催化作用
金属间化合物
三元运算
氨生产
离解(化学)
过渡金属
氨
材料科学
金属
化学
无机化学
化学物理
物理化学
冶金
有机化学
合金
计算机科学
程序设计语言
作者
Hongchen Li,Yutong Gong,Hongliang Yang,Xiao Yang,Ke Li,Junjie Wang,Hideo Hosono
出处
期刊:Chemsuschem
[Wiley]
日期:2023-08-16
卷期号:16 (22)
被引量:3
标识
DOI:10.1002/cssc.202301016
摘要
Intermetallic electrides have recently drawn considerable attention due to their unique electronic structure and high catalytic performance for the activation of inert chemical bonds under mild conditions. However, the relationship between electride (anionic) electron abundance and catalytic performance is undefined; the key deciding factor for the performance of intermetallic electride catalysts remains to be addressed. Here, the secret behind electride catalysts La-TM-Si (TM=Co, Fe and Mn) with the same crystal structure but different anionic electrons was studied. Unexpectedly, LaCoSi with the least anionic electrons showed the best catalytic activity. The experiments and first-principles calculations showed that the electride anions promote the N2 dissociation which alters the rate-determining step (RDS) for ammonia synthesis on the studied electrides. Different reaction mechanisms were found for La-TM-Si (TM=Fe, Co) and LaMnSi. A dual-site module was revealed for LaCoSi and LaFeSi, in which transition metals were available for the N2 dissociation and La accelerates the NHx formation, respectively, breaking the Sabatier scaling relation. For LaMnSi, which is the most efficient for the N2 activation, the activity for ammonia synthesis is limited and confined by the scaling relations. The findings provide new insight into the working mechanism of intermetallic electrides.
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