高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (11): 2492-2499.doi: 10.7503/cjcu20180459

• 物理化学 • 上一篇    下一篇

包覆氮化铁的Fe, N掺杂碳纳米纤维的制备及对氧还原反应的催化性能

刘培1,2,3, 程庆庆1,3, 陈驰1, 邹亮亮1, 邹志青1, 杨辉1,2()   

  1. 1. 中国科学院上海高等研究院, 上海 201210
    2. 上海科技大学物质科学与技术学院, 上海 201210
    3. 中国科学院大学, 北京 100039
  • 收稿日期:2018-06-26 出版日期:2018-11-10 发布日期:2018-08-31
  • 作者简介:联系人简介: 杨 辉, 男, 博士, 研究员, 主要从事燃料电池和液流电池等研究. E-mail: yangh@sari.ac.cn
  • 基金资助:
    国家重点研究发展计划项目(批准号: 2017YFA0206500)和国家自然科学基金(批准号: 21673275, 21533005)资助.

Preparation and Oxygen Reduction Reaction Catalytic Performance of Fe, N Co-doped Carbon Nanofibers with Encapsulated Iron Nitride

LIU Pei1,2,3, CHENG Qingqing1,3, CHEN Chi1, ZOU Liangliang1, ZOU Zhiqing1, YANG Hui1,2,*()   

  1. 1. Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China
    2. School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
    3. University of Chinese Academy of Sciences, Beijing 100039, China
  • Received:2018-06-26 Online:2018-11-10 Published:2018-08-31
  • Contact: YANG Hui E-mail:yangh@sari.ac.cn
  • Supported by:
    † Supported by the National Key Research and Development Program of China(No. 2017YFA0206500) and the National Natural Science Foundation of China(Nos.21673275, 21533005).

摘要:

通过静电纺丝、 碳化和氨气刻蚀制备了具有核-壳结构的包覆氮化铁(FexN)纳米颗粒的Fe, N共掺杂多孔碳纳米纤维(FexN@Fe-N-C), 并研究了其在酸性和碱性介质中对氧还原反应(ORR)的电催化性能. 结果表明, 该催化剂具有优异的氧还原催化活性, 在酸性介质中的半波电位(E1/2)可达0.81 V(vs. RHE), 在碱性条件下的E1/2高达0.897 V, 高于商业Pt/C催化剂. 在酸性介质中经过10000周加速衰减测试后, FexN@Fe-N-C的E1/2仅衰减了26 mV, 展示出极佳的耐久性. 离子探针和浓酸刻蚀实验结果表明, Fe-Nx以及FexN纳米颗粒均对ORR有重要催化作用.

关键词: Fe-N-C, 氮化铁, 氧还原反应, 碳纳米纤维, 氨气刻蚀

Abstract:

Fe, N co-doped porous carbon nanofibers with iron nitride(FexN) nanoparticles encapsulated in Fe, N co-doped carbon shell(FexN@Fe-N-C) were preparated through electrospinning, carbonization and NH3-etching. The FexN@Fe-N-C catalyst exhibits excellent catalytic activity for oxygen reduction reaction(ORR) in both acid and alkaline media. The half-wave potential(E1/2) in acidic medium can reach to 0.81 V(vs. RHE), while the E1/2 in alkaline medium is 0.897 V(vs. RHE), which is even higher than that of commercial Pt/C catalyst. After 10000 cycles of accelerated durability test in acid media, the E1/2 only decreases by 26 mV, demonstrating the excellent durability of FexN@Fe-N-C. Ion probing and acid-etching experiments indicate that both Fe-Nx sites and FexN nanoparticles contribute to the ORR activity.

Key words: Fe-N-C, Iron nitride, Oxygen reduction reaction(ORR), Carbon nanofibers, NH3-etching

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