期刊
ELECTROCHIMICA ACTA
卷 52, 期 2, 页码 385-393出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2006.05.019
关键词
oxygen reduction; methanol crossover; platinum alloys; direct methanol fuel cell; particle morphology
The oxygen reduction reaction (ORR) was studied on carbon dispersed Pt and Pt-Co alloyed nanocatalysts with high contents of Co in H2SO4 and H2SO4/CH3OH solutions. The characterization techniques considered were transmission electron microscopy (TEM), X-ray diffraction (XRD) and in situ X-ray absorption near edge structure (XANES). The electrochemical activity for the ORR was evaluated from steady state polarization measurements, which were carried out in an ultra thin layer rotating disk electrode. The results showed that with the increase of Co content, the nanoparticle size distributions become sharper and the mean particle diameters become smaller. XRD indicated low degree of alloy formation but significant phase segregation of Co was observed only for Pt-Co/C 1:3 and 1:5 (Pt:Co atomic ratios). The electrochemical measurements indicated that the four-electrons mechanism is mainly followed for the ORR on all materials and the electrocatalytic activities per gram of Pt is higher for the catalysts with higher Co contents. This was explained based on the XANES results which evidenced a decrease of the coverage of oxygenated Pt adsorbates due to the presence of Co. In the methanol-containing electrolyte, the Pt-Co/C 1:5 catalyst showed the highest performance. This was attributed to its low activity for the methanol oxidation due to the smaller probability for presenting three Pt neighboring Pt active sites. (c) 2006 Elsevier Ltd. All rights reserved.
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