物理化学学报 >> 2007, Vol. 23 >> Issue (05): 723-727.doi: 10.3866/PKU.WHXB20070519

研究论文 上一篇    下一篇

甲醇在欠电位沉积Ru修饰Pt电极上的催化氧化

李兰兰; 魏子栋; 严灿; 罗义辉; 尹光志; 孙才新   

  1. 重庆大学高电压与电工新技术教育部重点实验室, 重庆 400044; 重庆大学化学化工学院, 重庆 400044; 重庆大学材料科学与工程学院, 重庆 400044; 重庆大学西南资源开发及环境灾害控制工程教育部重点实验室, 重庆 400044
  • 收稿日期:2006-10-31 修回日期:2006-12-04 发布日期:2007-04-28
  • 通讯作者: 魏子栋 E-mail:zdwei@cqu.edu.cn

Methanol Oxidation on a Pt ElectrodeModified by Underpotential Deposition of Ru

LI Lan-Lan; WEI Zi-Dong; YAN Can; LUO Yi-Hui; YIN Guang-Zhi; SUN Cai-Xin   

  1. Key Laboratory of High Voltage Engineering and Electrical New Technology of the Ministry of Education, Chongqing University, Chongqing 400044, P. R. China; School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, P. R. China; School of Material Science and Engineering, Chongqing University, Chongqing 400044, P. R. China; Key Laboratory of Exploitation of Southwestern Resources&the Environmental Disaster Control Engineering of the Ministry of Education, Chongqing University, Chongqing 400044, P. R. China
  • Received:2006-10-31 Revised:2006-12-04 Published:2007-04-28
  • Contact: WEI Zi-Dong E-mail:zdwei@cqu.edu.cn

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摘要： 采用欠电位沉积(upd)方法在Pt 表面沉积亚单层的Ru制备出upd-Ru/Pt 电极. 通过欠电位沉积前后电极在0.5 mol·L-1 H2SO4溶液中循环伏安图-152 - 128 mV(vs Ag/AgCl)电位范围内对氢区的数值积分确定Pt表面Ru 的覆盖度. 用电化学方法测试了甲醇在upd-Ru/Pt电极上的催化氧化, 并讨论分析了欠电位沉积电位和Ru的表面覆盖度对甲醇氧化的影响. 结果表明, Ru能够欠电位沉积到Pt表面. Pt表面欠电位沉积少量的Ru 即能大大促进甲醇的氧化.只要控制upd-Ru的沉积量, upd-Ru原子就能大大促进甲醇氧化而与沉积电位无关. Ru原子对甲醇氧化的促进作用与Ru和Pt是否形成合金无关, 而取决于Ru 在Pt表面的百分含量.

关键词: 欠电位沉积, 甲醇电化学氧化, 欠电位沉积(upd)-Ru/Pt电极

Abstract: Underpotential deposition (upd) of rutheniumon a platinumelectrode was adopted to obtain a submonolayer of ruthenium on platinum surface. Ru coverage was evaluated according to the change of the hydrogen desorption area in the cyclic voltammograms (CV) of Pt electrodes before and after upd-Ru modification in 0.5 mol·L-1 H2SO4. The effects
of the potential for formation of upd-Ru and coverage of upd-Ru adtoms on methanol oxidation were investigated and analyzed. It was shown that Ru adatoms could be underpotentially deposited on a platinum surface. The submonolayer of upd-Ru on the Pt electrode could enhance methanol electrooxidation several times as large as that on the pure Pt electrode. It was also shown that as long as the amount of upd-Ru adatoms was controlled in a proper range, upd-Ru deposits would enhance the methanol oxidation independently of the deposition potential. The catalytic activity of binary Pt-Ru catalysts for methanol electrooxidation was highly associated with the surface composition of Pt and Ru, but was free of whether Pt-Ru deposits appear in a formof alloy, bimetallic compounds, adatoms, or something else.

Key words: Underpotential deposition, Methanol electrooxidation, Upd-Ru/Pt electrode