Artículo
Khoa Ly, H.; Wisitruangsakul, N.; Sezer, M.; Feng, J.-J.; Kranich, A.; Weidinger, I.M.; Zebger, I.; Murgida, D.H.; Hildebrandt, P. "Electric-field effects on the interfacial electron transfer and protein dynamics of cytochrome c" (2011) Journal of Electroanalytical Chemistry. 660(2):367-376
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Abstract:
Time-resolved surface enhanced resonance Raman and surface enhanced infrared absorption spectroscopy have been employed to study the interfacial redox process of cytochrome c (Cyt-c) immobilised on various metal electrodes coated with self-assembled monolayers (SAMs) of carboxyl-terminated mercaptanes. The experiments, carried out with Ag, Au and layered Au-SAM-Ag electrodes, afford apparent heterogeneous electron transfer constants (krelax) that reflect the interplay between electron tunnelling, redox-linked protein structural changes, protein re-orientation, and hydrogen bond re-arrangements in the protein and in the protein/SAM interface. It is shown that the individual processes are affected by the interfacial electric field strength that increases with decreasing thickness of the SAM and increasing difference between the actual potential and the potential of zero-charge. At thick SAMs of mercaptanes including 15 methylene groups, electron tunnelling (kET) is the rate-limiting step. Pronounced differences for kET and its overpotential-dependence are observed for the three metal electrodes and can be attributed to the different electric-field effects on the free-energy term controlling the tunnelling rate. With decreasing SAM thickness, electron tunnelling increases whereas protein dynamics is slowed down such that for SAMs including less than 10 methylene groups, protein re-orientation becomes rate-limiting, as reflected by the viscosity dependence of krelax. Upon decreasing the SAM thickness from 5 to 1 methylene group, an additional H/D kinetic isotope effect is detected indicating that at very high electric fields re-arrangements of the interfacial or intra-protein hydrogen bond networks limit the rate of the overall redox process. © 2010 Elsevier B.V. All rights reserved.
Registro:
| Documento: | Artículo |
| Título: | Electric-field effects on the interfacial electron transfer and protein dynamics of cytochrome c |
| Autor: | Khoa Ly, H.; Wisitruangsakul, N.; Sezer, M.; Feng, J.-J.; Kranich, A.; Weidinger, I.M.; Zebger, I.; Murgida, D.H.; Hildebrandt, P. |
| Filiación: | Technische Universität Berlin, Institut für Chemie, Straße des 17. Juni 135, D-10623 Berlin, Germany Iron and Steel Institute of Thailand, Bureau of Industrial Sectors Development Building, Trimitr Soi., Pharam 4 Rd. Phakhanong, Klongtoey Bangkok 10110, Thailand School of Chemistry and Environmental Science, Henan Normal University, Xinxiang, Henan 453007, China Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE-CONICET, Ciudad Universitaria, Pab. 2, Piso. 1, C1428EHA-Buenos Aires, Argentina |
| Palabras clave: | Cytochrome c; Electric field; Electron transfer; Surface enhanced infrared spectroscopy; Surface enhanced Raman spectroscopy; Dynamics; Electric fields; Electrodes; Electron transitions; Electron tunneling; Gold; Hydrogen bonds; Infrared spectroscopy; Isotopes; Proteins; Raman spectroscopy; Self assembled monolayers; Cytochrome C; Electric field strength; Electron transfer; Heterogeneous electron transfer; High electric fields; Hydrogen bond networks; Interfacial electron transfer; Kinetic isotope effects; Metal electrodes; Methylene groups; Protein dynamics; Rate limiting; Rate-limiting steps; Re-orientation; Redox process; Sams; Structural change; Surface enhanced infrared absorption spectroscopy; Surface enhanced infrared spectroscopy; Surface enhanced Raman spectroscopy; Surface enhanced resonance; Time-resolved; Zero charge; Electric field effects |
| Año: | 2011 |
| Volumen: | 660 |
| Número: | 2 |
| Página de inicio: | 367 |
| Página de fin: | 376 |
| DOI: | http://dx.doi.org/10.1016/j.jelechem.2010.12.020 |
| Título revista: | Journal of Electroanalytical Chemistry |
| Título revista abreviado: | J Electroanal Chem |
| ISSN: | 15726657 |
| CODEN: | JECHE |
| Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_15726657_v660_n2_p367_KhoaLy |
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Citas:
---------- APA ----------
Khoa Ly, H., Wisitruangsakul, N., Sezer, M., Feng, J.-J., Kranich, A., Weidinger, I.M., Zebger, I.,..., Hildebrandt, P. (2011) . Electric-field effects on the interfacial electron transfer and protein dynamics of cytochrome c. Journal of Electroanalytical Chemistry, 660(2), 367-376.http://dx.doi.org/10.1016/j.jelechem.2010.12.020
---------- CHICAGO ----------
Khoa Ly, H., Wisitruangsakul, N., Sezer, M., Feng, J.-J., Kranich, A., Weidinger, I.M., et al. "Electric-field effects on the interfacial electron transfer and protein dynamics of cytochrome c" . Journal of Electroanalytical Chemistry 660, no. 2 (2011) : 367-376.http://dx.doi.org/10.1016/j.jelechem.2010.12.020
---------- MLA ----------
Khoa Ly, H., Wisitruangsakul, N., Sezer, M., Feng, J.-J., Kranich, A., Weidinger, I.M., et al. "Electric-field effects on the interfacial electron transfer and protein dynamics of cytochrome c" . Journal of Electroanalytical Chemistry, vol. 660, no. 2, 2011, pp. 367-376.http://dx.doi.org/10.1016/j.jelechem.2010.12.020
---------- VANCOUVER ----------
Khoa Ly, H., Wisitruangsakul, N., Sezer, M., Feng, J.-J., Kranich, A., Weidinger, I.M., et al. Electric-field effects on the interfacial electron transfer and protein dynamics of cytochrome c. J Electroanal Chem. 2011;660(2):367-376.http://dx.doi.org/10.1016/j.jelechem.2010.12.020
