Abstract:
We present the results of combined molecular dynamics and full-quantum calculations aimed at elucidating the role of residue Thr122 of the enzyme methylamine dehydrogenase. Calculations were performed on the native structure and the T122A mutant. We found that the presence of Thr122 has a deleterious effect on the proton transfer step that is proposed to determine the rate of the reaction. Besides, at the PM3 level, the substitution of Thr122 by Ala does not significantly modify the preference of the proton by atom OD2 of Asp76. Transmission coefficients obtained form MP2/6-31G(d,p)//PBE/DZP minimum energy paths show that proton tunneling is significant. © 2008 Elsevier B.V. All rights reserved.
Registro:
Documento: |
Artículo
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Título: | The role of residue Thr122 of methylamine dehydrogenase on the proton transfer from the iminoquinone intermediate to residue Asp76 |
Autor: | Pierdominici-Sottile, G.; Martí, M.A.; Palma, J. |
Filiación: | Centro de Estudios e Investigaciones, Universidad Nacional de Quilmes, Sáenz Peña 352, B1876BXD Bernal, Argentina Departamento de Química Inorgánica, Analítica y Química-Física, INQUIMAE, CONICET, Pabellón 2, C1428EHA Buenos Aires, Argentina
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Palabras clave: | Amines; Molecular dynamics; Proton transfer; Quantum computers; Reaction rates; Substitution reactions; Enzyme methylamine dehydrogenase; Proton tunneling; Transmission coefficients; Enzyme kinetics |
Año: | 2008
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Volumen: | 456
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Número: | 4-6
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Página de inicio: | 243
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Página de fin: | 246
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DOI: |
http://dx.doi.org/10.1016/j.cplett.2008.03.023 |
Título revista: | Chemical Physics Letters
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Título revista abreviado: | Chem. Phys. Lett.
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ISSN: | 00092614
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CODEN: | CHPLB
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Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00092614_v456_n4-6_p243_PierdominiciSottile |
Referencias:
- Brooks, H.B., Jones, L.H., Davidson, V.L., (1993) Biochemistry, 32, p. 2725
- Basran, J., Sutcliffe, M.J., Scrutton, N.S., (1999) Biochemistry, 38, p. 3218
- Tresadern, G., Mcnamara, J.P., Mohr, M., Wang, H., Burton, N.A., Hillier, I.H., (2002) Chem. Phys. Lett., 358, p. 489
- Alhambra, C., Sanchez, M.L., Corchado, J.C., Gao, J., Truhlar, D.G., (2002) Chem. Phys. Lett., 355, p. 388
- Tresadern, G., Wang, H., Faulder, P.F., Burton, N.A., Hillier, I.H., (2003) Mol. Phys., 101, p. 2775
- Mincer, J.S., Schwartz, S.D., (2004) J. Chem. Phys., 120, p. 7755
- Siebrand, W., Smedarchina, Z., (2004) J. Phys. Chem. B, 108, p. 4185
- Pierdominici-Sottile, G., Echave, J., Palma, J., (2005) Int. J. Quantum Chem., 105, p. 937
- Pierdominici-Sottile, G., Echave, J., Palma, J., (2006) J. Phys. Chem. B, 110, p. 11592
- Nuńez, S., Tresadern, G., Hillier, I.H., Burton, N.A., (2006) Philos. Trans. R. Soc. London Ser. B, 361, p. 1387
- Ranaghan, K.E., Masgrau, L., Scrutton, N.S., Sutcliffe, M.J., Mulholland, A.J., (2007) Chem. Phys. Chem., 8, p. 1816
- Sun, D.P., Jones, L.H., Mathews, F.S., Davidson, V.L., (2001) Protein Eng., 14, p. 675
- Chen, L.Y., Doi, N., Durley, R.C.E., Chistoserdov, A.Y., Lidstrom, M.E., Davidson, V.L., Mathews, F.S., (1998) J. Mol. Biol., 276, p. 131
- Davidson, V.L., Zhu, Z.Y., (2000) J. Mol. Catal. B-Enzym., 8, p. 69
- Jones, L.H., Pearson, A.R., Tang, Y., Wilmot, C.M., Davidson, V.L., (2005) J. Biol. Chem., 280, p. 17392
- Case, D.A., (2002) Amber7, , University of California, San Fransisco
- M.J. Frisch et al., Gaussian Inc., Pittsburg, PA, 1998; Soler, J.M., Artacho, E., Gale, J.D., García, A., Junquera, J., Ordejón, P., Sánchez-Portal, D., (2002) J. Phys.: Condens. Matter, 14, p. 2745
- Wang, H.B., Sun, X., Miller, W.H., (1998) J. Chem. Phys., 108, p. 9726
- Wahnstrom, G., Carmeli, B., Metiu, H., (1988) J. Chem. Phys., 88, p. 2478
- Guallar, V., Harris, D.L., Batista, V.S., Miller, W.H., (2002) J. Am. Chem. Soc., 124, p. 1430
- Ahmed, Z., (1993) Phys. Rev. A, 47, p. 4761
Citas:
---------- APA ----------
Pierdominici-Sottile, G., Martí, M.A. & Palma, J.
(2008)
. The role of residue Thr122 of methylamine dehydrogenase on the proton transfer from the iminoquinone intermediate to residue Asp76. Chemical Physics Letters, 456(4-6), 243-246.
http://dx.doi.org/10.1016/j.cplett.2008.03.023---------- CHICAGO ----------
Pierdominici-Sottile, G., Martí, M.A., Palma, J.
"The role of residue Thr122 of methylamine dehydrogenase on the proton transfer from the iminoquinone intermediate to residue Asp76"
. Chemical Physics Letters 456, no. 4-6
(2008) : 243-246.
http://dx.doi.org/10.1016/j.cplett.2008.03.023---------- MLA ----------
Pierdominici-Sottile, G., Martí, M.A., Palma, J.
"The role of residue Thr122 of methylamine dehydrogenase on the proton transfer from the iminoquinone intermediate to residue Asp76"
. Chemical Physics Letters, vol. 456, no. 4-6, 2008, pp. 243-246.
http://dx.doi.org/10.1016/j.cplett.2008.03.023---------- VANCOUVER ----------
Pierdominici-Sottile, G., Martí, M.A., Palma, J. The role of residue Thr122 of methylamine dehydrogenase on the proton transfer from the iminoquinone intermediate to residue Asp76. Chem. Phys. Lett. 2008;456(4-6):243-246.
http://dx.doi.org/10.1016/j.cplett.2008.03.023