催化学报

催化学报 ›› 2016, Vol. 37 ›› Issue (7): 1103-1108.DOI: 10.1016/S1872-2067(16)62471-3

• 论文 • 上一篇    下一篇

介孔结构Fe/N/C作为质子交换膜燃料电池氧还原催化剂

石尉a, 王宇成a, 陈驰a,b, 杨晓冬a, 周志有a, 孙世刚a   

  1. a. 厦门大学化学化工学院, 能源材料化学创新中心, 固体表面物理化学国家重点实验室, 福建 厦门 361005;
    b. 华东理工大学化学工程国家重点实验室, 上海 200237
  • 收稿日期:2016-04-17 修回日期:2016-05-11 出版日期:2016-06-17 发布日期:2016-06-17
  • 通讯作者: Xiao-Dong Yang, Zhi-You Zhou
  • 基金资助:

    国家重点基础研究发展计划(973计划,2015CB932300);国家自然科学基金(21373175,21321062,21361140374);中央高校基本科研业务费专项资金(20720150109).

A mesoporous Fe/N/C ORR catalyst for polymer electrolyte membrane fuel cells

Wei Shia, Yu-Cheng Wanga, Chi Chena,b, Xiao-Dong Yanga, Zhi-You Zhoua, Shi-Gang Suna   

  1. a. State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China;
    b. State Key Laboratory of Chemical Engineering, College of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
  • Received:2016-04-17 Revised:2016-05-11 Online:2016-06-17 Published:2016-06-17
  • Contact: Xiao-Dong Yang, Zhi-You Zhou
  • Supported by:

    This work was supported by the National Basic Research Program of Chain (973 Program, 2015CB932300), the National Natural Science Foundation of China (21373175, 21321062, 21361140374), and Fundamental Research Funds for the Central Universities (20720150109).

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摘要：

燃料电池具有高效、低排放等优势,非常有希望作为未来电动汽车的能源转化装置.目前,燃料电池的商业化受制于昂贵的铂基催化剂,特别是动力学迟缓的阴极氧还原反应(ORR)铂催化剂.Fe/N/C被认为是最有潜力的ORR非贵金属催化剂,但其活性仍远低于Pt催化剂,必须依靠增加载量来弥补其与Pt催化剂的活性差距.然而,较厚的催化层(~100mm)会降低阴极传质速率.因此,改善Fe/N/C阴极的传质是提高电池性能的重要途径.本文选择高N含量的2-氨基苯并咪唑(ABI)为氮源,通过水热聚合包覆在碳黑表面,然后掺入FeCl3,经高温热解/酸洗制备了Fe/N/C-ABI催化剂,并与基于间苯二胺的微孔型Fe/N/C催化剂(Fe/N/C-PmPDA)进行比较.Ar等温吸附-脱附结果表明,Fe/N/C-ABI催化剂具有较高的比表面积(662m2/g)和丰富的双级孔结构(微孔和介孔);透射电镜表征显示Fe/N/C-ABI催化剂具有中空结构,介孔孔径大约为10-25nm.而Fe/N/C-PmPDA催化剂具有相当的比表面积(656m2/g),但以微孔为主,基本不含介孔.旋转环圆盘电极(RRDE)测试表明,在0.1mol/LH2SO4溶液中,Fe/N/C-ABI催化剂的起始还原电位为0.92V,在0.8V电位下质量电流密度可达9.21A/g;而Fe/N/C-PmPDA催化剂具有相近的起始电位,但具有更高的催化活性,质量电流密度为13.4A/g.氢氧燃料电池(PEMFC)系统测试结果表明,Fe/N/C-ABI催化剂在1个背压和80℃测试条件下的最大功率密度达710mW/cm2,高于Fe/N/C-PmPDA催化剂(616mW/cm2).燃料电池与RRDE测试活性顺序的差异归结于Fe/N/C-ABI的中空球状结构.PEMFC工作时阴极会产生大量的水,很容易堵塞氧气传输通道.Fe/N/C-ABI的介孔结构可以作为水的产生和排除的缓存空间,也有利于提高O2传质,从而提高燃料电池性能.本文为具有高传质速率的Fe/N/C催化剂研制提供了一种新思路.

关键词: 铁/氮/碳催化剂, 非铂催化剂, 氧还原, 介孔, 空壳结构

Abstract:

Fe/N/C is a promising non-platinum catalyst for the oxygen reduction reaction (ORR). Even so, mass transfer remains a challenge in the application of Fe/N/C to proton exchange membrane fuel cells, due to the high catalyst loadings required. In the present work, mesoporous Fe/N/C was synthesized through heat treatment of KJ600 carbon black coated with poly-2-aminobenzimidazole and FeCl3. The as-prepared Fe/N/C possesses a unique hollow-shell structure that contains a buffer zone allowing both water formation and vaporization, and also facilitates the mass transfer of gaseous oxygen. This catalyst generated an oxygen reduction reaction activity of 9.21 A/g in conjunction with a peak power density of 0.71 W/cm2.

Key words: Fe/N/C catalyst, Non-platinum catalyst, Oxygen reduction reaction, Mesopore, Hollow-shell structure