Spectroscopic characterization of the Leu513His variant of fungal laccase: Effect of increased axial ligand interaction on the geometric and electronic structure of the type 1 Cu site

Inorganic Chemistry

Volumn 42, Issue 13, 2003, Pages 4006-4017

  Palmer, Amy E ^a   Szilagyi, Robert K ^a   Cherry, Joel R ^b   Jones, Aubrey ^b   Xu, Feng ^b   Solomon, Edward I ^a  

^a STANFORD UNIVERSITY   (United States)

^b Novozymes Biotech Inc   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

COPPER; FUNGAL ENZYME; LACCASE; NITRITE REDUCTASE;

ARTICLE; CHEMICAL INTERACTION; CIRCULAR DICHROISM; COVALENT BOND; DENSITY; DENSITY FUNCTION CALCULATION; ELECTRON SPIN RESONANCE; ENZYME ACTIVE SITE; ENZYME ANALYSIS; FUNGUS; GEOMETRY; LIGAND BINDING; MYCELIOPHTHORA THERMOPHILA; OPTICAL ROTATION; SPECTROSCOPY; STEREOCHEMISTRY;

AMINO ACID SUBSTITUTION; CIRCULAR DICHROISM; COLD; COLOR; COPPER; DNA; ELECTRON SPIN RESONANCE SPECTROSCOPY; FUNGI; HISTIDINE; HYDROGEN-ION CONCENTRATION; LACCASE; LEUCINE; LIGANDS; MODELS, MOLECULAR; MOLECULAR CONFORMATION; MUTATION; SUBSTRATE SPECIFICITY;

EID: 0037563854     PISSN: 00201669     EISSN: None     Source Type: Journal    
DOI: 10.1021/ic026099n     Document Type: Article

References (46)

1. Solomon, E. I.; Sundaram, U. M.; Machonkin, T. E. Chem. Rev. 1996, 96, 2563-2605.
2. Solomon, E. I.; Chen, P.; Lee, S. K.; Metz, M.; Palmer, A. E. Angew. Chem. Int. Ed. 2001, 40, 4570-4590.
3. Messerschmidt, A.; Ladenstein, R.; Huber, R.; Bolognesi, M.; Avigliano, L.; Petruzzelli, R.; Rossi, A.; Finazzi-Agró, A. J. Mol. Biol. 1992, 224, 179-205.
4. Palmer, A. E.; Randall. D. W.; Xu, F.; Solomon, E. I. J. Am. Chem. Soc. 1999, 121, 7138-7149.
5. Iwasaki, H.; Noji, S.; Shidara, S. J. Biochem. 1975, 78, 355-361.
6. Liu, M.-Y.; Liu, M.-C.; Payne, W. J.; LeGall, J. J. Bacteriol. 1986, 166, 604-608.
7. Aikazyan, V. T.; Nalbandyan, R. M. FEBS Lett. 1975, 55, 272-274.
8. Sakurai, T.; Okamoto, H.; Kawahara, K.; Nakahara, A. FEBS Lett. 1982, 147, 220-224.
9. Kroes, S. J.; Hoitink, C. W. G.; Andrew, C. R.; Ai, J.; Sanders-Loehr, J.; Messerschmidt, A.; Hagen, W. R.; Canters, G. W. Eur. J. Biochem. 1996, 240, 342-351.
10. LaCroix, L. B.; Shadle, S. E.; Wang, Y.; Averill, B. A.; Hedman, B.; Hodgson, K. O.; Solomon, E. I. J. Am. Chem. Soc. 1996, 118, 7755-7768.
11. LaCroix, L. B.; Randall, D. W.; Nersissian, A. M.; Hoitink, C. W. G.; Canters, G. W.; Valentine, J. S.; Solomon, E. I. J. Am. Chem. Soc. 1998, 120, 9621-9631.
12. Messerschmidt, A.; Prade, L.; Kroes, S. J.; Sanders-Loehr, J.; Huber, R.; Canters, G. W. Proc. Natl. Acad. Sci. U.S.A. 1998, 95, 3443-3448.
13. van Gastel, M.; Canters, G. W.; Krupka, H.; Messerschmidt, A.; de Waal, E. C.; Warmerdam, G. C. M.; Groenen, E. J. J. J. Am. Chem. Soc. 2000, 122, 2322-2328.
14. Xu, F.; Berka, R. M.; Wahleithner, J. A.; Nelson, B. A.; Shuster, J. R.; Brown, S. H.; Palmer, A. E.; Solomon, E. I. Biochem. J. 1998, 334, 63-70.
15. Berka, R. M.; Schneider, P.; Golightly, E. J.; Brown, S. H.; Madden, M. S.; Brown, K. M.; Halkier, T.; Mondorf. K.; Xu, F. Appl. Environ. Microbiol. 1997, 63, 3151-3157.
16. Xu, F. Biochemistry 1996, 35, 7608-7614.
17. Felsenfeld, G. Arch. Biochem. Biophys. 1960, 87, 247-251.
18. Hanna, P. M.; Tamilarasan, R.; McMillin, D. R. Biochem. J. 1988, 256, 1001-1004.
19. Carithers, R. P.; Palmer, G. J. Biol. Chem. 1981, 256, 7967-7976.
20. Lozos, G. P.; Hoffman, B. M.; Franz, C. G. QCPE Bull.: QCPE program number QCMP155 1974, 11.
21. Peak-Fit version 4.06; SPSS, Inc., AISN Software, Inc., 1995.
22. Baerends, E. J. E.; Ellis, D. E.; Ros, P. D. Chem. Phys. 1973, 2, 41-51.
23. Versluis, L. Z.; Ziegler, T. J. Chem. Phys. 1988, 88, 322-328.
24. teVelde, G.; Baerends, E. J. J. Comput. Phys. 1992, 99, 84-98.
25. Guerra, C. F.; Snijders, J. G.; teVelde, G.; Baerends, E. J. Theor. Chem. Acc. 1998, 99, 391-403.
26. Becke, A. D. Phys. Rev. A: At., Mol., Opt. Phys. 1988, 38.
27. Perdew, J. P. Phys. Rev. B: Condens. Matter Mater. Phys. 1986, 33.
28. Vosko, S. H.; Wilk, L.; Nusair, M. Can. J. Phys. 1980, 58, 8.
29. Amsterdam Density Functional, 1st ed.; Scientific Computing and Modelling NV: Amsterdam, The Netherlands, 2000.
30. Ryde, U.; Olsson, M. H. M.; Pierloot, K. In Processes and Properties of Biological Systems; Eriksson, L., Ed.; Elsevier: Amsterdam, 2001; Vol. 9, pp 1-55.
31. Szilagyi, R. K.; Metz, M.; Solomon, E. I. J. Phys. Chem. B 2002. 106, 2994-3007.
32. Guss, J. M.; Bartunik, H. D.; Freeman, H. C. Acta Crystallogr. 1992, B48, 790-811.
33. The equatorial Cu-N, Cu-S and axial Cu-N distances vary from 2.01 to 2.20 Å, 2.16-2.28 Å. and 2.06-2.25 Å, respectively.
34. Shimizu, A.; Sasaki, T.; Kwon, J. H.; Odaka, A.; Satoh, T.; Sakurai, N.; Sakurai, T.; Yamaguchi, S.; Samejima, T. J. Biochem. (Tokyo) 1999, 125.
35. Xu, F.; Shin, W.; Brown, S. H.; Wahleithner, J. A.; Sundaram, U. M.; Solomon, E. I. Biochim. Biophys. Acta 1996, 1292, 303-311.
36. McGarvey, B. R. In Transition Metal Chemistry; Carlin, B. L., Ed., 1966; Vol. 3, pp 89-201.
37. 2MtL) was calculated to be 9.6%.
38. Piepho, S. B.; Schatz, P. N. Group Theory in Spectroscopy-With Applications to Magnetic Circular Dichroism; Wiley & Sons: New York, 1983.
39. Solomon, E. I.; Hanson, M. A. In Inorganic Electronic Structure and Spectroscopy; Solomon, E. I., Lever, A. P. B., Eds.; Wiley & Sons: New York, 1999; Vol. 2, pp 1-130.
40. It should be noted that attempts were made to obtain resonance Raman on MtLH (excitation λ = 413 and 468 nm). However, the total absorption was too low, and no peaks were observed above the noise.
41. Gewirth, A. A.; Solomon, E. I. J. Am. Chem. Soc. 1988, 110, 3811-3819.
42. There is no crystal structure available for MtL, but the crystal structure of Coprinus cinereus laccase does not show any Ser residues in the immediate vicinity of the T1 Cu.
43. The active-site structure labeled as HP2-SUB in ref 12 has the His π (MO74) at higher energy than that of the Cys σ (MO75), whereas this order is reversed in the other three structures (HP1-SUA, HP1SUB, HP2-SUA) in ref 12, as shown in Figure 4.
44. Basumallick, L.; Szilagyi, R. K.; Scholes, C. P.; Solomon, E. I. In preparation.
45. Marcus, R. A.; Sutin, N. Biochim. Biophys. Acta 1985, 811, 265.
46. Machonkin, T. E.; Quintanar, L.; Palmer, A. E.; Hassett, R.; Severance, S.; Kosman, D. J.; Solomon, E. I. J. Am. Chem. Soc. 2001, 123, 55075517.