高等学校化学学报 ›› 2013, Vol. 34 ›› Issue (4): 800-805.doi: 10.7503/cjcu20120658

• 研究论文: 无机化学 • 上一篇    下一篇

氮掺杂石墨烯的制备及氧还原电催化性能

李静, 王贤保, 杨佳, 杨旭宇, 万丽   

  1. 湖北大学材料科学与工程学院, 教育部功能材料的绿色制备与应用重点实验室, 武汉 430062
  • 收稿日期:2012-07-12 出版日期:2013-04-10 发布日期:2013-03-18
  • 通讯作者: 王贤保,男,博士,教授,博士生导师,主要从事碳纳米材料及其复合材料的可控制备、性能及应用研究.E-mail:wxb@hubu.edu.cn E-mail:wxb@hubu.edu.cn
  • 基金资助:

    国家自然科学基金(批准号:51272071)、高等学校博士学科点专项基金(博导类)(批准号:20114208110005)、湖北省教育厅项目(批准号:D20111002,B20111802)和武汉市学科带头人计划(批准号:201271130447)资助.

Synthesis of Nitrogen-doped Graphene and Its Electrocatalytic Performance Toward Oxygen Reduction Reaction

LI Jing, WANG Xian-Bao, YANG Jia, YANG Xu-Yu, WAN Li   

  1. Faculty of Materials Science and Engineering, Key Laboratory for the Synthesis and Application of Organic Functional Molecules, Ministry of Education, Hubei University, Wuhan 430062, China
  • Received:2012-07-12 Online:2013-04-10 Published:2013-03-18

摘要:

采用两步热解法, 用尿素掺杂氧化石墨烯(GO)得到N掺杂的还原氧化石墨烯(N-RGO), 通过控制反应温度, 制备了具有不同电催化活性的N掺杂的还原氧化石墨烯. 透射电子显微镜(TEM)和扫描电子显微镜(SEM)结果显示, 制得的氮掺杂石墨烯(nG)表面褶皱和重叠增加. X射线光电子能谱(XPS)证明, 氮元素以吡啶N、 吡咯N和石墨化的N 3种形式掺杂在石墨烯中, 最高摩尔分数为6.6%. 通过循环伏安(CV)和旋转圆盘电极(RDE)测试了nG的电化学性能, 结果表明, 在酸性电解质中对氧还原(ORR)有较高的催化活性, 起始电位在0.1 V左右, 电催化还原氧气时主要为四电子反应, 且相对商用的Pt/C催化剂有更好的电化学稳定性, 其中第一步热解温度为200℃制得的nG催化性能最好.

关键词: N掺杂石墨烯, 尿素, 热解, 氧还原反应, 电催化剂

Abstract:

A series nGs with different electrocatalytic abilities toward oxygen reduction reaction(ORR) was prepared via a two-steps pyrolysis method by controlling the reaction temperature on the physical mixture of graphene oxideand urea. Transmission electron microscopy and scanning electron microscopy display nG with highly wrinkled and overlapping structures. X-ray photoelectron spectroscopy shows that nitrogen is successfu-lly doped in graphene with the formation of pyridinic N, pyrrolic N and graphitic N, and the maximum nitrogen content is 6.6%(molar fraction). Cyclic voltammogram and rotating disk electrode measurement show that nGs exhibit high electrocatalytic activity with an onset potential of 0.1 V in an acid electrolyte. Moreover, the nGs catalyzed oxygen reduction revealed a favorable formation of water via a four-electron pathway and excellent stability over Pt/C catalyst. Furthermore, the nG obtained at 200 ℃ in the first pyrolysis step displays the best catalytic perfor-mance.

Key words: Nitrogen-doped graphene, Urea, Pyrolysis, Oxygen reduction reaction, Electrocatalyst

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