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Title: Gold copper based catalysts in the development of direct formic acid fuel cells
Author: Oseghale, Charles Ijogbemeye
ISNI:       0000 0004 7226 4726
Awarding Body: University of Sheffield
Current Institution: University of Sheffield
Date of Award: 2017
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There is a growing awareness of the need for fundamental and applied research in energy storage and conversion due to the global climate issue with energy sources, environmental and human health challenges. In this work, development of a new synthesis route for catalysts, physicochemical and electrochemical research is reported for direct formic acid fuel cells. The synthesis method is based on the sodium borohydride reduction of (Pd2+, Cu2+, Au3+) precursor, stabilised by polyvinylpyrrolidone for the preparation of a highly stable catalysts with, well-controlled particle size distribution. The surface and bulk properties of the catalysts were characterised by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), atomic force microscopy (AFM), and electrochemically by cyclic voltammetry and chronoamperometry. The results obtained for Pd-C showed that a uniform XRD estimated the size distribution in a narrow particle size range with an average size of 1.4 ± 0.11 nm. Electrochemical studies for formic acid electrooxidation reveals that Pd-CH3BO3 + NH4F(21wt.%) presents superior catalytic activity (over 44 %) than that of the Pd-CPVP(43.5wt.%) synthesis route. For an equivalent electrode paste, Pd-CPVP(43.5wt.%) exhibited a greater electrochemical surface area (ECSA) than Pd-CPVP(43.5wt.%) but achieved a lower utilisation of palladium. The electrooxidation of the catalyst shows three times higher activity for formic acid oxidation than commercial gold nanoparticles dispersed on the carbon support. The enhanced catalytic performance is attributed to the electronic synergistic effect of copper and the specific gold structure promoting oxidation of adsorbed intermediate species. Overall, these findings have significant implications for practical direct formic acid fuel cells (DFAFCs) technology by the controlled Au-shell Cu-core anode catalysts application. Overall, palladium catalysts demonstrated better electrocatalytic activities for formic oxidation than Au and gold copper catalysts. This work is part of the initial stages of the effort to develop a low-cost gold-catalyst for DFAFCs technology.
Supervisor: Hall, Peter Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available