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Effect of the Pd/MWCNTs anode catalysts preparation methods on their morphology and activity in a direct formic acid fuel cell

机译:Pd / MWCNTs阳极催化剂制备方法对其直接甲酸燃料电池的形貌和活性的影响

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摘要

Impact of Pd/MWCNTs catalysts preparation method on the catalysts morphology and activity in a formic acid electrooxidation reaction was investigated. Three reduction methods of Pd precursor involving reduction in a high pressure microwave reactor (Pdl), reduction with NaBH4 (Pd2) and microwave assisted polyol method (Pd3) were used in this paper. Crystallites size and morphology were studied using the scanning transmission electron microscopy (STEM), X-ray diffraction (XRD), whereas elemental composition, Pd chemical state and functional groups content by the X-ray photoelectron spectroscopy (XPS). The prepared catalysts were tested in a direct formic acid fuel cell (DFAFC) as an anode material. The catalytic activity was correlated with a mean fraction of the total Pd atoms exposed at the surface (FE). The value of FE was calculated from the crystallites size distribution determined by the STEM measurements. Non-linear dependence of a current density versus FE, approaching the maximum at FE approximate to 0.25 suggests that the catalytic process proceeded at Pd nanocrystallites faces, with inactive edges and corners. Pd2 catalyst exhibited highest activity due to its smallest Pd crystallites (3.2 nm), however the absence of Pd crystallites aggregation and low content of carbon in PdCx phase, i.e. x = 4 at.% may also affect the observed. (C) 2016 Elsevier B.V. All rights reserved.
机译:研究了Pd / MWCNTs催化剂制备方法对甲酸电氧化反应中催化剂形态和活性的影响。本文使用了三种还原Pd前体的方法,包括在高压微波反应器中还原(Pdl),用NaBH4还原(Pd2)和微波辅助多元醇法(Pd3)。使用扫描透射电子显微镜(STEM),X射线衍射(XRD)研究了微晶的尺寸和形态,而X射线光电子能谱(XPS)则研究了元素组成,Pd化学态和官能团含量。制备的催化剂在直接甲酸燃料电池(DFAFC)中作为阳极材料进行测试。催化活性与暴露在表面(FE)的总Pd原子的平均分数相关。由STEM测量确定的微晶尺寸分布计算出FE值。电流密度与FE的非线性相关性,在FE处接近最大值,接近0.25,表明催化过程在Pd纳米微晶的表面上进行,且边缘和拐角处于非活动状态。 Pd2催化剂由于其最小的Pd微晶(3.2 nm)而表现出最高的活性,但是PdCx相中不存在Pd微晶聚集和低碳含量,即x = 4 at。%也可能影响观察结果。 (C)2016 Elsevier B.V.保留所有权利。

著录项

  • 来源
    《Applied Surface Science》 |2016年第30期|929-937|共9页
  • 作者单位

    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland;

    Warsaw Univ Technol, Fac Chem & Proc Engn, Warynskiego 1, PL-00645 Warsaw, Poland;

    Warsaw Univ Technol, Fac Chem & Proc Engn, Warynskiego 1, PL-00645 Warsaw, Poland;

    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland|Warsaw Univ Technol, Fac Chem & Proc Engn, Warynskiego 1, PL-00645 Warsaw, Poland;

    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland;

    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland;

    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland;

    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland;

    Acad Sci Czech Republic, Inst Phys, Cukrovarnicka 10, Prague 16253 6, Czech Republic;

    Acad Sci Czech Republic, Inst Phys, Cukrovarnicka 10, Prague 16253 6, Czech Republic;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Electro-oxidation; DFAFC; Pd/MWCNTs; Preparation conditions; Reducing agents; Microwave conditions;

    机译:电氧化;DFAFC;Pd / MWCNTs;制备条件;还原剂;微波条件;

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