Journal
JOURNAL OF POWER SOURCES
Volume 220, Issue -, Pages 399-404Publisher
ELSEVIER
DOI: 10.1016/j.jpowsour.2012.07.098
Keywords
Electrocatalysis; Metal oxides; Fuel cells; Electronic interaction; Methanol oxidation
Funding
- Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan [19206079]
- Tokyo Tech. GCOE Program for Energy Science
- Government of Japan
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The current study addresses the electrocatalytic activity of tantalum oxide (TaOx)-modified Pt electrode as a novel catalyst for methanol oxidation in acidic media. The modified Pt electrode is shown to support a larger oxidation current of methanol compared to that obtained at the unmodified Pt electrode concurrently with a favorable significant shift of the onset potential of methanol oxidation. Tafel plots, with a slope close to 0.118 V decade(-1), were obtained for methanol oxidation at the unmodified and TaOx-modified Pt electrodes, reflecting that the methanol oxidation proceeds with the first electron transfer as the rate-determining step. The observed enhancement was attributed to a favorable d-d metal-metal oxide interaction which changes the electronic property of Pt and hence enhances the oxidation of the adsorbed reaction intermediates (e.g., COads). Moreover, a possible contribution of the OH spillover via a so-called bifunctional mechanism is proposed. The influence of the temperature on the oxidation current of methanol at the TaOx-modified Pt electrode is investigated and apparent activation energy, E-a, for methanol oxidation is calculated as 39 kJ mol(-1) at a specific potential. The proposed catalyst showed a good enhancement for methanol oxidation for a prolonged time of continuous potentiostatic electrolysis. (C) 2012 Elsevier By. All rights reserved.
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