Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 54, Issue 10, Pages 2950-2954Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201410773
Keywords
ammonia decomposition; electronic promoter; heterogeneous catalysis; lithium imide; nitrides
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Funding
- National Natural Science Funds for Distinguished Young Scholars [51225206]
- 973 Project [2010CB631304]
- National Natural Science Foundation of China [21133004, 21273187]
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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 NH3 decomposition, among which Li2NHMnN 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 Li2NH and 3d TM(N) to form ternary nitride of LiTMN and H-2, and 2)the ammoniation of LiTMN to Li2NH, TM(N) and N-2 resulting in the neat reaction of 2NH(3)N(2)+3H(2). Li2NH, as an NH3 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.
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