Journal
NATURE CHEMISTRY
Volume 3, Issue 7, Pages 532-537Publisher
NATURE PORTFOLIO
DOI: 10.1038/nchem.1051
Keywords
-
Categories
Funding
- Deutsche Forschungsgemeinschaft [SCHN950/2-1]
- international graduate school NanoCat
- Technische Universitat Munchen Graduate School
- Beilstein Institute as part of the NanoBiC research cooperative
- Center for Scientific Computing Frankfurt
Ask authors/readers for more resources
Bioinspired hydrogenation of N-2 to ammonia at ambient conditions by stepwise nitrogen protonation/reduction with metal complexes in solution has experienced remarkable progress. In contrast, the highly desirable direct hydrogenation with H-2 remains difficult. In analogy to the heterogeneously catalysed Haber-Bosch process, such a reaction is conceivable via metal-centred N-2 splitting and unprecedented hydrogenolysis of the nitrido ligands to ammonia. We report the synthesis of a ruthenium(IV) nitrido complex. The high nucleophilicity of the nitrido ligand is demonstrated by unusual N-C coupling with pi-acidic CO. Furthermore, the terminal nitrido ligand undergoes facile hydrogenolysis with H-2 at ambient conditions to produce ammonia in high yield. Kinetic and quantum chemical examinations of this reaction suggest cooperative behaviour of a phosphorus-nitrogen-phosphorus pincer ligand in rate-determining heterolytic hydrogen splitting.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available