mediated electron transfer at redox active monolayers在单层氧化还原活性介导的电子转移.pdfVIP

Sensors 2001, 1, 215-228 sensors ISSN 1424-8220 © 2001 by MDPI /sensors Mediated Electron Transfer at Redox Active Monolayers Michael E.G. Lyons Physical Electrochemistry Laboratory, Department of Chemistry, Nasr Institute of Advanced Materials Science, University of Dublin, Trinity College, Dublin 2, Ireland. Tel: 353-1-608 2051. Fax: 353-1- 671 2826. E-mail: melyons@mail.tcd.ie Received: 29 November 2001 / Accepted: 9 December 2001 / Published: 13 December 2001 Abstract: A theoretical model describing the transport and kinetic processes involved in heterogeneous redox catalysis of solution phase reactants at electrode surfaces coated with redox active monolayers is presented. Although the analysis presented has quite general applicability, a specific focus of the paper is concerned with the idea that redox active monolayers can be used to model an ensemble of individual molecular nanoelectrodes. Three possible rate determining steps are considered: heterogeneous electron transfer between immobilized mediator and support electrode ; bimolecular chemical reaction between redox mediator and reactant species in the solution phase, and diffusional mass transport of reactant in solution. A general expression for the steady state reaction flux is derived which is valid for any degree of reversibility of both the hetero