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作 者:徐莉[1] 乔锦丽[1] 丁蕾[1] 胡隆宇[1] 刘玲玲[1] 王海江
机构地区:[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V6T1W5
出 处:《物理化学学报》2011年第10期2251-2254,共4页Acta Physico-Chimica Sinica
基 金: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));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℃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(O_2气氛)中0.014 V(相对于标准氧电极(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.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℃. In 3.0 mol. L-1 KOH, 10%Co30%Py/C (in 02) 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).
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