高等学校化学学报

高等学校化学学报 ›› 2011, Vol. 32 ›› Issue (10): 2371.

• 研究论文 • 上一篇    下一篇

金属酞菁类大环化合物对氧气还原反应催化行为的阻抗谱研究

马金福1, 柳永宁2   

  1. 1. 北方民族大学材料科学与工程学院, 银川 750021;
    2. 西安交通大学材料科学与工程学院, 西安 710049
  • 收稿日期:2010-10-22 修回日期:2011-03-29 出版日期:2011-10-10 发布日期:2011-09-11
  • 通讯作者: 马金福 E-mail:majf0870@163.com
  • 基金资助:

    国家民委、宁夏回族自治区省部共建“粉体材料与特种陶瓷”重点实验室项目(批准号: 200901)和宁夏回族自治区自然科学基金项目（批准号:  NZ11144）资助.

Electrochemical Impedance Spectroscopy Studies on Oxygen Reduction Reaction Catalysed by Macrocyclic  Metal Phthalocyanine Compounds

MA Jin-Fu1*, LIU Yong-Ning2   

  1. 1.  School of Materials Science and Engineering,  North University for Ethnics, Yinchuan 750021, China;
    2.  State Key Laboratory for Mechanical Behavior of Materials, Xi′an Jiaotong University, Xi′an 710049, China
  • Received:2010-10-22 Revised:2011-03-29 Online:2011-10-10 Published:2011-09-11
  • Contact: MA Jin-Fu E-mail:majf0870@163.com
  • Supported by:

    国家民委、宁夏回族自治区省部共建“粉体材料与特种陶瓷”重点实验室项目(批准号: 200901)和宁夏回族自治区自然科学基金项目（批准号:  NZ11144）资助.

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被引次数

12

摘要： 通过电化学交流阻抗法研究了3种金属酞菁类大环化合物(FePc, CoPc, FeCoPc2)在碱性溶液中对氧气还原反应(ORR)的电化学催化行为, 各电极的交流阻抗 Nyquist 图谱在高频区和低频区均呈现出2个较明显的半圆和半圆之间(中频区)的压扁的弧形, 采用Zsimpwin阻抗谱分析软件对-02 V(vs. Hg/HgO)电位下的各交流阻抗谱进行等效电路拟合, 提出空气电极ORR反应的等效电路, 并对等效电路中各动力学参数进行了解释, 通过分析得出金属酞菁在碱性溶液中对ORR催化反应是一个伴随中间产物HO-2的2电子转移过程. 同时, 等效电路的拟合结果表明,  FeCoPc2/C作为ORR催化剂对减小Rc+Rct效果比FePc/C和CoPc/C明显, 具有更高的催化活性.

关键词: 金属酞菁, 空气电极, 交流阻抗, 氧还原反应

Abstract: The oxygen reduction reaction(ORR) catalyzed by metal phthalocyanine macrocycles(FePc, CoPc, FeCoPc2) in alkaline solution was investigated by line sweep voltammograms(LSV) and electrochemical impedance spectroscopy(EIS). The results of these two methods have the same trend.  The characteristic of two semi-circles and an arc on the gas diffusion electrodes were presented on the EIS Nyquist plot, and the EIS curves at the potential -02 V(vs. Hg/HgO) were fitted by the equivalent circuit with analytical software Z simpwin. The result show that ORR on MPcs is an 2-electron transfer process with an intermediate product of HO-2.  The simulated kinetics data of the equivalent circuit was also analyzed.  Fitting results of equivalent circuit show that the FeCoPc2/C as ORR catalyst for reducing has higher catalytic activity because of lower Rc+Rct than that of FePc/C, CoPc/C.

Key words: Metal phthalocyanine; , Air electrode, AC impedance, Oxygen reduction reaction

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