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碳载PtRuNi纳米复合材料作为质子交换膜燃料电池耐CO电催化剂的合成及构效关系探索

Synthesis and structure-activity relationship exploration of carbon-supported PtRuNi nanocomposite as a CO-tolerant electrocatalyst for proton exchange membrane fuel cells.

作者信息

Liang Yongmin, Zhang Huamin, Tian Zhiqun, Zhu Xiaobing, Wang Xiaoli, Yi Baolian

机构信息

Proton Exchange Membrane Fuel Cell Key Materials and Technology Laboratory, Dalian Institute of Chemical Physics, China Academy of Sciences, Dalian 116023, China.

出版信息

J Phys Chem B. 2006 Apr 20;110(15):7828-34. doi: 10.1021/jp0602732.

Abstract

A carbon-supported PtRuNi nanocomposite is synthesized via a microwave-irradiated polyol plus annealing synthesis strategy. The catalyst is characterized by transmission electron microscopy, powder X-ray diffraction, energy dispersive spectroscopy, and X-ray photoelectron spectroscopy. The data are discussed with respect to those for the carbon-supported PtRu nanocomposite prepared following the same way. The characterizations show that the inclusion of Ni in the PtRu system has only a small effect on the particle size, the structure, and the compositional homogeneity. CO-stripping voltammetry and measurements on the single proton exchange membrane fuel cells show that the PtRuNi/C catalyst has an improved activity for CO(ads) electro-oxidation. An accelerated durability test on the catalyst exhibits insignificant loss of activity in acidic media. On the basis of the exploration of the structure-activity relationship, a mechanism for the improved performance of the catalyst is proposed. It is suggested that the improved CO-tolerant performance of the PtRuNi/C nanocomposite should be related to the hydrogen spillover on the catalyst surface, the enhanced oxidation of CO(ads) by nickel hydroxides, and the high proton and electronic conductivity of the hydroxides. The nickel hydroxide passivated surface and/or anchoring of metallic nickel in the platinum lattice may contribute to the durability of the catalyst in acid solution.

摘要

通过微波辐照多元醇加退火合成策略合成了碳载PtRuNi纳米复合材料。采用透射电子显微镜、粉末X射线衍射、能量色散光谱和X射线光电子能谱对催化剂进行了表征。并将所得数据与采用相同方法制备的碳载PtRu纳米复合材料的数据进行了讨论。表征结果表明,在PtRu体系中引入Ni对粒径、结构和组成均匀性的影响较小。CO溶出伏安法和单质子交换膜燃料电池测试表明,PtRuNi/C催化剂对CO(ads)的电氧化活性有所提高。对该催化剂进行的加速耐久性测试表明,其在酸性介质中的活性损失不明显。在探索结构-活性关系的基础上,提出了催化剂性能提高的机理。研究表明,PtRuNi/C纳米复合材料耐CO性能的提高应与催化剂表面的氢溢流、氢氧化镍对CO(ads)氧化的增强以及氢氧化物的高质子和电子传导率有关。氢氧化镍钝化表面和/或金属镍在铂晶格中的锚定可能有助于催化剂在酸性溶液中的耐久性。

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