Synthesis And Characterization Of Platinum Based Catalysts For Fuel Cells

Platinum (Pt) and platinum alloys have attracted wide attention as catalysts to attain high performance to increase the power density and reduce the component cost of polymer electrolyte membrane fuel cells (PEMFCs). Extensive research has been conducted in the areas of new alloy development and understanding of mechanisms of electrochemical oxygen reduction reaction (ORR). The durability of PEMFCs is also a major barrier to the commercialization of these fuel cells. Recent studies have suggested that potential cycling can gradually lead to loss of active surface area due to Pt dissolution and nanoparticle grain growth [1]. In this thesis we report a one-step synthesis of highly-dispersed Pt nanoparticles and Pt- Cobalt supported on Ketjen carbon black (20% Pt/C & 20% Pt₃Co/C) as electro-catalysts for PEMFCs. Pt particles with size in the range of ~ 2.6nm (Pt/C) and 3.9 nm (Pt₃Co/C) were obtained through adsorption on carbon supports and subsequently thermal decomposition of platinum acetylacetonate (Pt(acac)₂). A comparative characterization analysis, including X-ray diffraction (XRD), high resolution transmission electron microscope (HR-TEM), FT-iR, EDAX, cyclic voltammetry (CV), and oxygen reduction reaction (ORR) activity, was performed on the synthesized and commercial (46.5wt% TKK) catalysts. The analysis was to reveal the Pt dispersion on the carbon support, particle size and distribution, electrochemical surface area (ECA), and ORR activities of these catalysts. It was found that the synthesized Pt/C showed similar particle size to that of the TKK catalysts (2.6nm and 2.7nm, respectively), but narrower particle size distribution; while the particle size for Pt₃Co/C was found to be ~3.9 nm. Accelerated durability tests (ADT) under potential cycles were also performed for Pt/C and TKK to study the electrochemical degradation of the catalysts in corrosive environments. The ADTs revealed that the two catalysts (Pt/C & TKK) were comparable with respect to degradation in ECA and ORR activities. Initial electrochemical evaluation of Pt₃Co/C was conducted, but durability studies were not attempted in this thesis due to its worse ORR kinetics than those of the Pt/C catalyst. From the experimental data, it was found that particle size impacted negatively the ECA and ORR activity of the catalysts.