Abstract:
In this paper we present a combined experimental and theoretical study of the heterogeneous electron transfer reaction of cytochrome c electrostatically adsorbed on metal electrodes coated with monolayers of 6-mercaptohexanoic acid. Molecular dynamics simulations and pathways calculations show that adsorption of the protein leads to a broad distribution of orientations and, thus, to a correspondingly broad distribution of electron transfer rate constants due to the orientation-dependence of the electronic coupling parameter. The adsorbed protein exhibits significant mobility and, therefore, the measured reaction rate is predicted to be a convolution of protein dynamics and tunnelling probabilities for each orientation. This prediction is confirmed by time-resolved surface enhanced resonance Raman which allows for the direct monitoring of protein (re-)orientation and electron transfer of the immobilised cytochrome c. The results provide a consistent explanation for the non-exponential distance-independence of electron transfer rates usually observed for proteins immobilized on electrodes. © 2009 Elsevier Ltd. All rights reserved.
Registro:
Documento: |
Artículo
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Título: | Computer simulation and SERR detection of cytochrome c dynamics at SAM-coated electrodes |
Autor: | Paggi, D.A.; Martín, D.F.; Kranich, A.; Hildebrandt, P.; Martí, M.A.; Murgida, D.H. |
Filiación: | Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE-CONICET, Facultad de Ciencias Exactas y Naturales, Ciudad Universitaria, Pab. 2, piso 1, C1428EHA Buenos Aires, Argentina Institut für Chemie, Technische Universität Berlin, Str. des 17, Juni 135, Sekr. PC14, D-10623 Berlin, Germany
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Palabras clave: | Cytochrome c; Molecular dynamics; Protein electron transfer; Self-assembled monolayers; SERR; Coated electrodes; Cytochrome c; Direct monitoring; Electron transfer; Electron transfer rates; Electron-transfer rate constants; Electronic coupling; Heterogeneous electron transfer; Metal electrodes; Molecular dynamics simulations; Protein dynamics; SERR; Surface enhanced resonance; Theoretical study; Time-resolved; Tunnelling probability; Adsorption; Coated wire electrodes; Electrodes; Electron transitions; Molecular dynamics; Molecular orientation; Rate constants; Reaction kinetics; Self assembled monolayers; Dynamics |
Año: | 2009
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Volumen: | 54
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Número: | 22
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Página de inicio: | 4963
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Página de fin: | 4970
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DOI: |
http://dx.doi.org/10.1016/j.electacta.2009.02.050 |
Título revista: | Electrochimica Acta
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Título revista abreviado: | Electrochim Acta
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ISSN: | 00134686
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CODEN: | ELCAA
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Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00134686_v54_n22_p4963_Paggi |
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Citas:
---------- APA ----------
Paggi, D.A., Martín, D.F., Kranich, A., Hildebrandt, P., Martí, M.A. & Murgida, D.H.
(2009)
. Computer simulation and SERR detection of cytochrome c dynamics at SAM-coated electrodes. Electrochimica Acta, 54(22), 4963-4970.
http://dx.doi.org/10.1016/j.electacta.2009.02.050---------- CHICAGO ----------
Paggi, D.A., Martín, D.F., Kranich, A., Hildebrandt, P., Martí, M.A., Murgida, D.H.
"Computer simulation and SERR detection of cytochrome c dynamics at SAM-coated electrodes"
. Electrochimica Acta 54, no. 22
(2009) : 4963-4970.
http://dx.doi.org/10.1016/j.electacta.2009.02.050---------- MLA ----------
Paggi, D.A., Martín, D.F., Kranich, A., Hildebrandt, P., Martí, M.A., Murgida, D.H.
"Computer simulation and SERR detection of cytochrome c dynamics at SAM-coated electrodes"
. Electrochimica Acta, vol. 54, no. 22, 2009, pp. 4963-4970.
http://dx.doi.org/10.1016/j.electacta.2009.02.050---------- VANCOUVER ----------
Paggi, D.A., Martín, D.F., Kranich, A., Hildebrandt, P., Martí, M.A., Murgida, D.H. Computer simulation and SERR detection of cytochrome c dynamics at SAM-coated electrodes. Electrochim Acta. 2009;54(22):4963-4970.
http://dx.doi.org/10.1016/j.electacta.2009.02.050