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High-throughput electrochemistry (HTP): a new approach to the rapid development of modified carbon electrodes

Record type: Thesis (Doctoral)

The major aim of this project was development of novel covalently modified glassy carbon electrodes for application in NADH-dependent biosensors using combinatorial and high-throughput methods. Studies on transition metal complexes containing redox active 1,1-phenanthroline-5,6-dione (phendione) ligand(s) showed they are effective electrocatalysts for oxidation of NADH. In order to covalently tether the metal complexes at the GC surface, the design of GC electrodes modified with novel metal complexes bearing phendione ligand(s) was proposed based on sequential electrochemical and solid-phase synthesis methods. Initial work involved optimisation of the process for modification of individual GC electrodes. Firstly, following earlier work, the GC electrodes were electrochemically functionalised by primary amines or a diazonium salt bearing Boc-protected amine groups, which allowed introduction of chelating ligands at the GC surface under solid-phase coupling conditions. The final step involved coordination of the bidentate ligand at the GC surface to the metal centre and formation of novel metal complexes under solid-phase coupling conditions. The successfully modified individual electrodes were applied in the design of a library of GC electrodes modified with different linkers, ligands and metal complexes and prepared in a combinatorial and parallel way. The library was electrochemically screened in a high-throughput way using a multichannel potentiostat, which allowed instant comparison of electrochemical and electrocatalytic properties between different members of the library. The experimental data extracted from HTP screening of the library were used for evaluation of a) the surface coverage obtained for different library members; b) the catalytic activity towards NADH oxidation and c) the kinetics parameters kcat and KM for the electrocatalytic oxidation of NADH for all members of the library.

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Citation

Pinczewska, Aleksandra (2011) High-throughput electrochemistry (HTP): a new approach to the rapid development of modified carbon electrodes University of Southampton, School of Chemistry, Doctoral Thesis , 204pp.

More information

Published date: December 2011
Organisations: University of Southampton, Chemistry

Identifiers

Local EPrints ID: 341808
URI: http://eprints.soton.ac.uk/id/eprint/341808
PURE UUID: 9070276f-019a-401d-9679-11e7cc258ded
ORCID for Philip Bartlett: ORCID iD orcid.org/0000-0002-7300-6900

Catalogue record

Date deposited: 12 Nov 2012 14:51
Last modified: 18 Jul 2017 05:32

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Contributors

Author: Aleksandra Pinczewska
Thesis advisor: Philip Bartlett ORCID iD

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