期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 15, 页码 4786-4789出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201600790
关键词
acetonitrile; nitrogen fixation; pincer ligands; rhenium; small-molecule activation
资金
- European Research Council (ERC) [646747]
- European Research Council (ERC) [646747] Funding Source: European Research Council (ERC)
About 20% of the ammonia production is used as the chemical feedstock for nitrogen-containing chemicals. However, while synthetic nitrogen fixation at ambient conditions has had some groundbreaking contributions in recent years, progress for the direct conversion of N-2 into organic products remains limited and catalytic reactions are unknown. Herein, the rhenium-mediated synthesis of acetonitrile using dinitrogen and ethyl triflate is presented. A synthetic cycle in three reaction steps with high individual isolated yields and recovery of the rhenium pincer starting complex is shown. The cycle comprises alkylation of a nitride that arises from N-2 splitting and subsequent imido ligand centered oxidation to nitrile via a 1-azavinylidene (ketimido) intermediate. Different synthetic strategies for intra- and intermolecular imido ligand oxidation and associated metal reduction were evaluated that rely on simple proton, electron, and hydrogen-atom transfer steps.
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