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Palladium nanocrystals enclosed by {100} and {111} facets in controlled proportions and their catalytic activities for formic acid oxidation

机译:由{100}和{111}晶面围成的比例可控的钯纳米晶体及其对甲酸氧化的催化活性

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This article reports a seed-mediated approach to polyhedral nanocrystals of Pd with controlled sizes, shapes, and different proportions of {100} to {111} facets on the surface. The success of this synthesis relies on the use of Pd nanocubes with different sizes as the seeds and the use of formaldehyde as a relatively mild reducing agent. By controlling the ratio of Pd precursor to the seed, we obtained uniform polyhedrons such as truncated cubes, cuboctahedrons, truncated octahedrons, and octahedrons in a purity approaching 100%. The sizes of these polyhedrons were determined by the edge length of the cubic seeds. Since these Pd polyhedrons were characterized by different proportions of {111} to {100} facets, they could serve as model catalysts to uncover the correlation between the surface structure and the catalytic performance for formic acid oxidation. Our measurements indicate that Pd nanocubes exhibited the highest maximum current density in the forward anodic scan, but the peak position was also located at a potential higher than those of the other polyhedrons. When both the current density and the operation potential are taken into consideration, Pd nanocubes with slight truncation at the corners become the best choice of catalyst for formic acid oxidation. Our study also revealed that the size of Pd polyhedrons had essentially no effect on the activity for formic acid oxidation.
机译:本文报道了一种种子介导的Pd多面体纳米晶体方法,该方法具有可控制的大小,形状和表面上{100}至{111}小面的不同比例。该合成的成功取决于使用大小不同的Pd纳米立方作为种子,以及使用甲醛作为相对温和的还原剂。通过控制Pd前体与晶种的比例,我们获得了纯度接近100%的均匀多面体,例如截头的立方体,立方八面体,截头的八面体和八面体。这些多面体的大小由立方晶种的边长确定。由于这些Pd多面体的特征是{111}至{100}面的比例不同,因此它们可以用作模型催化剂,揭示表面结构与甲酸氧化催化性能之间的相关性。我们的测量表明,Pd纳米立方体在正向阳极扫描中表现出最高的最大电流密度,但峰值位置也位于比其他多面体更高的电势上。当同时考虑电流密度和工作电位时,在拐角处略有截断的Pd纳米立方成为甲酸氧化的最佳催化剂选择。我们的研究还表明,Pd多面体的大小对甲酸氧化活性基本没有影响。

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  • 来源
    《Energy & environmental science》 |2012年第4期|p.6352-6357|共6页
  • 作者单位

    Department of Biomedical Engineering, Washington University, St Louis, Missouri, 63130, USA,State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, Xiamen University, Xiamen, Fujian, 361005, P. R. China;

    Department of Biomedical Engineering, Washington University, St Louis, Missouri, 63130, USA,State Key Laboratory of Silicon Materials, Department of Materials Science and Engineering, Zhejiang University, Hangzhou, Zhejiang, 310027, P. R. China;

    State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, Xiamen University, Xiamen, Fujian, 361005, P. R. China;

    Department of Biomedical Engineering, Washington University, St Louis, Missouri, 63130, USA;

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