高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (7): 1480-1487.doi: 10.7503/cjcu20190020

• 物理化学 • 上一篇    下一篇

高活性位点密度Fe-N共掺杂碳纳米片的制备及氧还原性能

殷雯婧1,2, 刘啸1,2, 钱汇东1, 邹志青1()   

  1. 1. 中国科学院上海高等研究院, 上海 201210
    2. 中国科学院大学, 北京 100049
  • 收稿日期:2019-01-09 出版日期:2019-07-10 发布日期:2019-07-12
  • 作者简介:邹志青, 男, 博士, 研究员, 主要从事纳米电催化和燃料电池研究. E-mail: zouzq@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, 21872165)资助.

Preparation and Oxygen Reduction Performance of Fe, N co-Doped arbon Nanoplate with High Density of Active Sites

YIN Wenjing1,2, LIU Xiao1,2, QIAN Huidong1, ZOU Zhiqing1,*()   

  1. 1. Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China
    2. University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2019-01-09 Online:2019-07-10 Published:2019-07-12
  • Contact: ZOU Zhiqing E-mail:zouzq@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, 21872165).

摘要:

从三聚氰胺和均苯四甲酸酐单体出发, 通过熔融盐法合成了三嗪结构聚酰亚胺纳米片, 借助类石墨相氮化碳(g-C3N4)与铁离子的配位作用, 经高温热处理形成了高效掺杂的Fe-N/C催化剂. 研究结果表明, 该催化剂为表面粗糙的纳米片结构, 比表面积高达1794 m2/g. 通过g-C3N4的引入和含量的调控, 催化剂中铁元素的掺杂量最高可达1.13%(摩尔分数), 为未引入g-C3N4的3.3倍, 其原因可归结于g-C3N4配位锚定了铁离子, 其较强的配位作用可以避免高温热处理时铁元素的迁移和聚集. 该催化剂在酸性条件下氧还原反应半波电位为0.79 V, 10000周加速测试后的半波电位衰减了30 mV, 表现出较好的氧还原活性.

关键词: 非贵金属催化剂, 氧还原反应, 类石墨相氮化碳, 配位作用, 聚酰亚胺

Abstract:

Fe, N co-doped carbon nanoplate catalyst with high active sites was developed via methods of polymerization of triazine polyimide and carbonization within melting salt of ZnCl2/KCl with the aid of g-C3N4 to anchor Fe3+. The as-prepared NPT-C3N4-0.5 catalyst displays high specific surface area of 1794 m2/g. The iron atoms uniformly distribute in the carbon skeleton with an increased doping amount up to the molar percentage of 1.13%, 3.3 times of the one without g-C3N4, which can be attributed to the coordination between g-C3N4 and iron to decrease its aggregation under high temperature. The catalyst exhibits excellent catalytic activity for oxygen reduction reaction(ORR) in acid media. Typically, the half-wave potential(E1/2) of the catalyst can reach up to 0.79 V(vs. RHE) and only decreases by 30 mV after 10000 potential cycles of accelerated durability test in acid media, showing high activity towards ORR.

Key words: Non-precious metal catalyst, Oxygen reduction reaction, Graphitic carbon nitride, Coordination, Polyimide

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