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钌修饰的铂表面作为用于一氧化碳电氧化的模型燃料电池电催化剂。

Ru-decorated Pt surfaces as model fuel cell electrocatalysts for CO electrooxidation.

作者信息

Maillard F, Lu G-Q, Wieckowski A, Stimming U

机构信息

Laboratoire d'Electrochimie et de Physicochimie des Matériaux et des Interfaces, UMR CNRS 5631, ENSEEG, BP75, 38402 Saint Martin d'Hères, France.

出版信息

J Phys Chem B. 2005 Sep 1;109(34):16230-43. doi: 10.1021/jp052277x.

DOI:10.1021/jp052277x
PMID:16853064
Abstract

This feature article concerns Pt surfaces modified (decorated) by ruthenium as model fuel cell electrocatalysts for electrooxidation processes. This work reveals the role of ruthenium promoters in enhancing electrocatalytic activity toward organic fuels for fuel cells, and it particularly concerns the methanol decomposition product, surface CO. A special focus is on surface mobility of the CO as it is catalytically oxidized to CO(2). Different methods used to prepare Ru-decorated Pt single crystal surfaces as well as Ru-decorated Pt nanoparticles are reviewed, and the methods of characterization and testing of their activity are discussed. The focus is on the origin of peak splitting involved in the voltammetric electrooxidation of CO on Ru-decorated Pt surfaces, and on the interpretative consequences of the splitting for single crystal and nanoparticle Pt/Ru bimetallic surfaces. Apparently, screening through the literature allows formulating several models of the CO stripping reaction, and the validity of these models is discussed. Major efforts are made in this article to compare the results reported by the Urbana-Champaign group and the Munich group, but also by other groups. As electrocatalysis is progressively more and more driven by theory, our review of the experimental findings may serve to summarize the state of the art and clarify the roads ahead. Future studies will deal with highly dispersed and reactive nanoscale surfaces and other more advanced catalytic materials for fuel cell catalysis and related energy applications. It is expected that the metal/metal and metal/substrate interactions will be increasingly investigated on atomic and electronic levels, with likewise increasing participation of theory, and the structure and reactivity of various monolayer catalytic systems involving more than two metals (that is ternary and quaternary systems) will be interrogated.

摘要

这篇专题文章关注通过钌修饰(装饰)的铂表面,作为用于电氧化过程的模型燃料电池电催化剂。这项工作揭示了钌促进剂在增强燃料电池对有机燃料的电催化活性方面的作用,尤其关注甲醇分解产物表面一氧化碳。特别关注的是一氧化碳在催化氧化为二氧化碳时的表面迁移率。综述了用于制备钌修饰的铂单晶表面以及钌修饰的铂纳米颗粒的不同方法,并讨论了其活性的表征和测试方法。重点在于钌修饰的铂表面上一氧化碳伏安电氧化中涉及的峰分裂的起源,以及该分裂对单晶和纳米颗粒铂/钌双金属表面的解释结果。显然,通过文献筛选可以制定几种一氧化碳脱附反应模型,并讨论这些模型的有效性。本文主要致力于比较伊利诺伊大学厄巴纳 - 香槟分校团队和慕尼黑团队以及其他团队所报道的结果。随着电催化越来越受理论驱动,我们对实验结果的综述可能有助于总结当前的技术水平并阐明未来的方向。未来的研究将涉及用于燃料电池催化及相关能源应用的高度分散且反应性强的纳米级表面和其他更先进的催化材料。预计将在原子和电子层面上越来越多地研究金属/金属和金属/底物相互作用,理论的参与度也会同样增加,并且将研究涉及两种以上金属(即三元和四元体系)的各种单层催化体系的结构和反应性。

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