Proton transfer impedance of electrodes modified with acid thiol monolayers

Analytical expressions describing the electrochemical impedance spectrum of a metallic electrode modified with an acid thiol monolayer, that undergoes a potential-induced proton transfer, have been derived from an electrostatic model of the interface. The frequency dispersion of the electrode impeda...

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Detalles Bibliográficos
Autores: Luque, Antonio M., Mulder, Willem H., Calvente Pacheco, Juan José, Andreu Fondacabe, Rafael Jesús
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2018
País:España
Institución:Universidad de Sevilla (US)
Repositorio:idUS. Depósito de Investigación de la Universidad de Sevilla
OAI Identifier:oai:idus.us.es:11441/154294
Acceso en línea:https://hdl.handle.net/11441/154294
https://doi.org/10.1016/j.jelechem.2017.09.059
Access Level:acceso abierto
Palabra clave:Self-assembled monolayers
11-mercaptoundecanoic acid
Potential-induced dissociation
Electrode impedance
Proton transfer
Descripción
Sumario:Analytical expressions describing the electrochemical impedance spectrum of a metallic electrode modified with an acid thiol monolayer, that undergoes a potential-induced proton transfer, have been derived from an electrostatic model of the interface. The frequency dispersion of the electrode impedance is described by an equivalent circuit that bears some similarities with that associated with a surface redox process. Good agreement is found between the theoretical predictions and the impedance of a Au(111) electrode modified with a 11-mercaptoundecanoic monolayer recorded as a function of ac frequency, dc potential and surface concentration of electrochemically active carboxylic groups. The same thermodynamic and kinetic parameter values are obtained from independent analysis of the voltammetric and impedimetric responses, except in the case of the reorganization energy for proton transfer, which seems to be affected by a slow potential-induced reorientation and dissociation of the external acid groups of the monolayer.