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Boron doped diamond electrochemical sensors for the environment : towards in-situ analysis
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Reily-Horne, Nicole Elizabeth (2021) Boron doped diamond electrochemical sensors for the environment : towards in-situ analysis. PhD thesis, University of Warwick.
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Official URL: http://webcat.warwick.ac.uk/record=b3856561~S15
Abstract
Environmental monitoring is hugely important to aid understanding of the natural processes of the planet and the impact of humans. Electrochemical sensors provide low cost, sensitive devices that could be operated at the source or in-situ due to their low power requirements and portability. Boron doped diamond (BDD) retains all the physical and mechanical properties of diamond with the added property of electrical conductivity. BDD is a relatively catalytically inert material making it an ideal sensor material due to low background currents across a large potential range. Through controlled introduction of a very robust and stable form of sp2 carbon into the BDD surface, pH sensitive quinone groups (BDD-Q) are formed. Such electrodes can be utilised for voltammetric pH sensing.
In Chapter 3, BDD-Q sensors are incorporated into the disc of a ring disc dual electrode arrangement and used to track dynamic pH perturbations driven on the BDD ring electrode by water oxidation. The time-dependant pH changes are shown to vary depending on the buffer capacity of the solution and in this way a methodology for buffer capacity measurements is highlighted.
In Chapter 4, the BDD ring – BDD-Q disc electrode was again used but this time to track the local pH changes associated with the electrocatalytic reduction of dissolved oxygen, nitrate ions and water on both BDD and a Cu nanoparticle functionalised BDD electrode.
In Chapter 5, advancements in heavy metal detection were considered through (i) a new electrode design for electrochemical X-ray fluorescence (EC-XRF) and (ii) use of the BDD ring-disc electrode for at the source Cu detection. In particular, local acidification of the disc environment by water oxidation on the ring, to promote electrodeposition of metallic Cu, in the ppb concentration range.
Finally, in Chapter 6, the impact of bacterial biofilm formation on BDD is investigated under potential control conditions. One of the major barriers to long term in-situ measurements is biofilm formation on the electrode surface. Whilst BDD is a low fouling material with time biofilms will form. The application of low voltages to discourage cell adhesion was investigated as a method to prolong long-term sensor performance in aquatic systems. Pseudomonas aeruginosa was used as a model monospecies biofilm system.
Item Type: | Thesis (PhD) | ||||
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Subjects: | Q Science > QD Chemistry | ||||
Library of Congress Subject Headings (LCSH): | Boron, Nanodiamonds, Electrochemical sensors, Biosensors, Environmental chemistry | ||||
Official Date: | December 2021 | ||||
Dates: |
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Institution: | University of Warwick | ||||
Theses Department: | Department of Chemistry | ||||
Thesis Type: | PhD | ||||
Publication Status: | Unpublished | ||||
Supervisor(s)/Advisor: | Macpherson, Julie V | ||||
Extent: | xxvi, 276 leaves :illustrations (colour) | ||||
Language: | eng |
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