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Ammonia Synthesis Under Ambient Conditions: Selective Electroreduction of Dinitrogen to Ammonia on Black Phosphorus Nanosheets
Author(s) -
Zhang Lili,
Ding LiangXin,
Chen GaoFeng,
Yang Xianfeng,
Wang Haihui
Publication year - 2019
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.201813174
Subject(s) - catalysis , ammonia , electrochemistry , zigzag , electrocatalyst , nitrogen , density functional theory , nitrogen fixation , ammonia production , inorganic chemistry , chemistry , materials science , phosphorus , yield (engineering) , black phosphorus , metal , redox , chemical engineering , organic chemistry , electrode , computational chemistry , metallurgy , geometry , mathematics , optoelectronics , engineering
Constructing efficient catalysts for the N 2 reduction reaction (NRR) is a major challenge for artificial nitrogen fixation under ambient conditions. Herein, inspired by the principle of “like dissolves like”, it is demonstrated that a member of the nitrogen family, well‐exfoliated few‐layer black phosphorus nanosheets (FL‐BP NSs), can be used as an efficient nonmetallic catalyst for electrochemical nitrogen reduction. The catalyst can achieve a high ammonia yield of 31.37 μg h −1 mg −1 cat. under ambient conditions. Density functional theory calculations reveal that the active orbital and electrons of zigzag and diff‐zigzag type edges of FL‐BP NSs enable selective electrocatalysis of N 2 to NH 3 via an alternating hydrogenation pathway. This work proves the feasibility of using a nonmetallic simple substance as a nitrogen‐fixing catalyst and thus opening a new avenue towards the development of more efficient metal‐free catalysts.