A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry

A molecular theory of chemically modified electrodes is applied to study redox polyelectroyte modified electrodes. The molecular approach explicitly includes the size, shape, charge distribution, and conformations of all of the molecular species in the system as well as the chemical equilibria (redo...

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Autores principales:	Tagliazucchi, Mario Eugenio, Calvo, Ernesto Julio
Publicado:	2008
Materias:	Charge regulation Modified electrode Molecular theory Polyelectrolyte Redox Amines Bioelectric phenomena Charge distribution Cyclic voltammetry Electrodes Electrolysis Gold Gold compounds Metallizing Molecular structure Organic compounds Osmium Parameter estimation Propane Size distribution Thick films Voltammetry (001) parameter (e ,2e) theory (I ,J) conditions Acid base Applied (CO) bipyridine Chemical equilibriums Chemically modified electrode (CME) Covalently bound Electrochemical behaviors Electrolyte compositions Elsevier (CO) Gold electrodes Inhomogeneous distribution Intermolecular interactions (IMI) Modified electrodes Molecular approach Molecular species Nanometric Phenomenological modeling Polymer layers Redox states Self-assembled Spatial arrangements voltammetric experiments Molecules
Acceso en línea:	https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00134686_v53_n23_p6740_Tagliazucchi http://hdl.handle.net/20.500.12110/paper_00134686_v53_n23_p6740_Tagliazucchi
Aporte de:	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires

id	paper:paper_00134686_v53_n23_p6740_Tagliazucchi
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spelling	paper:paper_00134686_v53_n23_p6740_Tagliazucchi2023-06-08T14:35:56Z A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry Tagliazucchi, Mario Eugenio Calvo, Ernesto Julio Charge regulation Modified electrode Molecular theory Polyelectrolyte Redox Amines Bioelectric phenomena Charge distribution Cyclic voltammetry Electrodes Electrolysis Gold Gold compounds Metallizing Molecular structure Organic compounds Osmium Parameter estimation Propane Size distribution Thick films Voltammetry (001) parameter (e ,2e) theory (I ,J) conditions Acid base Applied (CO) bipyridine Chemical equilibriums Chemically modified electrode (CME) Covalently bound Electrochemical behaviors Electrolyte compositions Elsevier (CO) Gold electrodes Inhomogeneous distribution Intermolecular interactions (IMI) Modified electrodes Molecular approach Molecular species Molecular theory Nanometric Phenomenological modeling Polymer layers Redox states Self-assembled Spatial arrangements voltammetric experiments Molecules A molecular theory of chemically modified electrodes is applied to study redox polyelectroyte modified electrodes. The molecular approach explicitly includes the size, shape, charge distribution, and conformations of all of the molecular species in the system as well as the chemical equilibria (redox and acid-base) and intermolecular interactions. An osmium pyridine-bipyridine complex covalently bound to poly(allyl-amine) backbone (PAH-Os) adsorbed onto mercapto-propane sulfonate (MPS) thiolated gold electrode is described. The potential and electrolyte composition dependent redox and nonredox capacitance can be calculated with the molecular theory in very good agreement with voltammetric experiments under reversible conditions without the use of freely adjustable parameter. Unlike existing phenomenological models the theory links the electrochemical behavior with the structure of the polymer layer. The theory predicts a highly inhomogeneous distribution of acid-base and redox states that strongly couples with the spatial arrangement of the molecular species in the nanometric redox film. © 2008 Elsevier Ltd. All rights reserved. Fil:Tagliazucchi, M. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Calvo, E.J. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. 2008 https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00134686_v53_n23_p6740_Tagliazucchi http://hdl.handle.net/20.500.12110/paper_00134686_v53_n23_p6740_Tagliazucchi
institution	Universidad de Buenos Aires
institution_str	I-28
repository_str	R-134
collection	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
topic	Charge regulation Modified electrode Molecular theory Polyelectrolyte Redox Amines Bioelectric phenomena Charge distribution Cyclic voltammetry Electrodes Electrolysis Gold Gold compounds Metallizing Molecular structure Organic compounds Osmium Parameter estimation Propane Size distribution Thick films Voltammetry (001) parameter (e ,2e) theory (I ,J) conditions Acid base Applied (CO) bipyridine Chemical equilibriums Chemically modified electrode (CME) Covalently bound Electrochemical behaviors Electrolyte compositions Elsevier (CO) Gold electrodes Inhomogeneous distribution Intermolecular interactions (IMI) Modified electrodes Molecular approach Molecular species Molecular theory Nanometric Phenomenological modeling Polymer layers Redox states Self-assembled Spatial arrangements voltammetric experiments Molecules
spellingShingle	Charge regulation Modified electrode Molecular theory Polyelectrolyte Redox Amines Bioelectric phenomena Charge distribution Cyclic voltammetry Electrodes Electrolysis Gold Gold compounds Metallizing Molecular structure Organic compounds Osmium Parameter estimation Propane Size distribution Thick films Voltammetry (001) parameter (e ,2e) theory (I ,J) conditions Acid base Applied (CO) bipyridine Chemical equilibriums Chemically modified electrode (CME) Covalently bound Electrochemical behaviors Electrolyte compositions Elsevier (CO) Gold electrodes Inhomogeneous distribution Intermolecular interactions (IMI) Modified electrodes Molecular approach Molecular species Molecular theory Nanometric Phenomenological modeling Polymer layers Redox states Self-assembled Spatial arrangements voltammetric experiments Molecules Tagliazucchi, Mario Eugenio Calvo, Ernesto Julio A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry
topic_facet	Charge regulation Modified electrode Molecular theory Polyelectrolyte Redox Amines Bioelectric phenomena Charge distribution Cyclic voltammetry Electrodes Electrolysis Gold Gold compounds Metallizing Molecular structure Organic compounds Osmium Parameter estimation Propane Size distribution Thick films Voltammetry (001) parameter (e ,2e) theory (I ,J) conditions Acid base Applied (CO) bipyridine Chemical equilibriums Chemically modified electrode (CME) Covalently bound Electrochemical behaviors Electrolyte compositions Elsevier (CO) Gold electrodes Inhomogeneous distribution Intermolecular interactions (IMI) Modified electrodes Molecular approach Molecular species Molecular theory Nanometric Phenomenological modeling Polymer layers Redox states Self-assembled Spatial arrangements voltammetric experiments Molecules
description	A molecular theory of chemically modified electrodes is applied to study redox polyelectroyte modified electrodes. The molecular approach explicitly includes the size, shape, charge distribution, and conformations of all of the molecular species in the system as well as the chemical equilibria (redox and acid-base) and intermolecular interactions. An osmium pyridine-bipyridine complex covalently bound to poly(allyl-amine) backbone (PAH-Os) adsorbed onto mercapto-propane sulfonate (MPS) thiolated gold electrode is described. The potential and electrolyte composition dependent redox and nonredox capacitance can be calculated with the molecular theory in very good agreement with voltammetric experiments under reversible conditions without the use of freely adjustable parameter. Unlike existing phenomenological models the theory links the electrochemical behavior with the structure of the polymer layer. The theory predicts a highly inhomogeneous distribution of acid-base and redox states that strongly couples with the spatial arrangement of the molecular species in the nanometric redox film. © 2008 Elsevier Ltd. All rights reserved.
author	Tagliazucchi, Mario Eugenio Calvo, Ernesto Julio
author_facet	Tagliazucchi, Mario Eugenio Calvo, Ernesto Julio
author_sort	Tagliazucchi, Mario Eugenio
title	A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry
title_short	A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry
title_full	A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry
title_fullStr	A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry
title_full_unstemmed	A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry
title_sort	molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: reversible cyclic voltammetry
publishDate	2008
url	https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00134686_v53_n23_p6740_Tagliazucchi http://hdl.handle.net/20.500.12110/paper_00134686_v53_n23_p6740_Tagliazucchi
work_keys_str_mv	AT tagliazucchimarioeugenio amoleculartheoryofchemicallymodifiedelectrodeswithselfassembledredoxpolyelectrolyethinfilmsreversiblecyclicvoltammetry AT calvoernestojulio amoleculartheoryofchemicallymodifiedelectrodeswithselfassembledredoxpolyelectrolyethinfilmsreversiblecyclicvoltammetry AT tagliazucchimarioeugenio moleculartheoryofchemicallymodifiedelectrodeswithselfassembledredoxpolyelectrolyethinfilmsreversiblecyclicvoltammetry AT calvoernestojulio moleculartheoryofchemicallymodifiedelectrodeswithselfassembledredoxpolyelectrolyethinfilmsreversiblecyclicvoltammetry
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A molecular theory of chemically modified electrodes with self-assembled redox polyelectrolye thin films: Reversible cyclic voltammetry

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