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Abstract:

The spectral features of Co(II)-substituted metallo-β-lactamases were analyzed. Nuclear magnetic resonance (NMR) evidence is provided that shows no magnetic coupling between the two metal ions in Co(II),Co(II)-βLII (β-lactamase II from Bacillus cereus), suggesting that no bridging ligand connects them. Ultraviolet-visible (UV-vis) data are rationalized on the basis of semiempirical quantum chemical calculations of the intermediate neglect of differential overlap type (ZINDO/S). The binuclear active sites of the enzymes from B. cereus (βLII) and B. fragilis (CcrA) were modeled from the protein data bank (PDB) coordinates, and calculations were performed at the multireference configuration interaction level. The active site geometries of these enzymes were examined using the experimental electronic spectra as a guide. The model which best fits to the spectroscopic data lacks a bridging solvent molecule, in agreement with the NMR data. The model could also reproduce spectral changes seen in the mixed Zn(II),Co(II) adduct. The bands in the visible range are associated with ligand field transitions at the high-affinity site, whereas the UV-calculated features originate in ligand-to-metal charge transfer to the open shell Co(II) in the low-affinity site. These results indirectly support the hypothesis that the Co(II),Co(II) derivative of CcrA is also unbridged, in contrast with the structure of the native zinc enzyme. These results indicate that the existence of a bridging ligand is not necessary for metallo-β-lactamase activity, and that the second zinc ion is not essential for lowering the pK a of the bound water. © 2002 Wiley Periodicals, Inc. Int. J. Quantum Chem.

Registro:

Documento: Artículo
Título:Is there a bridging ligand in metal-substituted zinc β-lactamases? A spectroscopic and theoretical answer
Autor:Estiú, G.L.; Rasia, R.M.; Cricco, J.A.; Vila, A.J.; Zerner, M.C.
Filiación:CEQUINOR, Departamento de Química, Universidad Nacional de la Plata, C.C. 962-1900 La Plata, Argentina
Departamento de Química Inorgánica, Analítica y Química Física, Universidad de Buenos Aires, Ciudad Universitaria, C1428EHA, Buenos Aires, Argentina
Area Biofísica, Facultad de Ciencias Bioquímicas y Farmacéuticas, Universidad Nacional de Rosario, Suipacha 531, 2000 Rosario, Argentina
University of Florida, Gainesville, FL 32611, United States
Palabras clave:Co(II); Electronic spectra; Metallo-β-lactamase; NMR; Theoretical calculation; Bridging ligands; Band structure; Charge transfer; Electronic structure; Enzymes; Nuclear magnetic resonance; Positive ions; Spectrum analysis; Ultraviolet spectroscopy; Zinc compounds; Quantum theory
Año:2002
Volumen:88
Número:1
Página de inicio:118
Página de fin:132
DOI: http://dx.doi.org/10.1002/qua.10098
Título revista:International Journal of Quantum Chemistry
Título revista abreviado:Int J Quantum Chem
ISSN:00207608
CODEN:IJQCB
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00207608_v88_n1_p118_Estiu

Referencias:

  • Frère, J.M., (1995) Mol Microbiol, 16, p. 385
  • Philippon, A., Dusart, J., Joris, B., Frère, J.M., (1998) Cell Mol Life Sci, 54, p. 341
  • Cricco, J.A., Orellano, E.G., Rasia, R.M., Ceccarelli, E.A., Vila, A.J., (1999) Coord Chem Rev, 190-192, p. 519
  • Rasmussen, B.A., Bush, K., (1997) Antimicrob Agents Chemother, 41, p. 223
  • Cricco, J.A., Vila, A.J., (1999) Curr Pharm Design, 5, p. 915
  • Wang, Z., Fast, W., Valentine, A.M., Benkovic, S.J., (1999) Curr Op Chem Biol, 3, p. 614
  • Sabath, L.B., Abraham, E.P., (1966) Biochem J, 98, pp. 11c
  • Cuchural G.J., Jr., Malamy, M.H., Tally, F.P., (1986) Antimicrob Agents Chemother, 30, p. 645
  • Davies, R.B., Abraham, E.P., (1974) Biochem J, 143, p. 129
  • Wang, Z., Benkovic, S.J., (1998) J Biol Chem, 273, p. 22402
  • Bounaga, S., Laws, A.P., Galleni, M., Page, M.I., (1998) Biochem J, 31, p. 703
  • Wang, Z., Fast, W., Benkovic, S.J., (1999) Biochemistry, 38, p. 10013
  • Orellano, E.G., Girardini, J.E., Cricco, J.A., Ceccarelli, E.A., Vila, A.J., (1998) Biochemistry, 37, p. 10173
  • Paul-Soto, R., Bauer, R., Frère, J.M., Galleni, M., Meyer-Klaucke, W., Nolting, H., Rossolini, G.M., Adolph, H.W., (1999) J Biol Chem, 274, p. 13242
  • Paul-Soto, R., Hernandez Valladares, M., Galleni, M., Bauer, R., Zeppezauer, M., Frère, J.M., Adolph, H.W., (1998) FEBS Lett, 438, p. 137
  • Felici, A., Amicosante, G., Oratore, A., Strom, R., Ledent, P., Joris, B., Fanuel, L., Frère, J.M., (1993) Biochem J, 291, p. 151
  • Fabiane, S.M., Sohi, M.K., Wan, T., Payne, D.J., Bateson, J.H., Mitchell, T., Sutton, B.J., (1998) Biochemistry, 37, p. 12404
  • Concha, N., Rasmussen, B.A., Bush, K., Herzberg, O., (1996) Structure, 4, p. 823
  • Concha, N.O., Janson, C.A., Rowling, P., Pearson, S., Cheerer, C.A., Clarke, B.P., Lewis, C., Abdel-Meguid, S.S., (2000) Biochemistry, 39, p. 4288
  • Ullah, J.H., Walsh, T.R., Taylor, I.A., Emery, D.C., Verma, C.S., Gamblin, S.J., Spencer, J.J., (1998) Mol Biol, 284, p. 125
  • Que L., Jr., (2000) Physical Methods in Bioinorganic Chemistry: Spectroscopy and Magnetism, , Universe Science Books: Sausalito
  • Bertini, I., Luchinat, C., (1985) Adv Inorg Biochem, 6, p. 71
  • Baldwin, G.S., Galdes, A., Hill, H.A.O., Waley, S.G., Abraham, E.P., (1980) J Inorg Biochem, 13, p. 189
  • Gilson, H.S.R., Krauss, M., (1999) J Am Chem Soc, 121, p. 6984
  • Roos, B.O., (1999) Acc Chem Res, 32, p. 137
  • Díaz, N., Suárez, D., Merz K.M., Jr., (2000) J Am Chem Soc, 122, p. 4197
  • Zerner, M.C., (2000) ZINDO Quantum Theory Project, , Universe of Florida, Gainesville, FL
  • Ridley, J., Zerner, M.C., (1973) Theor Chim Acta, 32, p. 111
  • Estiú, G.L., Zerner, M.C., (1994) J Phys Chem, 98, p. 4793
  • Estiú, G.L., Zerner, M.C., (1996) J Phys Chem, 100, p. 16874
  • Estiú, G.L., Zerner, M.C., (2000) J Phys Chem A, 104, p. 233
  • Estiú, G.L., Zerner, M.C., (1999) J Am Chem Soc, 121, p. 1893
  • Stavrev, K.K., Zerner, M.C., (1995) Chem Phys Lett, 233, p. 179
  • Cory, M.G., Hirose, H., Zerner, M.C., (1995) Inorg Chem, 34, p. 2969
  • Loew, G., Harris, D., (2000) Chem Rev, 100, p. 407
  • Culberson, J.C., Kanppe, P., Rosch, N., Zerner, M.C., (1987) Theor Chim Acta, 71, p. 21
  • Estiú, G.L., Rosch, N., Zerner, M.C., (1995) J Phys Chem, 99, p. 13819
  • Cory, M.G., Zerner, M.C., Hu, X., Shulten, K., (1998) J Phys Chem B, 102, p. 7640
  • Thompson, M., Zerner, M.C., (1991) J Am Chem Soc, 113, p. 8210
  • Harris, D., Loew, G., (1993) J Am Chem Soc, 115, p. 8775
  • Loew, G., Harris, D., Dupuis, M., (1997) J Mol Struct (THEOCHEM), p. 497
  • Stavrev, K.K., Zerner, M.C., (1997) Theor Chim Acc, 96, p. 141
  • Stavrev, K.K., Zerner, M.C., (1998) Int J Quantum Chem, 70, p. 1159
  • Inubushi, T., Becker, E.D., (1983) J Magn Reson, 51, p. 128
  • La Mar, G.N., De Ropp, J.S., (1993) Biological Magnetic Resonance, 12. , Berliner L.J.; Reuben J., Eds.; NMR of Paramagnetic Molecules; Plenum: New York
  • Martin, C.H., Zerner, M.C., (1999) Inorganic Electronic Structure and Spectroscopy, , Solomon, E. I.; Lever, A. B. P., Eds.; John Wiley: New York
  • Zerner, M.C., (1991) Reviews in Computational Chemistry, , Lipkowitz, K. D.; Boyd, D. B., Eds.; VCH: New York
  • Pople, J., Beveridge, D., Dobash, P.J., (1967) Chem Phys, 47, p. 2026
  • Pople, J., Santry, D., Segal, G., (1965) J Chem Phys, 43, p. 5129
  • DelBene, J., Jaffe, H.H., (1968) J Chem Phys, 48, p. 1807
  • DelBene, J., Jaffe, H.H., (1968) J Chem Phys, 48, p. 4050
  • Slater, J.C., (1960) Quantum Theory of Atomic Structure, , McGraw-Hill: New York
  • Pauncz, R., (1979) Spin Eigenfunctions, , Plenum: New York
  • Lever, A.B.P., (1984) Inorganic Electronic Spectroscopy, , Elsevier: Amsterdam
  • Bertini, I., Luchinat, C., (1996) NMR of Paramagnetic Substances, , Elsevier: Amsterdam
  • Bertini, I., Gerber, M., Lanini, G., Luchinat, C., Maret, W., Rawer, S., Zeppezauer, M., (1984) J Am Chem Soc, 106, p. 1826
  • Vila, A.J., (1994) FEBS Lett, 355, p. 15
  • Vila, A.J., Fernandez, C.O., (1996) J Am Chem Soc, 118, p. 7291
  • Vila, A.J., Ramirez, B.E., DiBilio, A.J., Mizoguchi, T.J., Richards, J.H., Gray, H.B., (1997) Inorg Chem, 36, p. 4567
  • Fernandez, C.O., Sannazzaro, A.I., Villa, A.J., (1997) Biochemistry, 36, p. 10566
  • Bertini, I., Turano, P., Vila, A.J., (1993) Chem Rev, 93, p. 2833
  • Solomon, E.I., (1995) Phys Rev, 99, p. 559
  • Banci, L., Bertini, I., Luchinat, C., Nuclear and electron relaxation (1991) The Magnetic Nucleus - Unpaired Electron Coupling in Solution, , VCH: Weinheim
  • Bertini, I., Lanini, G., Luchinat, C., (1983) Inorg Chim Acta, 80, p. 123
  • Banci, L., Bertini, I., Luchinat, C., Monnanni, R., Scozzafava, A., Salvato, B., (1986) Gazz Chim Ital, 116, p. 51
  • Voityuk, A.A., Albert, K., Romao, M.J., Huber, R., Rosch, N., (1998) Inorg Chem, 37, p. 176
  • Romao, M.J., Huber, R., Rosch, N., (1997) J Biol Inorg Chem, 2, p. 782
  • Voityuk, A.A., Albert, K., Kostmeier, S., Nasluzov, V.A., Neyman, K.M., Hof, P., Huber, R., Rosch, N., (1997) J Am Chem Soc, 119, p. 3159
  • Pierloot, K., DeKerpel, J.O.A., Ryde, U., Roos, B.O., (1997) J Am Chem Soc, 119, p. 218
  • Cory, M.G., Zerner, M.C., (1991) Chem Rev, 91, p. 813
  • Bachrach, S.M., (1994) Reviews in Computational Chemistry, , Lipkowitz, K. D.; Boyd, D. B., Eds.; VCH: New York
  • Lipscomb, W.N., Strater, N., (1996) Chem Rev, 96, p. 2375
  • Bertini, I., Luchinat, C., (1993) Bioinorganic Chemistry, , Bertini, I.; Gray, H. B.; Lippard, S. J.; Valentine, J. S., Eds.; Mary Miller University Books: Los Angeles
  • Strater, N., Lipscomb, W.N., Klabunde, T., Krebs, B., (1996) Angew Chem Int Ed Ingl, 35, p. 2024
  • Rasia, R.M., Vila, A.J., Biochemistry, , in press
  • Kaminskaia, N.V., Spingler, B., Lippard, S.J., (2000) J Am Chem Soc, 122, p. 6411
  • Kaminskaia, N.V., He, C., Lippard, S.J., (2000) Inorg Chem, 39, p. 3365
  • Bennett, B., Holz, R.C., (1997) J Am Chem Soc, 119, p. 1923
  • Carfi, A., Dueé, E., Paul-Soto, R., Galleni, M., Frère, J.M., Dideberg, O., (1998) Acta Crystallogr, D54, p. 47
  • Zhan, C.G., DeSouza, O.M., Rittenhouse, R., Ornstein, R.L., (1999) J Am Chem Soc, 121, p. 7279

Citas:

---------- APA ----------
Estiú, G.L., Rasia, R.M., Cricco, J.A., Vila, A.J. & Zerner, M.C. (2002) . Is there a bridging ligand in metal-substituted zinc β-lactamases? A spectroscopic and theoretical answer. International Journal of Quantum Chemistry, 88(1), 118-132.
http://dx.doi.org/10.1002/qua.10098
---------- CHICAGO ----------
Estiú, G.L., Rasia, R.M., Cricco, J.A., Vila, A.J., Zerner, M.C. "Is there a bridging ligand in metal-substituted zinc β-lactamases? A spectroscopic and theoretical answer" . International Journal of Quantum Chemistry 88, no. 1 (2002) : 118-132.
http://dx.doi.org/10.1002/qua.10098
---------- MLA ----------
Estiú, G.L., Rasia, R.M., Cricco, J.A., Vila, A.J., Zerner, M.C. "Is there a bridging ligand in metal-substituted zinc β-lactamases? A spectroscopic and theoretical answer" . International Journal of Quantum Chemistry, vol. 88, no. 1, 2002, pp. 118-132.
http://dx.doi.org/10.1002/qua.10098
---------- VANCOUVER ----------
Estiú, G.L., Rasia, R.M., Cricco, J.A., Vila, A.J., Zerner, M.C. Is there a bridging ligand in metal-substituted zinc β-lactamases? A spectroscopic and theoretical answer. Int J Quantum Chem. 2002;88(1):118-132.
http://dx.doi.org/10.1002/qua.10098