催化作用
氨生产
纳米颗粒
纳米技术
化学
氨
灵敏度(控制系统)
材料科学
化学工程
有机化学
工程类
电子工程
作者
Lingling Li,Yafei Jiang,Tianhua Zhang,Hualin Cai,Yanliang Zhou,Bingyu Lin,Xingyi Lin,Ying Zheng,Lirong Zheng,Xiuyun Wang,Chaoqun Xu,Chak Tong Au,Lilong Jiang,Jun Li
出处
期刊:Chem
[Elsevier]
日期:2022-03-01
卷期号:8 (3): 749-768
被引量:36
标识
DOI:10.1016/j.chempr.2021.11.008
摘要
Summary
Ammonia synthesis is structure sensitive, and a minute change in the catalyst structure would cause a dramatic change in activity. To date, none of the studies reveal the metal size effect at a subnanometer scale on NH3 synthesis, and such investigation remains a challenge. Here, we report the synthesis of Ru catalysts with sizes ranging from single atoms, atomic clusters (ACCs), sub-nanometric clusters, to nanoparticles (NPs) by adjusting precursor and/or loading of Ru. Sub-nanometric Ru catalysts not only exhibit performance different from that of NPs but also follow a different route for N2 activation. The strong intra-cluster interaction of Ru atomic clusters enables the formation of strong interactions of Ru d-orbitals with the σ and π orbitals of N2 molecules, resulting in N2 activation over Ru ACCs to occur more easily than that over Ru NPs. Consequently, Ru ACCs display an unprecedentedly high NH3 synthesis rate and large turnover frequency at mild conditions.
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