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TDMNPPFe(Ⅱ)/C的制备及电催化氧还原性能研究
  • ISSN号:1002-087X
  • 期刊名称:电源技术
  • 时间:0
  • 页码:859-878
  • 语言:中文
  • 分类:TM911[电气工程—电力电子与电力传动]
  • 作者机构:[1]山东理工大学化学工程学院,山东淄博255049, [2]天津大学化工学院,天津300072
  • 相关基金:国家自然科学基金(20776081);山东省自然科学基金(Y2006B37)
  • 相关项目:平面聚合含氮大环配合物燃料电池催化剂的制备研究
中文摘要:

采用模板法制备了卟啉化合物Meso-5,10,15,20-四(N,N-二甲氨基苯基)卟啉铁(Ⅱ)(TDMNPPFe(Ⅱ)),用活性碳固载、活化制成催化剂。用TEM、XRD对催化剂的微观形貌进行了表征,结果表明,TDMNPPFe(Ⅱ)均匀分散在活性碳表面,当活化温度高于950℃时,催化剂表面开始出现金属原子簇结构的晶体。利用旋转圆盘电极表征了TDMNPPFe(Ⅱ)的催化氧还原活性,考察了活化温度、Fe(Ⅱ)载量对催化活性的影响。结果表明,最佳活化温度为600℃,最佳Fe(Ⅱ)载量为6%(质量分数)。把600℃活化的6%载量的催化剂(Catmax)与Pt/C(ω=30%)作了比较,结果表明Catmax比Pt/C催化剂氧还原起始电位负约90mV,但反应电子转移数相差不大。利用循环伏安法和线性伏安法测试了Catmax催化剂的耐甲醇性能,结果表明,甲醇的加入对催化剂的催化氧还原行为没有任何影响,表明TDMNPPFe(Ⅱ)具有良好的耐甲醇性能。

英文摘要:

Meso-5, 10, 15, 20-tetra (N, N-dimethylaminophenyl) porphyrin Fe ( II ) [TDMNPPFe ( II )] were synthesized by one pot method of mixed solvents (propionic acid, acetic acid and nitrobenzene), using Fe( II ) as template. It was adsorbed on the VulcanXC-72 carbon with different proportion and then heat-treated on temperature from 400 ℃ to 1 050 ℃. They were characterized by TEM and XRD, and the result shows that TDMNPPFe ( II ) was adsorbed on the surface of the VulcanXC-72 carbon homogeneously. XRD spectra shows metal crystalline species appears when heat-treated beyond 950 ℃. The catalytic reduction behavior of TDMNPPFe ( II ) catalyst modified on the glass carbon electrode. Using RDE, their electrocatalytic performance for oxygen reduction was investigated by linear voltammetry in O2 satured 0.5 mol/L H2SO4. The influences of activation temperature and Fe ( II ) Ioadings were investigated by K-L curves. The result indicates that TDMNPPFe ( II ) catalysts shows best electrocatalysts capability when heat treat at 600 ℃, and with 6% Fe ( II ) Ioadings (Catmax). Compared Catmax with Pt/C (ω=30%), the original reduction potential was approximately negative 90 mV than Pt/C, but the number of electrons transferred per oxygen molecule were 3.82, similarly with Pt/C. This indicates that almost all the oxygen molecule was reduced to water. The effect of methanol was investigated by means of the cyclic voltammetry and linear voltammetry. The result indicates that Pt/C has two oxidation apices of methanol but TDMNPPFe( II ) catalyst does not. The oxygen reduction curves with or without methanol showed that methanol has no effect with the oxygen reduction reaction. So the TDMNPPFe( II ) catalyst was methanol-tolerant.

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期刊信息
  • 《电源技术》
  • 中国科技核心期刊
  • 主管单位:中国电子科技集团公司
  • 主办单位:中国电子科技集团公司第十八研究所
  • 主编:黄永才
  • 地址:天津市西青海泰华科七路6号
  • 邮编:300384
  • 邮箱:cjps@tips.ac.cn
  • 电话:022-23959362
  • 国际标准刊号:ISSN:1002-087X
  • 国内统一刊号:ISSN:12-1126/TM
  • 邮发代号:6-28
  • 获奖情况:
  • 国家期刊提名奖,国家“双效”期刊,连续四届天津市优秀期刊
  • 国内外数据库收录:
  • 美国化学文摘(网络版),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),中国北大核心期刊(2000版)
  • 被引量:11796