This thesis focuses on developing support materials for direct methanol fuel cell (DMFC) catalysts. The approach involves using graphene based materials including reduced graphene oxide (rGO), reduced graphene oxide-activated carbon (rGO-AC) hybrid and reduced graphene oxide-silicon carbide (rGO-SiC) hybrid as a support for Pt and Pt-Ru nanoparticles. Pt/rGO and Pt-Ru/rGO catalysts were synthesized by three chemical reduction methods: (1) modified polyol, (2) ethylene glycol (EG) reduction and (3) mixed reducing agents (EG + NaBH4) methods. The synthesized catalysts were characterized by physical and electrochemical techniques. The results demonstrated that Pt/rGO-3 and Pt-Ru/rGO-3 catalyst synthesized with Method-3 exhibit higher electrochemical active surface area (ECSA) than the other rGO supported and Vulcan supported commercial electrocatalysts. In addition, Pt/rGO-3 and Pt-Ru/rGO-3 catalysts showed better oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activities, respectively. The DMFC tests under different cell temperature (30, 50 and 70°C) and methanol concentration (1, 2 and 4 M) conditions further demonstrated the higher catalytic activity of the catalysts. The peak power density obtained with Pt/rGO-3 cathode and Pt-Ru/rGO-3 anode catalysts at 70°C with 1 M methanol was 63.3 mW/cm2 which is about 59 % higher than that of commercial Pt/C and Pt-Ru/C catalysts. The enhanced performance was attributed to the highly accessible and uniformly dispersed nanoparticles on rGO support with large surface area and high conductivity. Pt/rGO-AC (reduced graphene oxide-activated carbon) and Pt-Ru/rGO-AC catalysts were synthesized with various rGO:AC support ratios by using biomass derived AC. The results showed that the catalysts with content of 20 wt. % AC support (Pt/rGO-AC20 and Pt-Ru/rGO-AC20) exhibited higher ECSA, better catalytic activity and stability among all the tested catalysts. With 1 M methanol and 70°C cell temperature, the MEA with Pt/rGO-AC20 cathode and Pt-Ru/rGO-AC anode catalysts gave 19.3 % higher peak power density (75.5 mW/cm2), than that of Pt/rGO-3 and Pt-Ru/rGO-3 catalysts. The better DMFC performance was due to the incorporation of AC particles into rGO structure which builds electron-conductive paths between rGO sheets, facilitates the transport of reactant and products and provides higher specific surface area for the uniform distribution of nanoparticles. Pt/rGO-SiC catalysts were synthesized with variable silicon carbide (SiC) content in the hybrid support. Pt/rGO-SiC10 (10 wt. % of SiC support) catalyst showed higher ECSA and better catalytic activity compared to the Pt/SiC, Pt/rGO-3 and Pt/rGO-SiC20 catalysts. In addition, the Pt/rGO-SiC10 gave 14.2 % higher DMFC performance than the Pt/rGO-3 catalyst in terms of power density. The high performance can be attributed to the insertion of the SiC nanoparticles into rGO structure that improves the conductivity and stability of the catalyst by playing a spacer role between rGO layers. In summary, the overall results showed that the catalytic performance of the catalysts followed the trend in terms of support material: rGO-AC20 > rGO-SiC10 > rGO > Vulcan. The study demonstrated that the novel rGO-AC and rGO-SiC hybrids are promising catalyst supports for direct methanol fuel cell applications.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:748029 |
| Date | January 2017 |
| Creators | Özdinçer, Baki |
| Contributors | Garforth, Arthur ; Holmes, Stuart |
| Publisher | University of Manchester |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | https://www.research.manchester.ac.uk/portal/en/theses/novel-support-materials-for-direct-methanol-fuel-cell-catalysts(f7dfe29a-a593-44a6-a9e3-e9e8f5b8b2a2).html |
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