The effects of the dimethylether bridging moiety in the H-cluster of the Clostridium pasteurianum hydrogenase on the mechanism of H2 production: A quantum mechanics/molecular mechanics study

International Journal of Hydrogen Energy

Volumn 35, Issue 24, 2010, Pages 13179-13185

  Trohalaki, Steven ^a,b   Pachter, Ruth ^a  

^a AIR FORCE RESEARCH LABORATORY   (United States)

^b GENERAL DYNAMICS INFORMATION TECHNOLOGY   (United States)

Author keywords

All iron hydrogenase; Dimethyletherdithiolate; Hydrogen production; Hydrogenase mechanism; QM MM

Indexed keywords

ACTIVE SITE; CATALYTIC CYCLES; CLOSTRIDIUM PASTEURIANUM; CO LIGANDS; DESULFOVIBRIO DESULFURICANS; DIMETHYL ETHERS; DIMETHYLAMINES; DIMETHYLETHERDITHIOLATE; DITHIOLATES; EXPERIMENTAL VERIFICATION; FE ATOMS; H-CLUSTER; HYDROGENASES; METALLOENZYMES; NATURALLY OCCURRING; QM/MM; QM/MM METHOD; TERMINAL POSITION;

ACTIVATION ENERGY; CLOSTRIDIUM; DENSITY FUNCTIONAL THEORY; GAS PRODUCERS; IRON ALLOYS; LIGANDS; X RAY CRYSTALLOGRAPHY;

HYDROGEN PRODUCTION;

EID: 78049475959     PISSN: 03603199     EISSN: None     Source Type: Journal    
DOI: 10.1016/j.ijhydene.2010.08.095     Document Type: Article

References (21)

1. J.W. Peters, W.N. Lanzilotta, B.J. Lemon, and L.C. Seefeldt X-ray crystal structure of the Fe-only hydrogenase (CpI) from Clostridium pasteurianium to 18 angstrom resolution Science 282 1998 1853 1858
2. Y. Nicolet, B.J. Lemon, J.C. Fontecilla-Camps, and J.W. Peters A novel FeS cluster in Fe-only hydrogenases Trends Biochem Sci 25 2000 138 143
3. Y. Nicolet, C. Piras, P. Legrand, E.C. Hatchikian, and J.C. Fontecilla-Camps Desulfovibrio desulfuricans iron hydrogenase: the structure shows unusual coordination to an active site Fe binuclear center Structure 7 1999 13 23
4. A. Volbeda, and J.C. Fontecilla-Camps The active site and catalytic mechanism of NiFe hydrogenases Dalton Trans 2003 4030 4038
5. Y. Nicolet, A.L. De Lacey, X. Vernede, V.M. Fernandez, E.C. Hatchikian, and J.C. Fontecilla-Camps Crystallographic and FTIR spectroscopic evidence of changes in Fe coordination upon reduction of the active site of the Fe-only hydrogenase from Desulfovibrio desulfuricans J Am Chem Soc 123 2001 1596 1601
6. F.A. Armstrong Hydrogenases: active site puzzles and progress Curr Opin Struct Biol 8 2004 133 140
7. 10-Methylenetetrahydromethanopterin dehydrogenase from Methanobacterium thermoautotrophicum has hydrogenase activity FEBS Lett 261 1990 112 116
8. E. Lyon, S. Shima, G. Buurman, S. Chowdhuri, A. Batschauer, and K. Steinbach UV-A/blue-light inactivation of the metal-free hydrogenase (Hmd) from methanogenic archaea. The enzyme contains functional iron after all Eur J Biochem 271 2004 195 204
9. Y. Nicolet, C. Cavazza, and J.C. Fontecilla-Camps Fe-only hydrogenases: structure, function and evolution J Inorg Biochem 91 2002 1 8
10. 14N HYSCORE investigation of the H-cluster of [FeFe] hydrogenase: evidence for a nitrogen in the dithiol bridge Phys Chem Chem Phys 11 2009 6592 6599
11. A.S. Pandey, T.V. Harris, L.J. Giles, J.W. Peters, and R.K. Szilagyi Dithiomethylether as a ligand in the hydrogenase H-cluster J Am Chem Soc 130 2008 11106 11113
12. U. Ryde, C. Greco, and L.D. Gioia Quantum refinement of [Fe-Fe] hydrogenase indicates a dithiomethylamine ligand J Am Chem Soc 132 2010 4512 4513
13. S. Trohalaki, and R. Pachter Mechanism of hydrogen production in [Fe-Fe]-hydrogenase: a QM/MM study Int J Hydrogen Energy 35 2010 5318 5331
14. P.E.M. Siegbahn, J.W. Tye, and M. Hall Computational Studies of [NiFe] and [FeFe] hydrogenases Chem Rev 107 2007 4414 4435
15. C. Greco, M. Bruschi, L.D. Gioia, and U. Ryde A QM/MM investigation of the activation and catalytic mechanism of Fe-only hydrogenases Inorg Chem 46 2007 5911 5921
16. Z.-P. Liu, and P. Hu A density functional theory study on the active center of Fe-only hydrogenase: characterization and electronic structure of the redox states J Am Chem Soc 124 2002 5175 5182
17. H.-J. Fan, and M.B. Hall A capable bridging ligand for Fe-only hydrogenase: density functional calculations of a low-energy route for heterolytic cleavage and formation of dihydrogen J Am Chem Soc 123 2001 3828 3829
18. S. Trohalaki, and R. Pachter Mechanism of hydrogen production in [Fe-Fe]-hydrogenase: a density functional theory study Energy & Fuels 21 2007 2278 2286
19. Z. Cao, and M.B. Hall Modeling the active sites in metalloenzymes. 3. Density functional calculations on models for [Fe]-hydrogenase: structures and vibrational frequencies of the observed redox forms and the reaction mechanism at the Diiron Active Center J Am Chem Soc 123 2001 3734 3742
20. Y. Monte, P. Amara, A. Volbeda, X. Vernede, C.E. Hatchikian, and M.J. Field Gas access to the active site of Ni-Fe hydrogenases probed by X-ray crystallography and molecular dynamics Nat Struct Biol 4 1997 523 526
21. H subcluster environment on the properties of key intermediates in the catalytic cycle of [FeFe] hydrogenases: hints for the rational design of synthetic catalysts Angew Chem Int Edition 48 2009 3503 3506