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Lithium Imide Synergy with 3d Transition‐Metal Nitrides Leading to Unprecedented Catalytic Activities for Ammonia Decomposition
Author(s) -
Guo Jianping,
Wang Peikun,
Wu Guotao,
Wu Anan,
Hu Daqiang,
Xiong Zhitao,
Wang Junhu,
Yu Pei,
Chang Fei,
Chen Zheng,
Chen Ping
Publication year - 2015
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.201410773
Subject(s) - catalysis , nitride , imide , alkali metal , ternary operation , transition metal , decomposition , chemistry , ammonia , inorganic chemistry , lithium (medication) , materials science , organic chemistry , medicine , layer (electronics) , computer science , programming language , endocrinology
Alkali metals have been widely employed as catalyst promoters; however, the promoting mechanism remains essentially unclear. Li, when in the imide form, is shown to synergize with 3d transition metals or their nitrides TM(N) spreading from Ti to Cu, leading to universal and unprecedentedly high catalytic activities in NH 3 decomposition, among which Li 2 NHMnN has an activity superior to that of the highly active Ru/carbon nanotube catalyst. The catalysis is fulfilled via the two‐step cycle comprising: 1) the reaction of Li 2 NH and 3d TM(N) to form ternary nitride of LiTMN and H 2 , and 2) the ammoniation of LiTMN to Li 2 NH, TM(N) and N 2 resulting in the neat reaction of 2 NH 3 ⇌N 2 +3 H 2 . Li 2 NH, as an NH 3 transmitting agent, favors the formation of higher N‐content intermediate (LiTMN), where Li executes inductive effect to stabilize the TMN bonding and thus alters the reaction energetics.