Climbing nitrogenase: Toward a mechanism of enzymatic nitrogen fixation

Accounts of Chemical Research

Volumn 42, Issue 5, 2009, Pages 609-619

  Hoffman, Brian M ^a   Dean, Dennis R ^b   Seefeldt, Lance C ^c  

^a NORTHWESTERN UNIVERSITY   (United States)

^b VIRGINIA POLYTECHNIC INSTITUTE AND STATE UNIVERSITY   (United States)

^c UTAH STATE UNIVERSITY   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

MOLYBDENUM IRON PROTEIN; NITROGENASE;

ARTICLE; BIOLOGICAL MODEL; CHEMICAL STRUCTURE; CHEMISTRY; NITROGEN FIXATION; OXIDATION REDUCTION REACTION; SIGNAL TRANSDUCTION;

MODELS, BIOLOGICAL; MOLECULAR STRUCTURE; MOLYBDOFERREDOXIN; NITROGEN FIXATION; NITROGENASE; OXIDATION-REDUCTION; SIGNAL TRANSDUCTION;

EID: 66149110298     PISSN: 00014842     EISSN: None     Source Type: Journal    
DOI: 10.1021/ar8002128     Document Type: Article

References (42)

1. Zhao, Y.; Bian, S.-M.; Zhou, H.-N.; Huang, J.-F. Diversity of nitrogenase systems in diazotrophs. J. Intear. Plant Biol. 2006, 48, 745-755.
2. Burgess, B. K.; Lowe, D. L. Mechanism of molybdenum nitrogenase. Chem. Rev. 1996, 96, 2983-3011.
3. Thorneley, R. N. F.; Lowe, D. J. In Molybdenum Enzymes; Spiro, T. G., Ed.; Wiley-Interscience: New York, 1985; Vol. 7; pp 89-116.
4. Wilson, P. E.; Nyborg, A. C.; Watt, G. D. Duplication and extension of the Thorneley and Lowe kinetic model for Klebsiella pneumoniae nitrogenase catalysis using a MATHEMATICA software platform. Biophvs. Chem. 2001, 91, 281-304.
5. Rees, D. C.; Tezcan, F. A.; Haynes, C. A.; Walton, M. Y.; Andrade, S.; Einsle, 0.; Howard, J. B. Structural basis of biological nitrogen fixation. Philos. Trans. R. Soc. A 2005, 363, 971-984.
6. 2? A mechanistic overview of biological nitrogen fixation. Proc. Natl. Acad. Sci. U.S.A. 2006, 103, 17088-17093.
7. Schrock, R. R. Reduction of dinitrogen. Proc. Natl. Acad. Sci. U.S.A. 2006, 103, 17087.
8. 2 triple bond: insights into the nitrogenase mechanism. Dalton Trans. 2006, 2277-2284.
9. Dos Santos, P. C.; Igarashi, R. Y.; Lee, H.-l.; Hoffman, B. M.; Seefeldt, L. C.; Dean, D. R. Substrate interactions with the nitrogenase active site. Acc. Chem. Res. 2005, 35, 208-214.
10. Seefeldt, L. C.; Hoffman, B. M.; Dean, D. R. Mechanism of Mo-dependent nitrogenase. Annu. Rev. Biochem. 2009, in press.
11. Davis, L. C.; Henzl, M. T.; Burris, R. H.; Orme-Johnson, W. H. Iron-sulfur clusters in the molybdenum-iron protein component of nigrogenase. Electron paramagnetic resonance of the carbon monoxide inhibited state. Biochemistry 1979, 18, 4860-4869.
12. Cameron, L. M.; Hales, B. J. Investigation of CO binding and release from Mo-nitrogenase during catalytic turnover. Biochemistry 1998, 37, 9449-9456.
13. Einsle, O.; Tezcan, F. A.; Andrade, S. L. A.; Schmid, B.; Yoshida, M.; Howard, J. B.; Rees, D. C. Nitrogenase MoFe-protein at 1.16 Å resolution: A central ligandinthe FeMo-cofactor. Science 2002, 297, 1696-1700.
14. Schrock, R. R. Catalytic reduction of dinitrogen to ammonia at a single molybdenum center. Acc. Chem. Res. 2005, 38, 955-962.
15. Eady, R. R. Structure-function relationships of alternative nitrogenases. Chem. Rev. 1996, 96, 3013-3030.
16. Madden, M. S.; Paustian, T. D.; Ludden, P. W.; Shah, V. K. Effects of homocitrate, homocitrate lactone, and fluorohomocitrate on nitrogenase in NifV-mutants of Azotobacter vinelandii. J. Bacteriol. 1991, 173, 5403-5405.
17. Lukoyanov, D.; Pelmenschikov, V.; Maeser, N.; Laryukhin, M.; Yang, T. C.; Noodleman, L.; Dean, D.; Case, D.; Seefeldt, L.; Hoffman, B. Testing if the interstitial atom, X, of the nitrogenase molybdenum-iron cofactor is N or C: ENDOR, ESEEM, and DFT studies of the S = 3/2 resting state in multiple environments. Inorg. Chem. 2007, 46, 11437-11449.
18. Blankenship, R. E. Molecular Mechanisms of Photosynthesis. 1st ed.; Blackwell Science, Ltd.: Oxford, U.K., 2002.
19. Sorlie, M.; Christiansen, J.; Lemon, B. J.; Peters, J. W.; Dean, D. R.; Hales, B. J. Mechanistic features and structure of the nitrogenase a-Gln195 MoFe protein. Biochemistry 2001, 40, 1540-1549.
20. 2 binding and reduction, HD formation, and azide reduction with a-195His- and a-191 Gin-substituted MoFe proteins of Azotobacter vinelandii nitrogenase. Biochemistrv 2000, 39, 15570-15577.
21. Lee, H.-L.; Igarashi, R. Y.; Laryukhin, M.; Doan, P. E.; Dos Santos, P. C.; Dean, D. R.; Seefeldt, L. C.; Hoffman, B. M. An organometallic intermediate during alkyne reduction by nitrogenase. J. Am. Chem. Soc. 2004, 126, 9563-9569.
22. 2 and CO. J. Am. Chem. Soc. 2005, 127, 15880-15890.
23. 2 evolution: Characterization by ENDOR spectroscopy. J. Am. Chem. Soç. 2005, 727, 6231-6241.
24. Barney, B. M.; Laryukhin, M.; Igarashi, R. Y.; Lee, H.-l.; Santos, P. C. D.; Yang, T.-C.; Hoffman, B. M.; Dean, D. R.; Seefeldt, L. C. Trapping a hydrazine reduction intermediate on the nitrogenase active site. Biochemistry 2005, 44, 8030-8037.
25. 2. J. Am. Chem. Soc. 2005, 127, 14960-14961.
26. 3)-derived species bound to the nitrogenase active-site FeMo cofactor: Implications for mechanism. Proc. Natl. Acad. Sci. U.S.A. 2006, 103, 17113-17118.
27. 2 reduction. Biochemistrv 2007, 46, 6784-6794.
28. Hoffman, B. M.; DeRose, V. J.; Doan, P. E.; Gurbiel, R. J.; Houseman, A. L P.; Telser, J. Metalloenzyme active-site structure and function through multifrequency CW and pulsed ENDOR. Biol. Magn. Reson 1993, 13 (EMR of Paramagnetic Molecules), 151-218.
29. Schweiger, A.; Jeschke, G. Principles of Pulse Electron Paramagnetic Resonance, Oxford University Press: Oxford, U.K., 2001.
30. 57Fe isotopomers. J. Am. Chem. Soc. 1996, 118, 8707-8709.
31. 1H Q-band ENDOR investigation. J. Am. Chem. Soc. 1997, 119, 10121-10126.
32. Pickett, C. J. The Chatt cycle and the mechanism of enzymic reduction of molecular nitrogen. JBIC. J. Biol. Inorg. Chem 1996, 7, 601-606.
33. Hinnemann, B.; Norskov, J. K. Chemical activity of the nitrogenase FeMo cofactor with a central nitrogen ligand: Density functional study. J. Am. Chem. Soc. 2004, 126, 3920-3927.
34. Dilworth, M. J.; Thorneley, R. N. F. Nitrogenase of Klebsiella pneumoniae. Hydrazine is a product of azide reduction. Biochem. J. 1981, 193, 971-983.
35. Davis, L. C. Hydrazine as a substrate and inhibitor of Azotobacter vinelandii nitrogenase. Arch. Biochem. Biophys. 1980, 204, 270-276.
36. Lees, N. S.; McNaughton, R. L.; Gregory, W. V.; Vela, J.; Holland, P. L.; Hoffman, B. M. ENDOR characterization of a synthetic diiron hydrazido complex as a model for nitrogenase intermediates. J. Am. Chem. Soc. 2008, 130, 546-555.
37. Mehn, M. P.; Peters, J. C. Mid- to high-valent imido and nitrido complexes of iron. J. Inorg. Biochem. 2006, 100, 634-643.
38. Holland, P. L. Electronic structure and reactivity of three-coordinate iron complexes. Acc. Chem. Res. 2008, 41, 905-914.
39. 2 binding state. Proc. Natl. Acad. Sci. U.S.A. 2007, 104, 1451-1455.
40. Lowe, D. J.; Fisher, K.; Thorneley, R. N. F. Klebsiella pneumoniae nitrogenase. Mechanism of acetylene reduction and its inhibition bv carbon monoxide. Biochem. J. 1990, 272, 621-5.
41. Davydov, R.; Matsui, T.; Fujii, H.; Ikeda-Saito, M.; Hoffman, B. M. Kinetic isotope effects on the rate-limiting step of heme oxygenase catalysis indicate concerted proton transfer/heme hydroxylation. J. Am. Chem. Soc. 2003, 125, 16208-16209.
42. Chan, J. M.; Christiansen, J.; Dean, D. R.; Seefeldt, L. C. Spectroscopie evidence for changes in the redox state of the nitrogenase P-cluster during turnover. Biochemistry 1999, 38, 5779-5785.