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电化学合成具有可调组成的介孔 Pt-Au 二元合金,以提高电化学性能。

Electrochemical synthesis of mesoporous Pt-Au binary alloys with tunable compositions for enhancement of electrochemical performance.

机构信息

World Premier International (WPI) Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan.

出版信息

J Am Chem Soc. 2012 Mar 21;134(11):5100-9. doi: 10.1021/ja209044g. Epub 2012 Mar 6.

Abstract

Mesoporous Pt-Au binary alloys were electrochemically synthesized from lyotropic liquid crystals (LLCs) containing corresponding metal species. Two-dimensional exagonally ordered LLC templates were prepared on conductive substrates from diluted surfactant solutions including water, a nonionic surfactant, ethanol, and metal species by drop-coating. Electrochemical synthesis using such LLC templates enabled the preparation of ordered mesoporous Pt-Au binary alloys without phase segregation. The framework composition in the mesoporous Pt-Au alloy was controlled simply by changing the compositional ratios in the precursor solution. Mesoporous Pt-Au alloys with low Au content exhibited well-ordered 2D hexagonal mesostructures, reflecting those of the original templates. With increasing Au content, however, the mesostructural order gradually decreased, thereby reducing the electrochemically active surface area. Wide-angle X-ray diffraction profiles, X-ray photoelectron spectra, and elemental mapping showed that both Pt and Au were atomically distributed in the frameworks. The electrochemical stability of mesoporous Pt-Au alloys toward methanol oxidation was highly improved relative to that of nonporous Pt and mesoporous Pt films, suggesting that mesoporous Pt-Au alloy films are potentially applicable as electrocatalysts for direct methanol fuel cells. Also, mesoporous Pt-Au alloy electrodes showed a highly sensitive amperometric response for glucose molecules, which will be useful in next-generation enzyme-free glucose sensors.

摘要

介孔 Pt-Au 二元合金是通过含有相应金属物种的溶致液晶(LLC)电化学合成的。二维菱方有序 LLC 模板是通过在包括水、非离子表面活性剂、乙醇和金属物种的稀释表面活性剂溶液中滴涂在导电基底上制备的。使用这种 LLC 模板的电化学合成能够制备没有相分离的有序介孔 Pt-Au 二元合金。介孔 Pt-Au 合金中的骨架组成可以通过改变前驱体溶液中的组成比来简单控制。具有低 Au 含量的介孔 Pt-Au 合金表现出具有良好有序的二维六方介孔结构,反映了原始模板的结构。然而,随着 Au 含量的增加,介孔结构的有序性逐渐降低,从而降低了电化学活性表面积。广角 X 射线衍射谱、X 射线光电子能谱和元素映射表明,Pt 和 Au 都在框架中原子分布。与非多孔 Pt 和介孔 Pt 薄膜相比,介孔 Pt-Au 合金对甲醇氧化的电化学稳定性得到了极大提高,这表明介孔 Pt-Au 合金薄膜有望作为直接甲醇燃料电池的电催化剂。此外,介孔 Pt-Au 合金电极对葡萄糖分子表现出高灵敏度的安培响应,这将在下一代无酶葡萄糖传感器中很有用。

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