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Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Tuning Electron Distribution of Single‐Atomic Iron Sites
Author(s) -
Li Yan,
Li Junwei,
Huang Junheng,
Chen Junxiang,
Kong Yan,
Yang Bin,
Li Zhongjian,
Lei Lecheng,
Chai Guoliang,
Wen Zhenhai,
Dai Liming,
Hou Yang
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202100526
Subject(s) - electrocatalyst , catalysis , faraday efficiency , chemistry , electrochemistry , gibbs free energy , inorganic chemistry , redox , carbon fibers , nitrogen , yield (engineering) , materials science , electrode , thermodynamics , organic chemistry , physics , composite material , composite number , metallurgy
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 (Fe SA ‐NO‐C) matrix of an inverse opal structure, leading to a remarkably high NH 3 yield rate of 31.9 μgNH3 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 Fe SA ‐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 N 2 and ions but also effectively decrease the binding energy between the isolated Fe atom and *N 2 intermediate and the thermodynamic Gibbs free energy of the rate‐determining step (*N 2 → *NNH).