期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 38, 页码 11417-11420出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201604917
关键词
ammonia; dihydrogen; nitride; nitrogen fixation; osmium
资金
- European Research Council (ERC) [646747]
Low-valent osmium nitrides are discussed as intermediates in nitrogen fixation schemes. However, rational synthetic routes that lead to isolable examples are currently unknown. Here, the synthesis of the square-planar osmium(IV) nitride [OsN(PNP)] (PNP=N(CH2CH2P(tBu)(2))(2)) is reported upon reversible deprotonation of osmium(VI) hydride [Os(N)H(PNP)](+). The Os-IV complex shows ambiphilic nitride reactivity with SiMe3Br and PMe3, respectively. Importantly, the hydrogenolysis with H-2 gives ammonia and the polyhydride complex [OsH4(HPNP)] in 80% yield. Hence, our results directly demonstrate the role of low-valent osmium nitrides and of heterolytic H-2 activation for ammonia synthesis with H-2 under basic conditions.
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