动力学
化学
氨生产
氨
无机化学
氮气
材料科学
物理
量子力学
有机化学
作者
Yan Li,Junwei Li,Jianfeng Huang,Junxiang Chen,Yan Kong,Bin Yang,Lecheng Lei,Guoliang Chai,Zhenhai Wen,Liming Dai,Yang Hou
标识
DOI:10.1002/anie.202100526
摘要
Electrocatalytic nitrogen reduction reaction (NRR) plays a vital role for next-generation electrochemical energy conversion technologies. However, the NRR kinetics is still limited by the sluggish hydrogenation process on noble-metal-free electrocatalyst. Herein, we report the rational design and synthesis of a hybrid catalyst with atomic iron sites anchored on a N,O-doped porous carbon (FeSA -NO-C) matrix of an inverse opal structure, leading to a remarkably high NH3 yield rate of 31.9 μg NH 3 h-1 mg-1 cat. and Faradaic efficiency of 11.8 % at -0.4 V for NRR electrocatalysis, outperformed almost all previously reported atomically dispersed metal-nitrogen-carbon catalysts. Theoretical calculations revealed that the observed high NRR catalytic activity for the FeSA -NO-C catalyst stemmed mainly from the optimized charge-transfer between the adjacent O and Fe atoms homogenously distributed on the porous carbon support, which could not only significantly facilitate the transportation of N2 and ions but also effectively decrease the binding energy between the isolated Fe atom and *N2 intermediate and the thermodynamic Gibbs free energy of the rate-determining step (*N2 → *NNH).
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