Acta Chimica Sinica ›› 2006, Vol. 64 ›› Issue (11): 1173-1178. Previous Articles     Next Articles

Original Articles

铂催化甲醇氧化开始步骤的研究

李兰兰1,2,3,魏子栋*,1,2,3,李莉d,孙才新1   

  1. (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)
    (2重庆大学化学化工学院 重庆 400044)
    (3重庆大学材料科学与工程学院 重庆 400044)
    (4西华师范大学化学系 南充 637002)
  • 收稿日期:2005-06-21 修回日期:2006-02-08 出版日期:2006-06-15 发布日期:2006-06-15
  • 通讯作者: 魏子栋

Study of the Initial Steps of Methanol Electrooxidation Catalyzed by Pt

LI Lan-Lan1,2,3, WEI Zi-Dong*,1,2,c, LI Li4, SUN Cai-Xin1   

  1. (1 Key Laboratory of High Voltage Engineering and Electrical New Technology, The Ministry of Education,
    Chongqing University, Chongqing 400044)
    (2 School of Chemical Engineering, Chongqing University, Chongqing 400044)
    (3 School of Material Science and Engineering, Chongqing University, Chongqing 400044)
    (4 Department of Chemistry, China West Normal Universit, Nanchong 637002)
  • Received:2005-06-21 Revised:2006-02-08 Online:2006-06-15 Published:2006-06-15
  • Contact: WEI Zi-Dong

The dehydrogenation of methanol on low-index single Pt crystal surfaces has been studied by means of the ab initio and DFT approaches. Besides the well-known Bagotzky pattern, three adsorptive and dehydrogenation patterns of methanol on platinum were put forward and confirmed through the ab initio calculations. The three in situ detected intermediates of methanol dehydrogenation on Pt surface, i.e., CHOH, CH2OH and CH3O, were confirmed by ab initio and DFT approaches. It is concluded that whether hydrogen atom dehydrogenates from methanol molecule depends on whether it is absorbed by Pt atom and forms Pt—H bond. Different adsorptive patterns occured on different platinum planes correspondingly because of the specific atomic arrangement and electronic structure of Pt planes, leading to specific intermediates on platinum surface.

Key words: ab initio, methanol oxidation, direct methanol fuel cell