Comparison between the Geometric and Electronic Structures and Reactivities of {FeNO}7 and {FeO2}8 Complexes: A Density Functional Theory Study

Journal of the American Chemical Society

Volumn 126, Issue 2, 2004, Pages 505-515

  Schenk, Gerhard ^a   Pau, Monita Y M ^a   Solomon, Edward I ^a  

^a STANFORD UNIVERSITY   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

CHEMICAL BONDS; ENZYMES; MATHEMATICAL MODELS; PROBABILITY DENSITY FUNCTION; SPECTROSCOPIC ANALYSIS;

BONDING INTERACTIONS;

ELECTRONIC STRUCTURE;

FERRIC ION; FERROMAGNETIC MATERIAL; IRON DERIVATIVE; IRON OXIDE; NITROGEN OXIDE; OXYGEN;

ARTICLE; CALCULATION; CHEMICAL BOND; COMPLEX FORMATION; DENSITY FUNCTIONAL THEORY; ELECTRONICS; ENERGY TRANSFER; GEOMETRY; HYPOTHESIS; METHODOLOGY; REACTION ANALYSIS; SPECTROSCOPY;

FERRIC COMPOUNDS; FERROUS COMPOUNDS; MODELS, CHEMICAL; MODELS, MOLECULAR; NITRIC OXIDE; OXIDATION-REDUCTION; OXYGEN; THERMODYNAMICS;

EID: 0345825809     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja036715u     Document Type: Article

References (69)

1. Solomon, E. I.; Brunold, T. C.; Davis, M. I.; Kemsley, J. N.; Lee, S. K. ; Lehnert, N.; Neese, F.; Skulan, A. J.; Yang, Y.-S.; Zhou, J. Chem. Rev. 2000, 100, 235-349.
2. Arciero, D. M.; Orville, A. M.; Lipscomb, J. D. J. Biol. Chem. 1985, 260, 14035-14044.
3. Chen, V. J.; Orville, A. M.; Harpel, M. R.; Frolik, C. A.; Surerus, K. K.; Munck, E.; Lipscomb, J. D. J. Biol. Chem. 1989, 264, 21677-21681.
4. Pohl, K.; Wieghardt, K.; Nuber, B.; Weiss, J. J. Chem. Soc., Dalton Trans. 1987, 1, 187-192.
5. Brown, C. A.; Pavlosky, M. A.; Westre, T. E.; Zhang, Y.; Hedman, B.; Hodgson, K. O.; Solomon, E. I. J. Am. Chem. Soc. 1995, 117, 715-732.
6. Ray, M.; Golombek, A. P.; Hendrich, M. P.; Yap, G. P. A.; Liable-Sands, L. M.; Rheingold, A. L.; Borovik, A. S. Inorg. Chem. 1999, 38, 3110-3115.
7. Enemark, J. H.; Feltham, R. D. Coord. Chem. Rev. 1974, 13, 339.
8. Rodriguez, J. H.; Xia, Y.-M.; Debrunner, P. G. J. Am. Chem. Soc. 1999, 121, 7846-7863.
9. Hauser, C.; Glaser, T.; Eckhard, B.; Weyhermüller, T.; Wieghardt, K. J. Am. Chem. Soc. 2000. 122, 4352-4365.
10. Hohenberg, P.; Kohn, W. Phys. Rev. 1964, 136, B864-B871.
11. Koch, W.; Holthausen, M. C. A Chemist's Guide to Density Functional Theory; Wiley-VCH: Weinheim, 2000.
12. Siegbahn, P. E. M.; Blomberg, M. R. A. Chem. Rev. 2000. 100, 421-437.
13. Eriksson, L. A. Theoretical Biochemistry: Processes and Properties of Biological systems; Elsevier: Amsterdam, 2001; Vol. 9.
14. Friesner, R. A.; Dunietz, B. D. Acc. Chem. Res. 2001, 34, 351-358.
15. Perdew, J. P. Phys. Rev. B: Condens. Matter 1986, 33, 8822-8824.
16. Becke, A. D. Phys. Rev. A: Gen. Phys. 1988, 38, 3098-3100.
17. Pople, J. A.; Head-Gordon, M.; Fox, D. J.; Raghavachari, K.; Curtiss, L. A. J. Chem. Phys. 1989, 90, 5622-5629.
18. Curtiss, L. A.; Jones, C.; Trucks, G. W.; Raghavachari, K.; Pople, J. A. J. Chem. Phys. 1990, 93, 2537-2545.
19. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Zakrzewski, V. G.; Montgomery, J. A. J.; Stratmann, R. E. ; Burant, J. C.; Dapprich, S.; Millam, J. M.; Daniels, A. D.; Kudin, K. N.; Strain, M. C.; Farkas, O.; Tomasi, J.; Barone, V.; Cossi, M.; Cammi, R.; Mennucci, B.; Pomelli, C.; Adamo, C.; Clifford, S.; Ochterski, J.; Petersson, G. A.; Ayala, P. Y.; Cui, Q.; Morokuma, K.; Malick, D. K.; Rabuck, A. D.; Raghavachari, K.; Foresman, J. B.; Cioslowski, J.; Ortiz, J. V.; Stefanov, B. B.; Liu, G.; Liashenko, A.; Piskorz, P.; Komaromi, I.; Gomperts, R.; Martin, R. L.; Fox, D. J.; Keith, T.; Al-Laham, M. A.; Peng, C. Y.; Nanayakkara, A.; Gonzalez, C.; Challacombe, M.; Gill, P. M. W.; Johnson, B.; Chen, W.; Wong, M. W.; Andres, J. L.; Head-Gordon, M.; Replogle, E. S.; Pople, J. A. Gaussian 98, revision A.1; Gaussian, Inc.; Pittsburgh, PA, 1998.
20. Kohn, W.; Sham, L. J. Phys. Rev. 1965, 140, A1133-A1138.
21. Slater, J. C. The Self-Consistent Field for Molecules and Solids. Quantum Theory; McGraw-Hill: New York, 1974: Vol. 4.
22. Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B: Condens. Matter 1988, 37, 785-789.
23. Miehlich, B.; Savin, A.; Stoll, H.; Preuss, H. Chem. Phys. Lett. 1989, 157, 200-206.
24. Perdew, J. P.; Zunger, A. Phys. Rev. B: Condens. Matter 1981, 23, 5048-5079.
25. Vosko, S. H.; Wilk, L.; Nusair, M. Can. J. Phys. 1980, 58, 1200-1211.
26. Becke, A. D. J. Chem. Phys. 1993, 98, 5648-5652.
27. Becke, A. D. J. Chem. Phys. 1993, 98, 1372-1377.
28. Schaftenaar, G.; Noordik, J. H. J. Comput.-Aided Mol. Des. 2000, 14, 123-134.
29. Pascual-Ahuir, J. L.; Silla, E.; Tomasi, J.; Bonaccorsi, R. J. Comput. Chem. 1987, 8, 778-787.
30. Floris, F.; Tomasi, J. J. Comput. Chem. 1989, 10, 616-627.
31. Cossi, M.; Barone, V.; Cammi, R.; Tomasi, J. Chem. Phys. Lett. 1996, 255, 327-335.
32. Barone, V.; Cossi, M.; Tomasi, J. J. Comput. Chem. 1998, 19, 404-417.
33. Casida, M. E. In Recent Advances in Density Functional Theory; Chong, D. P., Ed.; World Scientific: Singapore, 1995; Vol. 1, p 155.
34. Gross, E. U. K. In Density Functional Theory; Nalewajski, R. F., Ed.; Springer: Heidelberg, 1996.
35. Stratmann, R. E.; Scuseria, G. E.; Frisch, M. J. J. Chem. Phys. 1998, 109, 8218-8224.
36. Ziegler, T.; Rauk, A.; Baerends, E. J. Theor. Chim. Acta 1977, 43, 261-271.
37. Baerends, E. J.; Ellis, D. E.; Ros, P. Chem. Phys. 1973, 2, 41-51.
38. Versluis, L.; Ziegler, T. J. Chem. Phys. 1988, 88, 322-328.
39. Te Velde, G.; Baerends, E. J. J. Comput. Phys. 1992, 99, 84-98.
40. Mulliken, R. S. J. Chem. Phys. 1955, 23, 1833-1840.
41. Reed, A. E.; Curtiss, L. A.; Weinhold, F. Chem. Rev. 1988, 88, 899-926.
42. Gorelsky, S. I. AOMix program, revision 5.2.
43. Gorelsky, S. I.; Lever, A. B. P. J. Orgamet. Chem. 2001, 635, 187-196.
44. Hay, P. J.; Wadt, W. R. J. Chem. Phys. 1985, 82, 270-283.
45. Wadt, W. R.; Hay, P. J. J. Chem. Phys. 1985, 82, 284-298.
46. Hay, P. J.; Wadt, W. R. J. Chem. Phys. 1985, 82, 299-310.
47. McGrath, M. P.; Radom, L. J. Chem. Phys. 1991, 94, 511-516.
48. Curtiss, L. A.; McGrath, M. P.; Blaudeau, J.-P.; Davis, N. E.; Binning, R. C. J.; Radom, L. J. Chem. Phys. 1995, 103, 6104-6113.
49. Schaefer, A.; Huber, C.; Ahlrichs, R. J. Chem. Phys. 1994, 100, 5829-5835.
50. Rassolov, V. A.; Pople, J. A.; Ratner, M. A.; Windus, T. L. J. Chem. Phys. 1998, 109, 1223-1229.
51. Hehre, W. J.; Random, L.; Schleyer, P. v. R.; Pople, J. A. Ab Initio Molecular Orbital Theory; Wiley: New York, 1986.
52. In Tables of Interatomic Distances and Configuration in Molecules and Ions; Sutton, L. E., Ed.; Chemical Society: London, 1958.
53. Tronc, M.; Huetz, A.; Landau, M.; Pichou, F.; Reinhardt, J. J. Phys. B 1975, 8, 1160-1169.
54. Similarly, poor agreement with experimental transitions is observed in TDDFT calculations for the FeNO model optimized with B3LYP and 6-311G*/6-31G* as shown in Figure S1.
55. eff ≈ 25.60 (Table S1).
56. eff = 25.60 (Table S1) with two different functionals and two different structures shows that spin densities have a stronger dependence on geometry than the choice of functional (Table S2). This observation supports the choice of BP86 + 10% HFX, which gives the best geometric agreement to the crystal structure.
57. tot = 3 states, respectively.
58. 8 models optimized with BP86 + 10% HFX and the basis sets LanL2DZ and 6-311G*/6-31G*, respectively (Table S3).
59. 8 are more pronounced than in the models optimized with the mixed basis set (Table 6).
60. 8 at ≥ 140° is due to a change in the ground-state electronic description.
61. Davis, M. I.; Wasinger, E. C.; Decker, A.; Pau, M. Y. M.; Vaillancourt, F. H.; Bolin, J. T.; Eltis, L. D.; Hedman, B.; Hodgson, K. O.; Solomon, E. I. J. Am. Chem. Soc. 2003, 125, 11214-11227.
62. Bartberger, M. D.; Liu, W.; Ford, E.; Miranda, K. M.; Switzer, C.; Fukuto, J. M.; Farmer, P. J.; Wink, D. A.; Houk, K. N. Proc. Natl. Acad. Sci. U.S.A. 2002, 99, 10959-10963.
63. Wood, P. M. Trends Biochem. Sci. 1987, 12, 250-251.
64. Sawyer, D. T. Oxygen Chemistry; Oxford University Press: New York, 1991.
65. op*).
66. Rabalais, J. W. Principles of Ultraviolet Photoelectron Spectroscopy; John Wiley & Sons: New York, 1977.
67. 2 models optimized with the mixed basis set 6-311G* /6-31G* were compared in a similar manner and results analogous to the ones described here were obtained. For completion, the relevant MOs and evergy levels are included in the Supporting Information (Figures S6-S12 and Table S4).
68. Vaillancourt, F. H.; Labbe, G.; Drouin, N. M.; Fortin, P. D.; Eltis, L. D. J. Biol. Chem. 2002, 277, 2019-2027.
69. 2-.61