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Synthesis of platinum and platinum-copper branched nanoparticles for electrooxidation of methanol.

机译:铂和铂-铜支化纳米颗粒的合成,用于甲醇的电氧化。

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摘要

Platinum and Pt alloys are among the most important heterogeneous catalysts for many organic reactions and electrochemical reactions associated with the fuel cell technologies. How to reduce Pt usage while maintaining the performance of the catalysts becomes a subject for intensive research in materials chemistry. For heterogeneous catalysis, the catalytic reactivity and selectivity are strongly correlated with different crystallographic facets exposed on the surface. The facets with high-index planes whose Miller indices with at one is larger than unity are generally more active than those with low-index planes (e.g., {100}, {111}, and {110}). Tuning the morphology of the nanoparticles to expose more high-index planes on the surface can improve the catalytic activity of the nanoparticles. As compared to isotropic nanoparticles, the branched nanostructures are the promising morphology that can improve both the activity and stability of the catalysts. In this work, a two-step polyol synthesis has been developed to synthesize the branched nanostructures of Pt at high-yield. This two-step process involves a slow reduction using ethylene glycol in the presence of oxidative etchants, following by a fast reduction using ascorbic acid. The slow reduction kinetics facilitates the formation of cubooctahedral single-crystal seeds while the fast reduction kinetics allows for the overgrowth of nanocrystals along the {111} facets in a short period of time, resulting in the branched nanostructures. By co-reducing Pt and Cu precursors, this approach has been demonstrated to synthesize the Pt-Cu dendritic nanostructures for the first time. The catalytic activity of these Pt and Pt-Cu nanostructures has been studied for MOR. It was found that Pt branched nanostructures reduced the CO-poisoning as compared to the Pt/C and the dendritic Pt-Cu nanostructures showed both enhanced resistance of CO-poisoning and improved efficiency of ethanol oxidation.
机译:铂和铂合金是与燃料电池技术相关的许多有机反应和电化学反应中最重要的非均相催化剂。如何在保持催化剂性能的同时减少Pt用量成为材料化学研究的主题。对于非均相催化,催化反应性和选择性与暴露在表面上的不同结晶学方面密切相关。具有高折射率平面且其Miller指数大于1的小平面通常比具有低折射率平面的小平面(例如{100},{111}和{110})更活跃。调节纳米颗粒的形态以在表面上暴露更多的高折射率平面可以改善纳米颗粒的催化活性。与各向同性的纳米粒子相比,支链的纳米结构是有前途的形态,可以改善催化剂的活性和稳定性。在这项工作中,已经开发了两步多元醇合成方法,以高产率合成Pt的支链纳米结构。此两步过程涉及在氧化蚀刻剂存在下使用乙二醇缓慢还原,然后使用抗坏血酸快速还原。缓慢的还原动力学促进了立方八面体单晶晶种的形成,而快速的还原动力学使得纳米晶在短时间内沿{111}小面过度生长,从而形成了分支的纳米结构。通过共还原Pt和Cu前驱体,已证明该方法首次合成了Pt-Cu树状纳米结构。已经研究了这些Pt和Pt-Cu纳米结构的催化活性。发现与Pt / C相比,Pt支化的纳米结构降低了CO中毒,并且树枝状Pt-Cu纳米结构显示了增强的CO中毒抵抗力和改善的乙醇氧化效率。

著录项

  • 作者

    Taylor, Eric.;

  • 作者单位

    University of Arkansas.;

  • 授予单位 University of Arkansas.;
  • 学科 Chemistry General.;Nanoscience.
  • 学位 M.S.
  • 年度 2013
  • 页码 53 p.
  • 总页数 53
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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