高等学校化学学报

高等学校化学学报 ›› 2011, Vol. 32 ›› Issue (2): 344.

• 研究论文 • 上一篇    下一篇

高温热裂解Ketjen Black EC 300J碳黑负载钴卟啉的氧还原性能

章虹,任奇志,何盛一,王庆宇,蒋宗润   

  1. 上海交通大学化学化工学院, 上海 200240
  • 收稿日期:2010-06-21 修回日期:2010-10-19 出版日期:2010-02-10 发布日期:2011-02-23
  • 通讯作者: 任奇志 E-mail:qzren@sjtu.edu.cn
  • 基金资助:

    国家自然科学基金(批准号: 20871082, 20471037)资助.

High-temperature Pyrolysis of Ketjen Black EC 300J Supported Cobalt Porphyrin Complexes as Electrocatalysis for Oxygen Reduction

ZHANG Hong, REN Qi-Zhi*,  HE Sheng-Yi, WANG Qing-Yu,  JIANG Zong-Run   

  1. School of Chemistry and Chemical Engineering, Shanghai Jiaotong University, Shanghai 200240, China
  • Received:2010-06-21 Revised:2010-10-19 Online:2010-02-10 Published:2011-02-23
  • Contact: REN Qi-Zhi E-mail:qzren@sjtu.edu.cn
  • Supported by:

    国家自然科学基金(批准号: 20871082, 20471037)资助.

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被引次数

6

摘要： 选用具有高介孔面积和导电性能的碳黑Ketjen Black EC 300J (简称KB) 作为载体，制备了碳黑负载钴卟啉(CoTMPP/KB)，经过900 ℃热处理后得到电催化剂，用于燃料电池阴极氧还原反应. 利用循环伏安法 (CV) 研究了碳载体不同预处理方法以及高温热处理对催化剂的氧还原催化性能影响. 结果表明，6 mol?L-1 HNO3 预处理步骤可以很好地改善KB性能，碳黑负载钴卟啉经过900 ℃ 热处理后，虽然钴卟啉的结构发生了裂解，催化剂具有较好的氧还原催化性能，阴极峰值电位 (Ep) 及最大电容电流 (Ip) 均为最佳. 采用IR、XRD、TEM和氮吸附/脱附等物理测试手段对KB碳黑以及电催化剂表面性质及微观结构进行了分析，经6 mol?L-1 HNO3 预处理的KB碳黑表面羟基 (-OH) 等含氧基团增多，团聚不明显, 平均粒径约30 nm；孔结构主要由孔径分布较窄的中孔组成，是一种较好的电催化剂载体；经900℃ 热处理后，电催化剂结构中有 CoC3 (101) 和金属态 Co(111) 结构出现，钴离子在碳黑表面的分散较好，平均孔径 8.2 nm，比表面积为463.4 m2?g-1.

关键词: Ketjen Black EC 300J, CoTMPP/KB, 预处理, 热处理, 循环伏安, 氧还原

Abstract: Carbon black EC 300J (KB) with high mesoporous area and electrical conductivity was used as support for cobalt tetramethoxyphenylporphyrin (CoTMPP) to prepare the cathode electrocatalysts (CoTMPP/KB) for the oxygen reduction in proton exchange membrane fuel cell (PEMFC). The influence of chemical pretreatment of carbon black supports and 900 ℃ heat-treating of the electrocatalysts on the electrocatalytic activities for oxygen reduction of CoTMPP/KB were investigated by cyclic voltammogram (CV). Results show that with 6 mol?L-1 HNO3 pretreatment of carbon support and 900 ℃ heat-treatment of the catalyst, although the pyrolysis occurred for the CoTMPP structure, the electrocatalyst shows the best catalytic performance for oxygen reduction, both the cathodic peak potential ( Ep ) and the maximum capacitive current ( Ip ) have been improved. The surface properties and the microstructures of both the carbon black KB and the electrocatalyst have been investigated by IR, XRD, TEM and nitrogen adsorption/desorption. After the pretreatment with 6 mol?L-1 HNO3, the concentration of hydroxyl group and other oxygen-groups has been increased on KB surface and no obvious particle aggregation of KB has been observed, an average particle size of about 30 nm of KB has been observed; The pore structure of the catalysts is mainly composed of mesopores and has a narrow pore size distribution, which prove CoTMPP/KB to be a good electrocatalyst; CoC3 (101) and metallic Co(111) have been formed in the catalyst after 900 ℃ heat-treatment, and the cobalt ions have been well dispersed in the carbon black surface, with mean pore size of 8.2 nm and surface area of 463.4 m2?g-1.

Key words: Ketjen Black EC 300J, CoTMPP/KB, Pretreatment, Heat-treatment, CV, Oxygen reduction

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