key step, and the kinetic parameters of this key step were calculated.
气态卤化氢与碱金属的反应为制氢提供了一条新途径。碱金属的结构和反应活性对于气态卤化物的还原至关重要。然而,传统的气相反应模型无法深入了解碱金属反应过程中发生的动态过程。本文基于氟化氢(HF)与碱金属钠(Na)之间的反应,建立了金属钠平板模型。HF分子随机插入到钠平板表面上方,构建了金属钠还原HF的反应模型。利用第一性原理分子动力学计算了HF在钠表面的反应。通过分析径向分布函数和均方位移来判断不同时刻钠表面和HF分子的构型及反应情况。Na原子与HF反应生成中间体NaFH,然后F-H键断裂形成NaF和H。中间体NaFH的F-H键断裂是关键步骤,并计算了该关键步骤的动力学参数。