物理化学学报 >> 2011, Vol. 27 >> Issue (10): 2251-2254.doi: 10.3866/PKU.WHXB20111015

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CoPy/C催化剂应用碱性介质氧还原催化的电化学性能

徐莉1, 乔锦丽1, 丁蕾1, 胡隆宇1, 刘玲玲1, 王海江2   

  1. 1. 东华大学环境科学与工程学院, 上海 201620;
    2. 加拿大国家研究院, 燃料电池创新研究所, 温哥华 V6T 1W5
  • 收稿日期:2011-07-11 修回日期:2011-08-05 发布日期:2011-09-27
  • 通讯作者: 乔锦丽 E-mail:qiaojl@dhu.edu.cn
  • 基金资助:

    国家自然科学基金(21173039), 上海市浦江人才基金(08PJ14096), 上海市自然科学基金(09ZR1433300), 浙江省重中之重学科开放基金(20110927), 教育部归国留学人员基金(2009(1001))和上海市重点学科项目(B604)资助

Electrocatalytic Activity of CoPy/C Catalyst for the Oxygen Reduction Reaction in Alkaline Electrolyte

XU Li1, QIAO Jin-Li1, DING Lei1, HU Long-Yu1, LIU Ling-Ling1, WANG Hai-Jiang2   

  1. 1. College of Environmental Science and Engineering, Donghua University, Shanghai 201620, P. R. China;
    2. Institute for Fuel Cell Innovation, National Research Council Canada, Vancouver, B.C., V6T 1W5, Canada
  • Received:2011-07-11 Revised:2011-08-05 Published:2011-09-27
  • Contact: QIAO Jin-Li E-mail:qiaojl@dhu.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21173039), Pujiang Foundation of Shanghai, China (08PJ14096), Natural Science Foundation of Shanghai Science and Technology Committee, China (09ZR1433300), Opening Foundation of Zhejing Provincial Top Key Discipline, China (20110927), Scientific Research Foundation for the Returned Overseas Chinese Scholars, Ministry of Education of China (2009(1001)), and Shanghai Leading Academic Discipline Project Fund, China (B604).

摘要: 利用碳黑(Vulcan XC-72R)中加入硫酸钴和吡啶(Py)作为催化剂前驱体, 经溶剂分散热处理构建了一类新型的高效氧还原CoPy/C复合催化剂. 并运用循环伏安法(CV)和旋转圆盘电极(RDE)技术研究了不同Co含量的CoPy/C催化剂在碱性介质中对氧还原的电催化活性. 结果表明: Co的存在对氧的催化剂活性位的形成有重要影响, 800 °C下所制备的10%Co30%Py/C (质量分数)复合催化剂表现出最佳的氧还原催化活性. 以其制备的气体扩散电极在3.0 mol·L-1 KOH电解质溶液(O2气氛)中0.014 V (相对于标准氢电极(RHE))即可产生明显的氧还原电流. 同40%Py/C 相比, 10%Co30%Py/C 催化氧还原的起峰电位正移了71 mV, 同时表现出明显的极限扩散电流. 在-0.16 V时电流密度达到最大值, 电流密度为1.0 mA·cm-2, 半波电位在-0.07 V. 透射电镜分析表明所制备的碳黑载吡啶钴(10%Co30%Py/C)催化剂平均粒径为20 nm.

关键词: 碱性燃料电池, CoPy/C, 热处理, 氧还原反应, 循环伏安, 旋转圆盘电极

Abstract: In this communication, we report a novel CoPy/C catalyst for the oxygen reduction reaction (ORR) in alkaline electrolyte using cobalt sulfate heptahydrate (CoSO4·7H2O) and pyridine (Py) as the Co and N precursors supported on Vulcan XC-72R, followed by heat treatment in an inert atmosphere. Electrochemical performances were evaluated using cyclic voltammograms (CVs) and rotating disk electrode (RDE) technique in terms of its ORR activity as a function of Co content in the catalyst synthesis. Results show that the presence of Co in the CoPy/C catalyst greatly affects the formation of ORR catalytic active sites and that the best performing catalyst is 10%Co%30Py/C, which was synthesized at 800°C. In 3.0 mol·L-1 KOH, 10%Co30%Py/C (in O2) produces an obvious ORR current with an on-set potential at 0.014 V. Compared with the 40% Py/C the on-set potential of the 10% Co30% Py/C for oxygen reduction shifted positively by 71 mV (versus RHE (reversible hydrogen electrode)) and a well-defined limiting current plateau was achieved. Therefore, a maximum current density of 1.0 mA·cm-2 was obtained at -0.16 V with a half-wave potential of -0.07 V. Transmission electron microscopy (TEM) measurements show that the nanoparticles with a diameter of 20 nm are uniformly dispersed on Vulcan carbon (Vulcan XC-72R).

Key words: Alkaline fuel cell, CoPy/C, Heat treatment, Oxygen reduction reaction, Cyclic voltammogram, Rotating disk electrode

MSC2000: 

  • O646