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Novel electrochemiluminescent interfaces for chemical sensing applications

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posted on 2023-01-18, 17:49 authored by David James Eastman Piper
Submission note: A thesis submitted in total fulfilment of the requirements for the degree of Doctor of Philosophy to the Department of Physics, Faculty of Science, Technology and Engineering, La Trobe University, Bundoora.

Electrogenerated Chemiluminescence otherwise known as Electrochemiluminescence (ECL) is an effective analytical tool for many organic compounds of clinical and environmental importance. The technique can allow for the regeneration of the luminescent reagent during the course of analysis making it well suited to the development of solid state sensing platforms. In addition, immobilisation of the luminescent reagent can provide opportunities for improved sensitivity and reproducibility compared to solution phase ECL systems. The overall aim of this thesis is to further the development of sensitive and stable ECL-based detection platforms. The thesis focuses on two distinct methods for the immobilisation of the luminescent reagent, tris(2,2`-bipyridyl) ruthenium(II). The first modification method involves the use of a composite polymer based on the perfluorinated ionomer, Nafion and the conducting polymer polypyrrole. The presence of polypyrrole results in improved layer stability when compared to Nafion-based layers. The improvement in layer stability comes at the cost of sensitivity, with detection limits for the model analytes oxalate and tripropylamine being 10 μM and 100 nM, respectively; an order of magnitude decrease in sensitivity compared with Nafion-based layers. The second electrode modification method investigates the use of aryl diazoniums to form thin films of luminescent reagent at the electrode surface. Diazoniums were used to form ECL active films via both the attachment of a ligand and subsequent complexation at the surface and the attachment of the luminescent complex directly at the electrode surface. Attachment of the luminescent complex was achieved via both electroreduction of the diazonium from aqueous solution and the spontaneous deposition of the film with the v resulting films characterised using CV, XPS, TOF-SIMS and AFM. The films were found to be stable over a period of several hours while remaining sensitive to low concentrations (10 nM) of model analytes such as 2-(dibutylamino)ethanol.

History

Center or Department

Faculty of Science, Technology and Engineering. Department of Physics.

Thesis type

  • Ph. D.

Awarding institution

La Trobe University

Year Awarded

2011

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This thesis contains third party copyright material which has been reproduced here with permission. Any further use requires permission of the copyright owner. The thesis author retains all proprietary rights (such as copyright and patent rights) over all other content of this thesis, and has granted La Trobe University permission to reproduce and communicate this version of the thesis. The author has declared that any third party copyright material contained within the thesis made available here is reproduced and communicated with permission. If you believe that any material has been made available without permission of the copyright owner please contact us with the details.

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