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Electrocatalytically Active Fe‐(O‐C 2 ) 4 Single‐Atom Sites for Efficient Reduction of Nitrogen to Ammonia
Author(s) -
Zhang Shengbo,
Jin Meng,
Shi Tongfei,
Han Miaomiao,
Sun Qiao,
Lin Yue,
Ding Zhenhua,
Zheng Li Rong,
Wang Guozhong,
Zhang Yunxia,
Zhang Haimin,
Zhao Huijun
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202005930
Subject(s) - electrocatalyst , faraday efficiency , catalysis , nitrogen , carbon fibers , chemistry , yield (engineering) , ammonia production , electrochemistry , inorganic chemistry , ammonia , metal , reversible hydrogen electrode , atom (system on chip) , electrode , materials science , working electrode , composite number , organic chemistry , metallurgy , composite material , computer science , embedded system
Single‐atom catalysts have demonstrated their superiority over other types of catalysts for various reactions. However, the reported nitrogen reduction reaction single‐atom electrocatalysts for the nitrogen reduction reaction exclusively utilize metal–nitrogen or metal–carbon coordination configurations as catalytic active sites. Here, we report a Fe single‐atom electrocatalyst supported on low‐cost, nitrogen‐free lignocellulose‐derived carbon. The extended X‐ray absorption fine structure spectra confirm that Fe atoms are anchored to the support via the Fe‐(O‐C 2 ) 4 coordination configuration. Density functional theory calculations identify Fe‐(O‐C 2 ) 4 as the active site for the nitrogen reduction reaction. An electrode consisting of the electrocatalyst loaded on carbon cloth can afford a NH 3 yield rate and faradaic efficiency of 32.1 μg h −1 mg cat. −1 (5350 μg h −1 mg Fe −1 ) and 29.3 %, respectively. An exceptional NH 3 yield rate of 307.7 μg h −1 mg cat. −1 (51 283 μg h −1 mg Fe −1 ) with a near record faradaic efficiency of 51.0 % can be achieved with the electrocatalyst immobilized on a glassy carbon electrode.