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Selectivity of Mixed Iron-Cobalt Spinels Deposited on a NS-Doped Mesoporous Carbon Support in the Oxygen Reduction Reaction in Alkaline Media

机译:碱性介质氧还原反应中沉积在NS掺杂的介孔碳载体上的混合铁 - 钴尖晶石的选择性

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摘要

One of the practical efforts in the development of oxygen reduction reaction (ORR) catalysts applicable to fuel cells and metal-air batteries is focused on reducing the cost of the catalysts production. Herein, we have examined the ORR performance of cheap, non-noble metal based catalysts comprised of nanosized mixed Fe-Co spinels deposited on N,S-doped mesoporous carbon support (N,S-MPC). The effect of the chemical and phase composition of the active phase on the selectivity of catalysts in the ORR process in alkaline media was elucidated by changing the iron content. The synthesized materials were thoroughly characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), and Raman spectroscopy (RS). Detailed S/TEM/EDX and Raman analysis of the phase composition of the synthesized ORR catalysts revealed that the dominant mixed iron-cobalt spinel is accompanied by minor fractions of bare cobalt and highly dispersed spurious iron oxides (Fe2O3 and Fe3O4). The contribution of individual phases and their degree of agglomeration on the carbon support directly influence the selectivity of the obtained catalysts. It was found that the mixed iron-cobalt spinel single phase gives rise to significant improvement of the catalyst selectivity towards the desired 4e− reaction pathway, in comparison to the reference bare cobalt spinel, whereas spurious iron oxides play a negative role for the catalyst selectivity.
机译:应用于燃料电池和金属电池的氧还原反应(ORR)催化剂的发展之一集中于降低催化剂生产的成本。在此,我们研究了由沉积在N,S掺杂的介孔碳载体(N,S-MPC)上的纳米化混合Fe-Co尖晶石组成的廉价非贵金属基催化剂的ORR性能。通过改变铁含量,阐明了活性相对活性相对活性相对碱培养基中的催化剂中催化剂的选择性的影响。通过透射电子显微镜(TEM),X射线衍射(XRD)和拉曼光谱(RS)进行彻底表征合成材料。详细的S / TEM / EDX和RAMAN分析合成的ORR催化剂的相组合物揭示了优势混合铁 - 钴尖晶石伴随着裸钴和高度分散的寄生铁氧化物(Fe2O3和Fe3O4)的少量逐渐分数。个体阶段的贡献及其在碳载体上的凝聚程度直接影响所得催化剂的选择性。结果发现,与参考裸钴尖晶石相比,混合铁 - 钴尖晶石单相使催化剂选择性对所需的4E-反应途径的显着改善,而寄生铁氧化物对催化剂选择性起作用的负面作用。

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