Hydrogenation and cleavage of dinitrogen to ammonia with a zirconium complex

Nature

Volumn 427, Issue 6974, 2004, Pages 527-530

  Pool, Jaime A ^a   Lobkovsky, Emil ^a   Chirik, Paul J ^a  

^a Baker Laboratory Cornell University ^*  (United States)

Author keywords

[No Author keywords available]

Indexed keywords

AMMONIA; CATALYSIS; CATALYSTS; CHEMICAL BONDS; HYDROGENATION; IONIZATION; STOICHIOMETRY; ZIRCONIUM COMPOUNDS;

IONIZATION POTENTIALS; NONPOLARITY;

NITROGEN;

AMMONIA; CYCLOPENTADIENE DERIVATIVE; LIGAND; METAL COMPLEX; NITROUS OXIDE; ZIRCONIUM DERIVATIVE;

AMMONIA; ZIRCONIUM;

ARTICLE; CATALYST; COMPLEX FORMATION; HIGH TEMPERATURE; HYDROGEN BOND; HYDROGENATION; IONIZATION; PRESSURE; PRIORITY JOURNAL; PROTON TRANSPORT; REACTION ANALYSIS; WARMING;

AMMONIA; CATALYSIS; CRYSTALLOGRAPHY, X-RAY; HYDROGEN; HYDROGEN BONDING; HYDROGENATION; MAGNETIC RESONANCE SPECTROSCOPY; MOLECULAR STRUCTURE; NITROGEN; PROTONS; TEMPERATURE; ZIRCONIUM;

HABER;

EID: 1142280731     PISSN: 00280836     EISSN: None     Source Type: Journal    
DOI: 10.1038/nature02274     Document Type: Article

References (19)

1. Schlögl, R. Catalytic synthesis of ammonia - A never-ending story. Angew. Chem. Int. Edn Engl. 42, 2004-2008 (2003).
2. Smil, V. Enriching the Earth (MIT Press, Cambridge, MA, 2001).
3. Bielawa, H., Hinrichsen, O., Birkner, A. & Muhler, M. The ammonia-synthesis catalyst of the next generation: barium-promoted oxide-supported ruthenium. Angew. Chem. Int. Edn Engl. 40, 1061-1063 (1999).
4. Fryzuk, M. D. & Johnson, S. A. The continuing story of dinitrogen activation. Coord. Chem. Rev. 200, 379-409 (2000).
5. Hidai, M. Chemical nitrogen fixation by molybdenum and tungsten complexes. Coord. Chem. Rev. 186, 99-108 (1999).
6. Yandulov, D. M. & Schrock, R. R. Catalytic reduction of dinitrogen to ammonia at a single molybdenum center. Science 301, 76-78 (2003).
7. Fryzuk, M. D., Love, J. B. & Rettig, S. J. Transformation of coordinated dinitrogen by reaction with dihydrogen and primary silanes. Science 275, 1445-1447 (1997).
8. Pool, J. A., Lobkovsky, E. & Chirik, P. J. Cyclopentadienyl substituent effects on reductive elimination reactions in group 4 metallocenes: kinetics, mechanism and application to dinitrogen activation. J. Am. Chem. Soc. 125, 2241-2251 (2003).
9. 2. Angew. Chem. Int. Edn Engl. 41, 3463-3466 (2002).
10. 2]? A theoretical study. J. Am. Chem. Soc. 121, 5754-5761 (1999).
11. 2] activate more than one hydrogen molecule? A theoretical study. Organometallics 19, 3393-3403 (2000).
12. Janiak, C., Versteeg, U., Lange, K. C. H., Weiman, R. & Hahn, E. The influence of electronic and steric effects and the importance of polymerization conditions in the ethylene polymerization with zirconocene/MAO catalysts. J. Organomet. Chem. 501, 219-234 (1995).
13. 2). J. Am. Chem. Soc. 98, 8351-8357 (1976).
14. Fryzuk, M. D. Activation and functionalization of molecular nitrogen by transition metal complexes. Chem. Rec. 3, 2-11 (2003).
15. Manriquez, J. M. et al. Solution structure and dynamics of binuclear dinitrogen complexes of bis(pentamethylcydopentadienyl) titanium (II) and bis(pentamethylcyclopentadienyl) zirconium (II). J. Am. Chem. Soc. 100, 3078-3083 (1978).
16. Manriquez, J. M. & Bercaw, J. E. Preparation of a dinitrogen complex of bis(pentamethylcydopentadienyl) zirconium (II). Isolation and protonation leading to stoichiometric reduction of dinitrogen to hydrazine. J. Am. Chem. Soc. 96, 6229-6230 (1974).
17. 3. J. Am. Chem. Soc. 110, 8731-8733 (1988).
18. Chaney, A. L. & Marbach, E. P. Modified reagents for determination of urea and ammonia. Clin. Chem. 8, 130-132 (1962).
19. Hillhouse, G. L. & Bercaw, J. E. Reactions of water and ammonia with bis(pentamethylcyclopentadienyl) complexes of zirconium and hafnium. J. Am. Chem. Soc. 106, 5472-5478 (1984).