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Synthesis, characterization and electrochemical studies of novel platinum-based nanomaterials.

机译:新型铂基纳米材料的合成,表征和电化学研究。

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摘要

Platinum (Pt) as well as its alloys represent some of the most efficient catalyst materials among intermetallic compounds and alloys. An important clue throughout this work is the development of a desired synthetic approach of Pt-based nanomaterials---a one-step hydrothermal co-reduction of inorganic metal precursors. Slight modifications in experimental conditions have led to the production of Pt-based nanostructured materials with two distinct morphologies: (i) three-dimensional (3D) nanoporous Pt-M networks (M= Ru, Ir, Pb, Pd) when formaldehyde is used as a reducing agent; and (ii) 3D intermetallic Pt-M nanodendrites (M= Au, Pb, Bi or Pd) when formate ligands are present as multi-functional reagents in the hydrothermal process.;In the case of synthesizing Pt-based nanodendritic materials, ammonium formate and formic acid were used as multi-functional reagents in the hydrothermal-assisted fabrication of alloyed PtAu and PtPb nanodendrites, respectively. Electrochemical studies reveal that both PtAu and PtPb nanodendrites exhibit exceptionally high electrocatalytic activities in formic acid oxidation owing to their unique alloyed intermetallic crystal structures. The proposed coordination and co-reduction alloying mechanism together with the foreign particle-induced dendritic growth mechanism have been further proved to be universal for fabricating a wide range of intermetallic nanodendrites, including bimetallic Pt-Bi, Pt-Pd, Pd-Ru and trimetallic Pt-Pd-Pb with controllable compositions.;Those as-synthesized Pt-based nanoporous catalysts not only possess significantly high surface areas, but also exhibit superb electrocatalytic activities towards the electrochemical oxidation of methanol and formic acid. Among them, the nanoporous PtPb networks were further tested towards the electro-oxidation of glucose. Voltammetric and amperometric results demonstrate that the PtPb electrodes have strong and sensitive current responses to the incremental glucose concentrations, and are capable of sensing glucose with excellent selectivity in neutral media.
机译:铂(Pt)及其合金是金属间化合物和合金中最有效的催化剂材料。贯穿这项工作的重要线索是开发了一种基于Pt的纳米材料所需的合成方法-一步一步水热共还原无机金属前体。在实验条件下的轻微修改导致产生了具有两种不同形态的基于Pt的纳米结构材料:(i)使用甲醛时的三维(3D)纳米多孔Pt-M网络(M = Ru,Ir,Pb,Pd)作为还原剂; (ii)当水热过程中甲酸配体作为多功能试剂存在时的3D金属间Pt-M纳米树枝晶(M = Au,Pb,Bi或Pd);在合成基于Pt的纳米树枝状材料时,甲酸铵在水热辅助制备合金化PtAu和PtPb纳米枝晶中,分别使用甲酸和甲酸作为多功能试剂。电化学研究表明,由于PtAu和PtPb纳米枝晶具有独特的合金化金属间晶体结构,因此它们在甲酸氧化中表现出异常高的电催化活性。所提出的配位和共还原合金化机制以及异物引起的树枝状生长机制已被进一步证明可用于制造多种金属间纳米树枝晶,包括双金属Pt-Bi,Pt-Pd,Pd-Ru和三金属具有可控制组成的Pt-Pd-Pb;这些合成的Pt基纳米多孔催化剂不仅具有显着高的表面积,而且对甲醇和甲酸的电化学氧化也显示出极好的电催化活性。其中,进一步测试了纳米多孔PtPb网络对葡萄糖的电氧化作用。伏安法和安培法结果表明,PtPb电极对增加的葡萄糖浓度具有强而敏感的电流响应,并且能够在中性介质中以出色的选择性检测葡萄糖。

著录项

  • 作者

    Wang, Jingpeng.;

  • 作者单位

    University of Guelph (Canada).;

  • 授予单位 University of Guelph (Canada).;
  • 学科 Chemistry Inorganic.;Physics Condensed Matter.;Chemistry Physical.
  • 学位 Ph.D.
  • 年度 2009
  • 页码 168 p.
  • 总页数 168
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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