Philosophiae Doctor - PhD / High Temperature Polymer Electrolyte Membrane Fuel Cells (HT-PEMFC) have
received renewed interest in recent years due to its inherent advantages associated with the limitations faced by Low Temperature Polymer Electrolyte Membrane Fuel Cells (LT-PEMFC). The high Pt loadings required for PEMFCs have significantly hindered its commercialisation. Electrophoretic Deposition (EPD) is a promising route to reduce the noble metal loading. EPD is a method in which charged colloidal particles are deposited onto a target substrate under the force of an externally applied electric field. To effectively study the EPD method, the methodology of this study was divided into two parts: (i) the EPD method was studied via known empirical methods to fabricate, test and characterise MEAs suitable for HT-PEMFCs. The feasibility of the EPD method was determined by comparing the performance of the fabricated EPD MEAs to MEAs fabricated via spraying methods, and (ii) due to the promising results obtained in part (i) of the methodology, a theoretical model was developed to obtain a deep understanding about nature of the interactions between the Pt/C particles in a colloidal suspension. The theoretical model will serve as a foundation for future studies.
In part (i) of the methodology, the Pt/C particles were studied in organic solutions (i.e. Isopropyl Alcohol, IPA) via the Zetasizer Nano ZS instrument under various salt (NaCl) concentrations and pH conditions while introducing polymeric surfactants, i.e. Nafion® ionomer and Polytetrafluoroethylene (PTFE) to the suspension. The optimum catalyst suspensions were selected to fabricate GDEs via the EPD method. Physical characterisations revealed that the EPD GDEs exhibited cracked morphology with high porosity. Electrochemical characterisations revealed that the EPD MEA showed significantly better performance (i.e. 73% higher peak power) compared to the hand vi sprayed MEA due to lower charge transfer and mass transport resistance at high current densities. Compared to the ultrasonically sprayed MEA, the EPD MEA exhibited a peak power increase of ~12% at a slightly lower Pt loading (i.e. ~4 wt%). A comparative study between the Nafion® ionomer and PTFE in the CLs of two EPD MEAs revealed superior performance for the EPD MEA with the PTFE in the CLs. Part (ii) of the methodology deals with the electrical interfacial properties of the aqueous Pt/C suspension. The study consists of two sets of measurements (i.e. electrophoretic and coagulation dynamic studies) conducted for different electrolyte compositions. A theoretical background on determining the interfacial potential and charge from electrophoretic and coagulation dynamic measurements are provided. Detailed statements of the Standard Electrokinetic and Derjaguin, Landau, Vervey and Overbeek Models are given in the forms that are capable of addressing electrophoresis and the interaction of particles for an arbitrary ratio of the particle to Debye radius,
interfacial potential and electrolyte composition. The obtained experimental data were processed by using numerical algorithms based on the formulated models for obtaining the interfacial potential and charge. While analysing the dependencies of interfacial potential and charge on the electrolyte compositions charge, conclusions were made regarding the mechanisms of charge formation. It was established that the behaviour of system stability is in qualitative agreement with the results computed from the electrophoretic data. The verification of quantitative applicability of the employed models was conducted by calculating the Hamaker constant from the experimental data. It was proposed how to explain the observed variations of the predicted Hamaker constant and its unusually high value.
| Identifer | oai:union.ndltd.org:netd.ac.za/oai:union.ndltd.org:uwc/oai:etd.uwc.ac.za:11394/3550 |
| Date | January 2013 |
| Creators | Felix, Cecil |
| Contributors | Pasupathi, Sivakumar, Yaroshchuk, Andriy |
| Source Sets | South African National ETD Portal |
| Language | English |
| Detected Language | English |
| Rights | uwc |
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