物理化学学报 >> 2017, Vol. 33 >> Issue (7): 1429-1435.doi: 10.3866/PKU.WHXB201704131

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高分散钴氮共掺杂碳纳米纤维氧还原催化剂

周扬1,2,程庆庆2,黄庆红2,邹志青2,严六明1,杨辉2,*()   

  1. 1 上海大学理学院,上海200444
    2 中国科学院上海高等研究院,上海201210
  • 收稿日期:2017-02-20 发布日期:2017-05-31
  • 通讯作者: 杨辉 E-mail:yangh@sari.ac.cn
  • 基金资助:
    国家高技术研究发展计划(“863”计划)(2015AA043503);国家自然科学基金(21533005);国家自然科学基金(216673275)

Highly Dispersed Cobalt-Nitrogen Co-doped Carbon Nanofiber as Oxygen Reduction Reaction Catalyst

Yang ZHOU1,2,Qing-Qing CHENG2,Qing-Hong HUANG2,Zhi-Qing ZOU2,Liu-Ming YAN1,Hui YANG2,*()   

  1. 1 College of Sciences, Shanghai University, Shanghai 200444, P. R. China
    2 Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, P. R. China
  • Received:2017-02-20 Published:2017-05-31
  • Contact: Hui YANG E-mail:yangh@sari.ac.cn
  • Supported by:
    the National High-tech R&D Program(863 Program)(2015AA043503);the Nature Science Foundation of China(21533005);the Nature Science Foundation of China(216673275)

摘要:

过渡金属氮掺杂碳基催化剂已成为替代铂基氧还原反应(ORR)电催化剂的理想选择。本文通过静电纺丝技术制备了高比表面、高度分散的钴原子配位氮掺杂的碳纳米纤维催化剂(Co-N/C)。X射线衍射(XRD)和高分辨率透射电镜(HRTEM)结果证实Co元素高度分散于制备的Co-N/C催化剂中。X射线光电子能谱结果表明N元素主要以吡啶N和石墨N形式存在。该Co-N/C催化剂对ORR反应呈现出较高的电催化活性,其氧还原起始和半波电位分别为0.92 V和0.80 V(相对于标准氢电极),接近于商业化Pt/C催化剂的性能。以制备的Co-N/C催化剂作为阴极,25℃下锌空气燃料电池的开路电位1.54 V、最大功率密度达到了190 mV·cm-2表明该催化剂具有良好的应用前景。

关键词: 氧还原反应, 过渡金属-氮掺杂催化剂, 碳纳米纤维, 高分散, 静电纺丝

Abstract:

Transition metal-nitrogen doped carbon-based catalysts have become promising alternatives to precious metal catalysts for the oxygen reduction reaction (ORR). Here, we report a nitrogen-doped carbon nanofiber electrocatalyst coordinated with highly dispersed cobalt atoms (Co-N/C) with a high specific surface area prepared by an electrospinning method. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HR-TEM) results confirmed that Co was highly dispersed within the prepared Co-N/C catalyst. X-ray photoelectron spectroscopy for N 1s spectra showed that the N species mainly existed in the forms of pyridinic N and graphitic N. This Co-N/C catalyst exhibited considerable ORR performance with onset and half-wave potentials at 0.92 and 0.80 V (relative to the reversible hydrogen electrode (RHE)), which are comparable to those of commercial Pt/C. With the prepared Co-N/C catalyst as the cathode, a Zn-air battery displayed an open-circuit potential of 1.54 V and a peak power density of 190 mW·cm-2 at 25℃, which suggest a promising application.

Key words: Oxygen reduction reaction, Transition metal-nitrogen doped catalyst, Carbon nanofibers, Highly dispersed, Electrospinning