物理化学学报 >> 2010, Vol. 26 >> Issue (05): 1207-1213.doi: 10.3866/PKU.WHXB20100522

电化学 上一篇    下一篇

稀土Eu掺杂PtRu/C催化剂及其对甲醇电氧化的性能

安筱莎, 陈德俊, 周志有, 汪强, 樊友军, 孙世刚   

  1. 药用资源化学与药物分子工程教育部重点实验室, 广西师范大学化学化工学院, 广西 桂林 541004; 固体表面物理化学国家重点实验室, 厦门大学化学化工学院化学系, 福建 厦门 361005
  • 收稿日期:2009-09-28 修回日期:2010-02-08 发布日期:2010-04-29
  • 通讯作者: 樊友军, 孙世刚 E-mail:youjunfan@mailbox.gxnu.edu.cn; sgsun@xmu.edu.cn

Rare Earth Eu Doped PtRu/C Catalysts and Their Properties for Methanol Electrooxidation

AN Xiao-Sha, CHEN De-Jun, ZHOU Zhi-You, WANG Qiang, FAN You-Jun, SUN Shi-Gang   

  1. Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources (Ministry of Education of China), College of Chemistry and Chemical Engineering, Guangxi Normal University, Guilin 541004, Guangxi Zhuang Autonomous Region, P. R. China; State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China
  • Received:2009-09-28 Revised:2010-02-08 Published:2010-04-29
  • Contact: FAN You-Jun, SUN Shi-Gang E-mail:youjunfan@mailbox.gxnu.edu.cn; sgsun@xmu.edu.cn

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摘要：

采用化学还原和热处理方法对商业PtRu/C催化剂进行稀土Eu掺杂, 制备了不同Eu含量的PtRuEux/C催化剂. 透射电子显微镜(TEM)、X射线能量色散光谱(EDX)、X射线衍射(XRD)和X射线光电子能谱(XPS)等方法表征催化剂的结果表明, Eu的掺杂未改变PtRu/C催化剂的平均粒径(约为3 nm), 并且Eu以金属和氧化物两种形态修饰PtRu表面. 循环伏安和计时电流法测试显示, PtRuEux/C催化剂较商业PtRu/C对甲醇氧化具有更高的活性, 其中PtRuEu0.3/C的活性最高. 运用原位傅里叶变换红外(FTIR)光谱从分子水平研究了该催化剂对甲醇电催化氧化的反应过程, 检测到甲醇在催化剂上解离吸附的吸附态产物是线型吸附态CO (COL), Eu的掺杂使COL的氧化电位降低, 明显提高了催化剂的活性和抗CO毒化的能力.

关键词: 直接甲醇燃料电池, 甲醇电氧化, 阳极催化剂, 稀土改性, 原位FTIR光谱

Abstract:

Commercially available PtRu/C catalyst was doped with Eu by chemical reduction and sintering, resulting in PtRuEux/C catalysts with different Eu contents. The catalysts were characterized by transmission electron microscopy (TEM), energy dispersive X-ray (EDX) spectroscopy, X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Results showed that Eu doping did not change the average size of the PtRu/C catalysts (ca 3 nm), and their surfaces were modified by both Eu metal and oxide. Cyclic voltammetry and chronoamperometry demonstrated that the activity of the PtRuEux/C catalysts was higher than that of commercial PtRu/C for methanol electrooxidation. Among the PtRuEux/C catalysts, PtRuEu0.3/C exhibited the best performance. The electrocatalytic oxidation of methanol on the catalyst was further investigated by in situ Fourier transforminfrared (FTIR) spectroscopy at molecular level. Results indicated that the adsorbed species derived from the dissociative adsorption of methanol on the catalysts were linear-bonded CO (COL). Eu doping decreased the oxidation potential of COL and thus significantly enhanced the activity of the catalysts and their tolerance to CO.

Key words: Direct methanol fuel cell, Methanol electrooxidation, Anode catalyst, Rare earth doping, in situ FTIR spectroscopy