电合成
氨生产
电催化剂
催化作用
材料科学
氮气
无机化学
氨
化学工程
动力学
法拉第效率
电化学
氧化还原
化学
物理化学
有机化学
工程类
物理
量子力学
电极
作者
Yan Kong,Yan Li,Xiahan Sang,Bin Yang,Sixing Zheng,Qinghua Zhang,Siyu Yao,Xiaoxuan Yang,Lecheng Lei,Shaodong Zhou,Gang Wu,Yang Hou
标识
DOI:10.1002/adma.202103548
摘要
Developing highly active and stable nitrogen reduction reaction (NRR) catalysts for NH3 electrosynthesis remains challenging. Herein, an unusual NRR electrocatalyst is reported with a single Zn(I) site supported on hollow porous N-doped carbon nanofibers (Zn1 N-C). The Zn1 N-C nanofibers exhibit an outstanding NRR activity with a high NH3 yield rate of ≈16.1 µg NH3 h-1 mgcat-1 at -0.3 V and Faradaic efficiency (FE) of 11.8% in alkaline media, surpassing other previously reported carbon-based NRR electrocatalysts with transition metals atomically dispersed and nitrogen coordinated (TM-Nx ) sites. 15 N2 isotope labeling experiments confirm that the feeding nitrogen gas is the only nitrogen source in the production of NH3 . Structural characterization reveals that atomically dispersed Zn(I) sites with Zn-N4 moieties are likely the active sites, and the nearby graphitic N site synergistically facilitates the NRR process. In situ attenuated total reflectance-Fourier transform infrared measurement and theoretical calculation elucidate that the formation of initial *NNH intermediate is the rate-limiting step during the NH3 production. The graphitic N atoms adjacent to the tetracoordinate Zn-N4 moieties could significantly lower the energy barrier for this step to accelerate hydrogenation kinetics duing the NRR.
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