碱土金属
催化作用
分解
氨
无机化学
化学
氨生产
土(古典元素)
环境化学
碱金属
有机化学
数学
数学物理
作者
Zhen Zhang,Minghui Yu,Meiqing Shen,Wei Li,Gurong Shen
标识
DOI:10.1016/j.mcat.2025.115016
摘要
• Alkaline earth metals enhance catalyst's activity in ammonia decomposition. • The incorporation of alkaline earth metals enhances the basicity of catalyst. • Electron-rich metal Ni° facilitates N* recombination and desorption. • The modified Ni/CeO 2 mitigates the impact of hydrogen inhibition. • Developing kinetic model and validating hydrogen inhibition. Ni-based catalysts, as non-noble metal alternatives, are widely regarded for their potential in ammonia decomposition for hydrogen production. However, their performance at low temperatures is suboptimal, necessitating the addition of promoters and a clear understanding of their mechanisms to enhance catalytic activity. In this study, we have successfully improved the low-temperature ammonia decomposition performance of Ni/CeO 2 by incorporating alkaline earth metals and conducted a comprehensive analysis of the underlying structural and electronic effects. The findings reveal that alkaline earth metals can enhance the basicity of the catalyst and increase electron density around the active metal sites, thereby facilitating the rate-determining step of recombination and desorption of N atom. Moreover, the presence of alkaline earth metals disrupts hydrogen adsorption stability on the catalysts, effectively mitigating the impact of hydrogen inhibition. Based on systematic kinetic experiments, a kinetic model was developed that accurately captures the hydrogen inhibition effect for Ni/CeO 2 catalysts. The insights into the promotional mechanisms of alkaline earth metals offer theoretical guidance for the development of highly active and cost-effective catalysts for ammonia decomposition.
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