Promotion by hydrous ruthenium oxide of platinum for methanol electro-oxidation

Promotion by hydrous ruthenium oxide of platinum for methanol electro-oxidation
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铂水合氧化钌促进甲醇电氧化

DOI:
10.1016/j.jcat.2010.07.021
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发表时间:
2010-09
影响因子:
7.3
通讯作者:
--
中科院分区:
化学1区
文献类型:
--
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以非晶态水合氧化钌(RuOxHy)为唯一含钌物种,制备了以多壁碳纳米管为载体的Pt-(RuOxHy)m电催化剂(m为Ru/Pt原子比),并采用X射线衍射、X射线光电子能谱、程序升温还原、热重分析和透射电镜等技术对催化剂进行了表征.循环伏安法和计时电流法研究表明,RuOxHy的存在显著提高了Pt的抗CO能力和催化活性。在0.5M H_2SO_4溶液中反复CV预处理至高于0.46V(vs. SCE)时,RuOxHy的溶解明显,改变了Pt的RuOxHy含量、Pt-RuOxHy邻近性和表面结构,从而改变了Pt在最终电极中的电催化活性。然而,当预处理电位设定不高于0.46V时,未鉴定出RuOxHydissolution。根据RuOxHy 3作为电子/质子混合导体的特点,对RuOxHy 3的促进作用进行了讨论。
Pt–(RuOxHy)melectrocatalysts (m being the atomic Ru/Pt ratio) supported on multi-walled carbon nanotubes, in which amorphous hydrous ruthenium oxide (RuOxHy) is the exclusive Ru-containing species, were prepared and comprehensively characterized by X-ray diffraction, X-ray photoelectron spectroscopy, temperature-programmed reduction, thermogravimetric analysis and transmission electron microscopy techniques. Cyclic voltammetry (CV) and chronoamperometry studies of CO stripping and methanol electro-oxidation indicated that the CO tolerance and catalytic activity of Pt improved remarkably by the co-presence of RuOxHy. Repeated CV pretreatments in 0.5M H2SO4up to potentials higher than 0.46V (vs. SCE) induced significant dissolution of RuOxHy, which changed the RuOxHycontent, Pt–RuOxHyproximity and surface structure of Pt, and consequently altered the electrocatalytic activity of Pt in the final electrode. However, RuOxHydissolution was not identified when the pretreatment potentials was set no higher than 0.46V. Discussion on the promotional function of RuOxHywas made based on the peculiarity of RuOxHyas a mixed electron/proton conductor.
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