Conversion of Dinitrogen into Acetonitrile under Ambient Conditions
2016 | journal article. A publication with affiliation to the University of Göttingen.
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Conversion of Dinitrogen into Acetonitrile under Ambient Conditions
Klopsch, I.; Kinauer, M.; Finger, M.; Wuertele, C. & Schneider, S. (2016)
Angewandte Chemie International Edition, 55(15) pp. 4786-4789. DOI: https://doi.org/10.1002/anie.201600790
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Details
- Authors
- Klopsch, Isabel; Kinauer, Markus; Finger, Markus; Wuertele, Christian; Schneider, Sven
- Abstract
- 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.
- Issue Date
- 2016
- Status
- published
- Publisher
- Wiley-v C H Verlag Gmbh
- Journal
- Angewandte Chemie International Edition
- ISSN
- 1521-3773; 1433-7851
- Sponsor
- European Research Council (ERC) [646747]