Mechanism of H2 metabolism on Fe-only hydrogenases

Journal of Chemical Physics

Volumn 117, Issue 18, 2002, Pages 8177-8180

  Liu, Zhi Pan ^a   Hu, P ^a  

^a QUEEN'S UNIVERSITY BELFAST   (United Kingdom)

Author keywords

[No Author keywords available]

Indexed keywords

APPROXIMATION THEORY; CRYSTAL STRUCTURE; ENZYMES; HYDROGENATION; IRON; METABOLISM; MOLECULAR STRUCTURE; NUMERICAL ANALYSIS; PROBABILITY DENSITY FUNCTION; REDOX REACTIONS; X RAY ANALYSIS;

HYDROGENASES; REACTION BARRIERS;

HYDROGEN;

EID: 0037044954     PISSN: 00219606     EISSN: None     Source Type: Journal    
DOI: 10.1063/1.1519252     Document Type: Article

References (29)

1. M. W. W. Adams, Biochim. Biophys. Acta 1020, 115 (1990).
2. A. E. Pryzbyla, J. Robbins, N. Menon, and H. D. Peck, FEMS Microbiol. Rev. 88, 109 (1992).
3. R. Cammack, Nature (London) 397, 214 (1999).
4. M. W. W. Adams, L. E. Mortenson, and J. S. Chen, Biochim. Biophys. Acta 594, 105 (1981).
5. J. W. Peters, Curr. Opin. Struct. Biol. 9, 670 (1999).
6. Y. Nicolet, C. Piras, P. Legrand, E. C. Hatchikian, and J. C. Fontecilla-Camps, Structure (London) 7, 13 (1999).
7. J. W. Peters, W. N. Lanzilotta, B. J. Lemon, and L. C. Seefeldt, Science 282, 1853, (1998).
8. A. L. De Lacey, C. Stadler, C. Cavazza, E. C. Hatchikian, and V. M. Fernandez, J. Am. Chem. Soc. 122, 11232 (2000).
9. A. J. Pierik, M. Hulstein, W. R. Hagen, and S. P. Albracht, Eur. J. Biochem. 258, 572 (1998).
10. Y. Nicolet, A. L. De Lacey, X. Vernede, V. M. Fernandez, E. C. Hatchikian, and J. C. Fontecilla-Camps, J. Am. Chem. Soc. 123, 1596 (2001).
11. I. Dance, Chem. Comm. 17, 1655 (1999).
12. H.-J. Fan and M. B. Hall, J. Am. Chem. Soc. 123, 3828 (2001).
13. 2 metabolism and generalizes the feature the electronics structure of the 2Fe subunit. The proposed redox states are consistent with all experimental data, such as geometries, IR spectrum EPR properties.
14. (a) J. P. Perdew, J. A. Chevary, S. H. Vosko, K. A. Jackson, M. R. Pederson, D. J. Singh, and C. Fiolhais, Phys. Rev. B 46, 6671 (1992);
15. (b) D. Vanderbilt, ibid. Rev. B 41, 7892 (1990).
16. The calculation methods used in this work are the same as that described in our previous paper, Ref. 13. The program used is CASTEP (see Ref. 23), which implements the DFT total energy calculation with plane wave basis set and ultrasoft pseudopotentials [see Ref. 14(b)]. The transition states searched with constrained minimization technique (see Refs. 16, 17). The accuracy of the current DFT total energy calculation, in particular for the calculation of reaction barriers (the error of the barrier is normally within 0.1 eV), has been demonstrated previously (see Refs. 13, 16, 17 and references therein). This calculation methods has been used to study biological systems, e.g., nitrogen fixation on MoFe6S9 (the active site of nitrogenase) by Norskov group. [T. H. Rod, B. Hammer, and J. K. Norskov, Phys. Rev. Lett. 82, 4054 (1999)].
17. Z.-P. Liu and P. Hu, J. Am. Chem. Soc. 123, 12596 (2001);
18. J. Chem. Phys. 114, 8244 (2001);
19. J. Chem. Phys. 115, 4977 (2001);
20. J. Chem. Phys. 114, 5956 (2001).
21. C. J. Zhang and P. Hu, J. Am. Chem. Soc. 123, 1166, (2001);
22. A. Michaelides and P. Hu, J. Am. Chem. Soc. 123, 4235 (2001);
23. A. Michaelides and P. Hu, ibid. 122, 9866 (2000).
24. Z. X. Cao and M. B. Hall, J. Am. Chem. Soc. 123, 3734 (2001).
25. M. Razavet, S. C. Davies, D. L. Hughes, and C. J. Pickett, Chem. Comm. 9, 847 (2001).
26. 2O near the N in the DTN, complex 6 can be stable.
27. Here the barriers for the proton and electron transfer are not considered since these processes are well-addressed and are believed to be efficient the enzymatic catalysis (see Refs. 1-7).
28. d-H bond breaking increases to 0.52 eV.
29. M. C. Payne, M. P. Teter, D. C. Allan, T. A. Arias, and J. D. Joannopoulos, Rev. Mod. Phys. 64, 1045 (1992).