Trigonal Prismatic or not Trigonal Prismatic? On the Mechanisms of Oxygen-Atom Transfer in Molybdopterin-Based Enzymes

Angewandte Chemie - International Edition

Volumn 43, Issue 5, 2004, Pages 546-549

  Kaupp, Martin ^a  

^a UNIVERSITY OF WÜRZBURG   (Germany)

Author keywords

Bioinorganic chemistry; Molybdenum; Oxotransferase enzymes; Reaction mechanisms; Transition metal complexes

Indexed keywords

CATALYSIS; CHEMICAL BONDS; QUANTUM THEORY;

ATOM TRANSFER;

ENZYMES;

CYSTEINE; DIMETHYL SULFOXIDE; DIMETHYL SULFOXIDE REDUCTASE; DITHIOL DERIVATIVE; MALEONITRILE 1,2 DITHIOLATE; MOLYBDENUM; MOLYBDOPTERIN; NITRILE; NITROGENASE; OXYGEN; OXYGENASE; SELENOCYSTEINE; SULFITE OXIDASE; TRANSFERASE; TRANSITION ELEMENT; TUNGSTEN; UNCLASSIFIED DRUG; XANTHINE OXIDASE;

CATALYSIS; COMPLEX FORMATION; CRYSTALLOGRAPHY; DENSITY FUNCTIONAL THEORY; ENZYME ACTIVE SITE; HIGH TEMPERATURE; OXIDATION REDUCTION REACTION; QUANTUM CHEMISTRY; REVIEW; SEQUENCE HOMOLOGY;

COENZYMES; IRON-SULFUR PROTEINS; METALLOPROTEINS; MODELS, MOLECULAR; MOLECULAR STRUCTURE; OXIDOREDUCTASES; OXYGEN; PROTEIN CONFORMATION; PTERIDINES;

EID: 1042288501     PISSN: 14337851     EISSN: None     Source Type: Journal    
DOI: 10.1002/anie.200301690     Document Type: Review

References (25)

1. C. E. Webster, M. B. Hall, J. Am. Chem. Soc. 2001, 123, 5820.
2. S. Thapper, R. J. Deeth, E. Nordlander, Inorg. Chem. 2002, 41, 6695.
3. M. Kaupp, Angew. Chem. 2001, 113, 3642;
4. Angew. Chem. Int. Ed. 2001, 40, 3534 and references therein.
5. R. Hille, Chem. Rev. 1996, 96, 2757.
6. M. K. Johnson, D. C. Rees, W. W. Adams. Chem. Rev. 1996, 96, 2817.
7. a) H. Schindelin, C. Kisker, J. Hilton, K. V. Rajagopalan, D. C. Rees, Science 1996, 272, 1615;
8. b) S. D. Garton, J. Hilton, H. Oku, B. R. Crouse, K. V. Rajgopalan, M. K. Johnson, J. Am. Chem. Soc. 1997, 119, 12906;
9. c) B. E. Schultz, R. Hille, R. H. Holm, J. Am. Chem. Soc. 1995, 117, 827.
10. a) K.-M. Sung, R. H. Holm, J. Am. Chem. Soc. 2002, 124, 4312;
11. b) B. S. Lim, R. H. Holm, J. Am. Chem. Soc. 2001, 123, 1920;
12. c) B. S. Lim, K.-M. Sung, R. H. Holm, J. Am. Chem. Soc. 2000, 122, 7410.
13. 2- form of the dithiolene ligand. It is important to note that this conventional oxidation-state formalism is not expected to be a very faithful representation for the true electronic situation of the molybdenum complex in question, owing to extensive delocalization.
14. H.-K. Li, C. Temple, K. V. Rajagopalan, H. Schindelin, J. Am. Chem. Soc. 2000, 122, 7573; J. C. Boyington, V. N. Gladyshev, S. V. Khangulov, T. C. Stadtman, P. D. Sun, Science 1997, 275, 1305; M. K. Chan, S. Mukund, A. Kletzin, M. W. W. Adams, D. C. Rees, Science 1995, 267, 1463.
15. H.-K. Li, C. Temple, K. V. Rajagopalan, H. Schindelin, J. Am. Chem. Soc. 2000, 122, 7573; J. C. Boyington, V. N. Gladyshev, S. V. Khangulov, T. C. Stadtman, P. D. Sun, Science 1997, 275, 1305; M. K. Chan, S. Mukund, A. Kletzin, M. W. W. Adams, D. C. Rees, Science 1995, 267, 1463.
16. H.-K. Li, C. Temple, K. V. Rajagopalan, H. Schindelin, J. Am. Chem. Soc. 2000, 122, 7573; J. C. Boyington, V. N. Gladyshev, S. V. Khangulov, T. C. Stadtman, P. D. Sun, Science 1997, 275, 1305; M. K. Chan, S. Mukund, A. Kletzin, M. W. W. Adams, D. C. Rees, Science 1995, 267, 1463.
17. B. L. Valee, R. J. P. Williams, Proc. Natl. Acad. Sci. USA 1968, 59, 498; R. J. P. Willliams. Eur. J. Biochem. 1995, 234, 363.
18. B. L. Valee, R. J. P. Williams, Proc. Natl. Acad. Sci. USA 1968, 59, 498; R. J. P. Willliams. Eur. J. Biochem. 1995, 234, 363.
19. M. Czizek, J.-P. Dos Santos, J. Pommier, G. Giordane, V. Méjean, R. Haser, J. Mol. Biol. 1998, 284, 435.
20. M. Kaupp, Chem. Eur. J. 1998, 4, 1678.
21. X. Wang, L. Andrews, J. Am. Chem. Soc. 2002, 124, 5637; X. Wang, L. Andrews, J. Phys. Chem. A 2002, 106, 6720.
22. X. Wang, L. Andrews, J. Am. Chem. Soc. 2002, 124, 5637; X. Wang, L. Andrews, J. Phys. Chem. A 2002, 106, 6720.
23. A. K. Rappé, W. A. Goddard III, J. Am. Chem. Soc. 1982, 104, 3287.
24. See, for example: P. Pyykkö, Chem. Rev. 1988, 88, 563.
25. M. Kunz, I. D. Brown, J. Solid State Chem. 1995, 115, 395.