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Metal-free porous nitrogen-doped carbon nanotubes for enhanced oxygen reduction and evolution reactions

高活性的非金属多孔氮掺杂碳纳米管氧还原及析氧反应催化剂

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Science Bulletin

Abstract

Developing efficient metal-free bi-functional electrocatalysts is required to reduce costs and improve the slow oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics in electrochemical systems. Porous N-doped carbon nanotubes (NCNTs) were fabricated by KOH activation and pyrolysis of polypyrrole nanotubes. The NCNTs possessed a large surface area of more than 1,000 m2 g−1. NCNT electrocatalysts, particularly those annealed at 900 °C, exhibited excellent ORR electrocatalytic performance. Specifically, they yielded a more positive onset potential, higher current density, and long-term operation stability in alkaline media, when compared with a commercially available 20 wt% Pt/C catalyst. This resulted from the synergetic effect between the dominant pyridinic/graphitic-N species and the porous tube structures. The NCNT electrocatalyst also exhibited good performance for the OER. The metal-free porous nitrogen-doped carbon nanomaterials were prepared from low cost and environmentally friendly precursors. They are potential alternatives to Pt/C catalysts, for electrochemical energy conversion and storage.

摘要

电化学体系中的氧还原反应(ORR)和析氧反应(OER)受到反应动力学缓慢和催化剂成本昂贵的制约,成为了燃料电池性能和规模化应用的主要瓶颈。因此,研究开发廉价、高效的非金属双功能催化剂仍然是一项具有挑战性的工作。本文以聚吡咯纳米管为前驱体,通过氢氧化钾活化和高温煅烧,成功获得了比表面积高达1000 m2 g−1的氮掺杂多孔碳纳米管(NCNTs)。由于NCNTs中的高含量吡啶氮/石墨氮的催化活性作用,以及NCNTs中多孔结构和管状结构的共同作用,NCNTs,尤其是NCNT-900,在碱性体系中表现出优异的ORR和ORE活性。此外,NCNT-900还表现出良好的循环稳定性、高的耐甲醇和CO毒性。该氮掺杂的碳纳米电催化剂制备方法简单、成本低廉、性能优异,有望成为代替Pt/C的催化剂用于电化学能量的转换技术。

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Acknowledgments

This work was supported by the National Natural Science Foundation of China (51273008, 51473008), and the National Basic Research Program of China (2012CB933200).

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The authors declare that they have no conflict of interest.

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Correspondence to Xianyong Lu or Ying Zhu.

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Pan, T., Liu, H., Ren, G. et al. Metal-free porous nitrogen-doped carbon nanotubes for enhanced oxygen reduction and evolution reactions. Sci. Bull. 61, 889–896 (2016). https://doi.org/10.1007/s11434-016-1073-3

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  • DOI: https://doi.org/10.1007/s11434-016-1073-3

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