催化作用
氨生产
氨
过渡金属
碱金属
碱土金属
反应速率
化学
材料科学
无机化学
化学工程
组合化学
有机化学
工程类
作者
Zichuang Li,Yangfan Lu,Li Jiang,Miao Xu,Yanpeng Qi,SangWon Park,Masaaki Kitano,Hideo Hosono,Jie‐Sheng Chen,Tian‐Nan Ye
标识
DOI:10.1038/s41467-023-42050-7
摘要
Abstract The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides ( Ae NH) combined with transition metal (TM = Fe, Co and Ni) catalysts can overcome this difficulty by utilizing functionalities arising from concerted role of active defects on the support surface and loaded transition metals. These catalysts enable ammonia production through multiple reaction pathways. The reaction rate of Co/SrNH is as high as 1686.7 mmol·g Co −1 ·h −1 and the TOFs reaches above 500 h −1 at 400 °C and 0.9 MPa, outperforming other reported Co-based catalysts as well as the benchmark Cs-Ru/MgO catalyst and industrial wüstite-based Fe catalyst under the same reaction conditions. Experimental and theoretical results show that the synergistic effect of nitrogen affinity of 3d TMs and in-situ formed NH 2− vacancy of alkali earth imides regulate the reaction pathways of the ammonia production, resulting in distinct catalytic performance different from 3d TMs. It was thus demonstrated that the appropriate combination of metal and support is essential for controlling the reaction pathway and realizing highly active and low cost catalysts for ammonia synthesis.
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