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Bimetallic M/N/C catalysts prepared from pi-expanded metal salen precursors toward an efficient oxygen reduction reaction

机译:双金属M / N / C催化剂由PI-膨胀金属盐盐前体制备朝向有效的氧还原反应

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摘要

Nonprecious metal electrocatalysts are being explored as alternatives to platinum-groupmetal electrocatalysts for the oxygen reduction reaction (ORR) which is required for cathode materials in fuel cells. Herein, we describe a new method for preparing bimetallic nitrogen-containing carbon catalysts with high ORR activity using p-expanded M(salen) precursors. The M/N/C and bimetallic FeM/N/C ORR catalysts were obtained by pyrolysis of a mixture of a carbon support (Vulcan XC-72R) and the metal complex as a precursor. The bimetallic FeCu catalyst prepared from Fe and Cu complexes with the N,N'-bis(2-hydroxy-1-naphthylidene)- 1,2-phenylenediamine ligand (2NAPD) is found to have an onset potential of 0.87 V, which is positively shifted by 50 mV from that of the catalyst prepared from the monometallic Fe(2NAPD) complex. The FeCu/N/C catalyst promotes efficient four-electron reduction in the ORR. High-resolution transmission electron microscopy studies reveal that both Fe and Cu metals together with pyridinic nitrogen species are highly dispersed within the carbonaceous structure in FeCu/2NAPD@VC, suggesting that the N-coordinated Fe and Cu sites promote efficient four-electron reduction of O-2. This new methodology facilitates design of nonprecious bimetallic carbon catalysts with excellent ORR activity.
机译:非普烈的金属电催化剂正在探索作为铂 - 血液催化剂的替代品,用于氧气还原反应(ORR),其在燃料电池中的阴极材料所需的氧气还原反应。在此,我们描述了使用P-膨胀的M(Salen)前体制备具有高ORR活性的二金属氮碳催化剂的新方法。通过碳载体(Vulcan XC-72R)和金属络合物作为前体的混合物热解获得M / N / C和Bimetallic FEM / N / C ORR催化剂。发现由Fe和Cu络合物制备的二硫化性FECU催化剂与N,N'-BIS(2-羟基-1-萘二甲基) - 1,2-苯二胺配体(2NAPD)的起始潜力为0.87V,即从由单金属Fe(2NAPD)复合物制备的催化剂的催化剂正偏移50mV。 FECU / N / C催化剂促进ORR中有效的四电子减少。高分辨透射电子显微镜的研究表明,与吡啶氮物种两者的Fe和Cu金属一起被高度分散于FECU / 2NAPD @ VC含碳结构内,这表明在N协调Fe和Cu位促进有效的四电子还原O-2。这种新方法有助于设计具有优异的ORR活性的非普烈双金属碳催化剂。

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  • 来源
    《RSC Advances》 |2018年第6期|共8页
  • 作者单位

    Osaka Univ Grad Sch Engn Dept Appl Chem 2-1 Yamadaoka Suita Osaka 5650871 Japan;

    Osaka Univ Grad Sch Engn Dept Appl Chem 2-1 Yamadaoka Suita Osaka 5650871 Japan;

    Osaka Univ Grad Sch Engn Dept Appl Chem 2-1 Yamadaoka Suita Osaka 5650871 Japan;

    Osaka Univ Grad Sch Engn Dept Appl Chem 2-1 Yamadaoka Suita Osaka 5650871 Japan;

    Osaka Univ Res Ctr Ultra High Voltage Electron Microscopy Ibaraki 5670047 Japan;

    Osaka Univ Res Ctr Ultra High Voltage Electron Microscopy Ibaraki 5670047 Japan;

    Osaka Univ Grad Sch Engn Dept Appl Chem 2-1 Yamadaoka Suita Osaka 5650871 Japan;

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  • 正文语种 eng
  • 中图分类 化学;
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