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首页> 外文期刊>Journal of the American Chemical Society >Phenylenediamine-Based FeN_x/C Catalyst with High Activity for Oxygen Reduction in Acid Medium and Its Active-Site Probing
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Phenylenediamine-Based FeN_x/C Catalyst with High Activity for Oxygen Reduction in Acid Medium and Its Active-Site Probing

机译：在酸性介质中具有高氧还原活性的苯二胺基FeN_x / C催化剂及其活性位探测

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摘要

High-temperature pyrolyzed FeN_x/C catalyst is one of the most promising nonprecious metal electrocatalysts for oxygen reduction reaction (ORR). However, it suffers from two challenging problems: insufficient ORR activity and unclear active site structure. Herein, we report a FeN_x/C catalyst derived from poly-m-phenylenediamine (PmPDA-FeN_x/C) that possesses high ORR activity (11.5 A g~(-1) at 0.80 V vs RHE) and low H_2O_2 yield (＜1%) in acid medium. The PmPDA-FeN_x/C also exhibits high catalytic activity for both reduction and oxidation of H_2O_2. We further find that the ORR activity of PmPDA-FeN_x/C is not sensitive to CO and NO_x but can be suppressed significantly by halide ions (e.g., Cl~-, F~-, and Br~-) and low valence state sulfur-containing species (e.g., SCN~-, SO_2, and H_2S). This result reveals that the active sites of the FeN_x./C catalyst contains Fe element (mainly as Fe~Ⅲ at high potentials) in acid medium.
机译：高温热解FeN_x / C催化剂是氧还原反应（ORR）最有前途的非贵金属电催化剂之一。然而，它遭受两个挑战性的问题：ORR活性不足和活性位点结构不清楚。本文中，我们报道了一种由聚间苯二胺（PmPDA-FeN_x / C）衍生的FeN_x / C催化剂，该催化剂具有较高的ORR活性（相对于RHE在0.80 V时为11.5 A g〜（-1））和低H_2O_2收率（＜1 ％）在酸性介质中。 PmPDA-FeN_x / C对H_2O_2的还原和氧化也显示出高催化活性。我们进一步发现，PmPDA-FeN_x / C的ORR活性对CO和NO_x不敏感，但可以被卤离子（例如Cl〜-，F〜-和Br〜-）和低价态硫-显着抑制。含有物种（例如，SCN〜-，SO_2和H_2S）。结果表明，FeN_x。/ C催化剂的活性位在酸性介质中含有Fe元素（高电位时主要为Fe〜Ⅲ）。

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  • 来源
    《Journal of the American Chemical Society》 |2014年第31期|10882-10885|共4页
  • 作者

    Qiang Wang; Zhi-You Zhou; Yu-Jiao Lai; Yong You; Jian-Guo Liu; Xia-Ling Wu; Ephrem Terefe; Chi Chen; Lin Song; Muhammad Rauf; Na Tian; Shi-Gang Sun;

  • 作者单位

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    Eco-materials and Renewable Energy Research Center, Department of Materials Science and Engineering, and National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093, China;

    Eco-materials and Renewable Energy Research Center, Department of Materials Science and Engineering, and National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China,State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

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  • 入库时间 2022-08-18 03:11:08

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