氧化铁/氮掺杂碳纳米管催化剂的制备与氧还原性能研究

张颖, 李萍炜, 尹徐影, 赵斌

表面技术 ›› 2017, Vol. 46 ›› Issue (5) : 189-195.

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表面技术 ›› 2017, Vol. 46 ›› Issue (5) : 189-195. DOI: 10.16490/j.cnki.issn.1001-3660.2017.05.031
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氧化铁/氮掺杂碳纳米管催化剂的制备与氧还原性能研究

  • 张颖, 李萍炜, 尹徐影, 赵斌
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Preparation and Oxygen Reduction Reaction Performance of Iron Oxide/Nitrogen Doped Carbon Nanotube Catalyst

  • ZHANG Ying, LI Ping-wei, YIN Xu-ying, ZHAO Bin
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摘要

目的 探索非贵金属作为燃料电池阴极催化剂的氧还原性能。方法 采用磁控溅射的方法,在N2/Ar工作气氛中,将Fe溅射到碳纳米管阵列表面,同时将氮掺入样品中,然后在不同温度下退火制备氮掺杂碳纳米管负载氧化铁(Fe2O3/N-CNT)的氧还原催化剂。采用场发射扫描电镜、X射线衍射仪、X射线光电子能谱仪对样品的形貌、结构和成分进行分析。通过电化学测试研究样品的氧还原催化性能,并对样品的催化反应动力学进行研究。结果 退火温度对样品的形貌和氧还原催化性能具有显著影响,样品的氧还原催化活性随着退火温度的升高先增强后显著下降。其中450 ℃退火的样品表现出最佳的催化性能,该样品在0.1 mol/L KOH溶液中的起始电位和峰电位分别为0.715 V和0.6 V,电子转移数在3.3~3.6之间。结论 Fe2O3/N-CNT具有较好的氧还原催化活性,其中吡啶氮是可能的氧还原催化活性位点。实验中催化剂的制备方法简便且成本低廉,是一种有望替代Pt基贵金属的电催化材料。

Abstract

The work aims to explore oxygen reduction reaction (ORR) performance of non-noble metal as cathodic catalyst of fuel cell. Fe was sputtered on the surface of carbon nanotube (CNT) arrays in N2/Ar working atmosphere in the method of magnetron sputtering. Meanwhile, nitrogen was doped into the samples, then the samples were annealed at different temperature to prepare ORR catalysts for Fe2O3 supported on nitrogen-doped carbon nanotubes (Fe2O3/N-CNT). Scanning electron microscopy (SEM), X-ray diffractometer (XRD), and X-ray photoelectron spectroscopy (XPS) were employed to analyze morphology, structure and composition of the samples. And electrochemical test was conducted to study the ORR performance and catalytic kinetics of the samples. Annealing temperature had significant effects on morphology and ORR performance of the samples. ORR activity of the samples first increased, and then decreased significantly as the annealing temperature increased. The catalyst annealed at 450 ℃ exhibited the best catalytic performance with onset potential at 0.715 V, peak potential at 0.6 V and electron transfer number ranging within 3.3~3.6 in 0.1 mol/L KOH solution. The Fe2O3/N-CNT catalyst exhibits good oxygen reduction activity. Pyridinic-N is the possible active site of ORR in this catalyst. The feasible and inexpensive preparation method makes this electrocatalyst promising in replacing Pt-based noble metal.

关键词

氧还原;磁控溅射;碳纳米管;氧化铁;氮掺杂

Key words

oxygen reduction; magnetron sputtering; carbon nanotube; Fe2O3; nitrogen doping

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导出引用
张颖, 李萍炜, 尹徐影, 赵斌. 氧化铁/氮掺杂碳纳米管催化剂的制备与氧还原性能研究[J]. 表面技术. 2017, 46(5): 189-195
ZHANG Ying, LI Ping-wei, YIN Xu-ying, ZHAO Bin. Preparation and Oxygen Reduction Reaction Performance of Iron Oxide/Nitrogen Doped Carbon Nanotube Catalyst[J]. Surface Technology. 2017, 46(5): 189-195

基金

上海市自然科学基金(16ZR1423500)

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