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首页> 外文期刊>Chemistry: A European journal >Efficient Synthesis of Nitrogen- and Sulfur-co-Doped Ketjenblack with a Single-Source Precursor for Enhancing Oxygen Reduction Reaction Activity
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Efficient Synthesis of Nitrogen- and Sulfur-co-Doped Ketjenblack with a Single-Source Precursor for Enhancing Oxygen Reduction Reaction Activity

机译：高效合成氮气和硫 - 共掺杂Ketjenblack的单源前体，用于增强氧还原反应活性

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摘要

Promoting the oxygen reduction reaction (ORR) catalytic activities of cost-effective catalysts is of great significance for the development of various energy conversion and storage systems. Herein, we describe the preparation of a highly active N- and S-co-doped ketjenblack (Kb) by facile pyrolysis of a mixture of thiourea and Kb in the presence of FeCl_3·6H_2O followed by an acid-leaching process. This novel synthetic approach was rationally designed with the consideration that thiourea could easily introduce both N and S heteroatoms into the carbon matrix by a heat-treatment method by releasing plentiful reactive N- and S-containing gases, which could simultaneously optimize the porous structure of the resultant catalyst. Physical characterization revealed that N and S were homogeneously incorporated into the nanostructure of Kb and formed a hierarchical porous structure with a high specific surface area. The N/SKb catalyst showed impressive ORR activity, with an onset potential of 0.08 V at 0.1 mAcm~(-2), which is 20 mV more positive than that of commercial 20 wt.% Pt/C catalyst. This was coupled with long-term durability and superior methanol tolerance in alkaline media. The improved ORR performance can be mainly ascribed to synergistic contributions of highly efficient active sites arising from high contents of thiophene S and pyridinic N along with the high specific surface area and the favorable mass-transport properties arising from the hierarchical porous structure. The remarkable ORR performance and facile preparation method make the N/S-Kb catalyst a promising substitute for Pt in electrochemical energy devices.
机译：促进氧还原反应（ORR）成本效应催化剂的催化活性对于各种能量转换和储存系统的开发具有重要意义。在此，我们通过在FECL_3·6H_2O之后的硫脲和Kb的混合物中，通过容易地热解[3H_2O后，描述高活性N-和S-掺杂的Ketjenblack（Kb）的制备，然后是酸浸出方法。这种新颖的合成方法是合理设计的，考虑到硫脲可以通过热处理方法通过释放丰富的反应性的N-和S的气体容易地将N和S杂原子易于通过热处理方法引入碳基质中，这可以同时优化多孔结构所得催化剂。物理表征显示N和S均匀地掺入KB的纳米结构中，并形成具有高比表面积的分层多孔结构。 N / SKB催化剂显示出令人印象深刻的ORR活性，发病潜力为0.08V，0.1mmm〜（-2），其比商业20重量％的20mV更阳性。％Pt / C催化剂。这与碱性介质中的长期耐久性和优异的甲醇耐受性相结合。改善的ORR性能主要归因于从噻吩S和吡啶N的高含量和吡啶N的高含量以及高比表面积以及由等级多孔结构产生的有利的大规模转运性能的协同贡献。显着的ORR性能和容易制备方法使N / S-KB催化剂成为电化学能量装置中PT的有望替代品。

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  • 来源
    《Chemistry: A European journal》 |2017年第15期|共9页
  • 作者

    Guang-Chun Cheng; Guang-Lan Li; Cai-Di Liu; Li-Fang Yuan; Wen-Wen Chen; Ce Hao;

  • 作者单位

    State Key Laboratory of Fine Chemicals Institution Dalian University of Technology Panjin 124221 (P.R. China);

    State Key Laboratory of Fine Chemicals Institution Dalian University of Technology Panjin 124221 (P.R. China);

    State Key Laboratory of Fine Chemicals Institution Dalian University of Technology Panjin 124221 (P.R. China);

    State Key Laboratory of Fine Chemicals Institution Dalian University of Technology Panjin 124221 (P.R. China);

    State Key Laboratory of Fine Chemicals Institution Dalian University of Technology Panjin 124221 (P.R. China);

    State Key Laboratory of Fine Chemicals Institution Dalian University of Technology Panjin 124221 (P.R. China);

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 应用化学;
  • 关键词

    carbon; doping; electrochemistry; oxygen reduction reactions; three-dimensional porous structures;

    机译：碳;掺杂;电化学;氧还原反应;三维多孔结构;

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