Methanol (CH3OH) reformation with water (H2O) to in situ release hydrogen (H2) is regarded as a hopeful H2 production approach for polymer electrolyte membrane fuel cells, while developing highly efficient… Click to show full abstract
Methanol (CH3OH) reformation with water (H2O) to in situ release hydrogen (H2) is regarded as a hopeful H2 production approach for polymer electrolyte membrane fuel cells, while developing highly efficient CH3OH reformation catalysts still remains a great challenge. Herein, a series of Pt-based ultrafine nanowires (UNWs) with high surface atom ratio are used as highly active and stable catalysts for CH3OH reformation to H2. By tuning Pt3M (M = Fe, Co, Ni), support and the composition of the Pt xFe UNWs, the optimized Pt4Fe UNWs/Al2O3 exhibits excellent catalytic behaviors with the high H2 turnover frequency reaching to 2035.8 h-1, more than 4 times higher than that of Pt UNWs/Al2O3. The reaction mechanism investigated by diffuse reflectance infrared Fourier transform spectroscopy turns out that the production of H2 undergoes the CH3OH decomposition to *CO and gas-shift reaction of *CO with H2O. Combing with the XPS result and the density functional theory calculations, the high CH3OH reformation activity of Pt4Fe UNWs/Al2O3 is attributable to synergism between Pt and Fe, which facilitates H2 desorption and intermediate HCOO* and *COO formations via the reaction between *CO and OH-.
               
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