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首页> 外文期刊>Carbon: An International Journal Sponsored by the American Carbon Society >Ordered mesoporous Fe (or Co)-N-graphitic carbons as excellent non-precious-metal electrocatalysts for oxygen reduction
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Ordered mesoporous Fe (or Co)-N-graphitic carbons as excellent non-precious-metal electrocatalysts for oxygen reduction

机译:有序介孔的Fe(或Co)-N-石墨碳是用于还原氧的优异非贵金属电催化剂

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Novel mesoporous Fe (or Co)-N_x-C non-precious-metal catalysts (NPMCs) have been fabricated by a simple nanocasting-pyrolysis method using 1,10-phenanthroline metal, chelates as the precursors. Owing to the ordered hexagonal mesostructures, appropriate surface area, large-pore channels, and well-distributed metal-Nx moieties embedded within the graphitic carbon backbones, the prepared metal-N_x-C materials exhibit excellent catalytic activity for oxygen reduction reaction (ORR) in both alkaline and acidic media. The prepared Fe-N_x-C materials, when prepared with an optimized catalyst loading on the electrode, exhibit more positive ORR onset-potential and half-wave potential (E_(1/2)) than commercial Pt/C catalysts and the previously reported NPMCs in 0.1 M KOH electrolyte. They also have the comparable ORR onset-potential and current densities to Pt/C electrode in 0.1 M HCIO4 electrolyte. Moreover, ORR over mesoporous Fe-N_x-C was found to proceed by the direct four-electron mechanism with high selectivity in both electrolytes. The mesoporous Fe-N_x-C materials demonstrated higher ORR catalytic activity compared to the NPMCs made by alternative methods. Analysis of the catalytic behavior, structure and nature of surface species of N_x-C materials allows us to ascribe the origin of the excellent ORR catalytic activity of mesoporous Fe (or Co)-N_x-C in both electrolytes to Fe (or Co)-N_x moieties embedded within the graphitic carbon frameworks.
机译:新型介孔Fe(或Co)-N_x-C非贵金属催化剂(NPMC)是通过简单的纳米浇铸-热解法,以1,10-菲咯啉金属螯合物为前体制备的。由于有序的六角形介孔结构,适当的表面积,大孔通道以及分布在石墨碳骨架内的分布良好的金属-Nx部分,所制备的金属-N_x-C材料对氧还原反应(ORR)表现出优异的催化活性。在碱性和酸性介质中。所制备的Fe-N_x-C材料在电极上负载优化催化剂的情况下,比市售Pt / C催化剂和先前报道的材料具有更强的ORR起始电势和半波电势(E_(1/2))。 NPMC在0.1 M KOH电解液中。它们还具有与0.1 M HCIO4电解质中的Pt / C电极相当的ORR起始电位和电流密度。此外,发现在介孔Fe-N_x-C上的ORR通过直接四电子机理在两种电解质中均具有高选择性地进行。与通过替代方法制得的NPMC相比,中孔Fe-N_x-C材料显示出更高的ORR催化活性。对N_x-C材料的表面物种的催化行为,结构和性质的分析使我们能够将中孔Fe(或Co)-N_x-C在两种电解质中对Fe(或Co)-的优异ORR催化活性的起源归因于N_x部分嵌入石墨碳框架中。

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