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Aspects of Direct Alkaline Alcohol Fuel Cells

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Aspects of Direct Alkaline Alcohol Fuel Cells ( aspects-direct-alkaline-alcohol-fuel-cells )

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Energies 2010, 3 1502 2.1. Alcohol Oxidation The mechanism of electrochemical oxidation of methanol on platinum in alkaline systems involves formation of adsorbed methanolic species and OH on the Pt surface. The oxidation takes place through a series of reaction steps involving successive electron transfer, i.e. partial oxidation, to form adsorbed species. These react with adsorbed OH to potentially form carbon dioxide. The reaction mechanism has been written as follows [22]: Pt + OH−→Pt-(OH)ads + e− Pt + (CH3OH)sol→Pt-(CH3OH)ads Pt-(CH3OH)ads + OH−→Pt-(CH3O)ads + H2O + e− Pt-(CH3O)ads + OH−→Pt-(CH2O)ads + H2O + e− Pt-(CH2O)ads + OH−→Pt-(CHO)ads + H2O + e− Pt-(CHO)ads + OH−→Pt-(CO)ads + H2O + e− Pt-(CHO)ads + Pt-(OH)ads + 2OH−→2Pt + CO2 + 2H2O + 2e− Pt-(CHO)ads + Pt-(OH)ads + OH−→Pt + Pt-(COOH)ads + H2O + e− Pt-(CO)ads + Pt-(OH)ads + OH−→2Pt + CO2 + H2O + e− Pt-(CO)ads + Pt-(OH)ads  Pt + Pt-(COOH)ads Pt-(COOH)ads + OH−→Pt-(OH)ads + HCOO− Pt-(COOH)ads + Pt-(OH)ads→2Pt +CO2 + H2O (5) The rate-determining step is most likely the reaction with the oxidation of the active intermediate—CHO [23–29]. For other alcohols, the higher energy density and lower toxicity of polyhydric alcohols still attract lots of interest in applying these alcohols in fuel cells, but the electrochemical oxidation is more difficult and the reaction mechanism is more complicated, since it involves breaking C-C bond(s). The reaction at low temperature leads to a low Faradic efficiency. The mechanism and kinetics of oxidation of different alcohols using Pt-based and non-Pt based metal catalysts have been investigated. Tremiliosi-Filho et al. [30] and de Lima and Varela [31] investigated ethanol oxidation on polycrystalline gold electrodes. Liang et al. [32] and Nguyen et al. [33] have both studied ethanol oxidation on palladium catalysts. For ethanol oxidation in alkaline media, the formation of acetaldehyde or acetic acid was identified [34]. The steps involved can be presented as: 1. M + OH−→M-OHads + e− 2. M + CH3CH2OH→M-(CH3CH2OH)ads 3. M-(CH3CH2OH)ads + 3OH−→M-(CH3CO)ads + 3H2O + 3e− 4. M-(CH3CO)ads + M-OHads→M-CH3COOH + M 5. M-CH3COOH + OH−→M + CH3COO− + H2O M = Au or Pd. (6)

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