物理化学学报 >> 2004, Vol. 20 >> Issue (05): 524-528.doi: 10.3866/PKU.WHXB20040516

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CuO-ZnO-ZrO2催化甲醇水蒸汽重整反应机理和中间态

云虹;张慧;陈建华;陈鸿博;林昌健   

  1. 厦门大学化学系,固体表面物理化学国家重点实验室,厦门　361005
  • 收稿日期:2003-10-28 修回日期:2004-01-17 发布日期:2004-05-15
  • 通讯作者: 陈鸿博 E-mail:hbchen@jingxian.xmu.edu.cn

The Intermediate State and Mechanism of the Steam Reforming of Methanol over CuO-ZnO-ZrO2 Catalysts

Yun Hong;Zhang Hui;Chen Jian-Hua;Chen Hong-Bo;Lin Chang-Jian   

  1. Department of Chemistry, State Key Laboratory for Physical Chemistry of the Solid Surface , Xiamen University, Xiamen　361005
  • Received:2003-10-28 Revised:2004-01-17 Published:2004-05-15
  • Contact: Chen Hong-Bo E-mail:hbchen@jingxian.xmu.edu.cn

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摘要： 应用质谱在线技术,对CuO-ZnO-ZrO2催化甲醇水蒸汽重整（SRM）反应进行程序升温脱附（TPD）和程序升温表面反应（TPSR）研究.结果表明:在反应态催化剂表面,甲醇以分子吸附态形式存在,甲醇水蒸汽重整反应经历甲酸根中间物种.分别用CuO、CuO-ZnO、CuO-ZnO-ZrO2作催化剂,甲醇在气流中的摩尔分数分别高于5.4％、0.37％和0.17％时,甲酸根中间态的分解产物为CO2和H2；而甲醇在气流中的摩尔分数分别低于5.4％、0.37％和0.17％时,甲酸根中间态的分解产物为CO、CO2和H2.

关键词: 铜锌锆催化剂, 甲醇水蒸汽重整, 甲醇, 反应机理, 中间态

Abstract: The temperature-programmed desorption (TPD) and temperature-programmed surface reaction (TPSR) were studied by in situ mass spectrographic analysis. The results showed that methanol exists on the reactive surface of catalysts as molecular state and that adsorbed formate is one of intermediate species for the steam reforming of methanol (SRM).When the concentration of methanol among gas mixture is higher then 5.4％,0.37％ and 0.17％ for catalyst CuO, CuO-ZnO and CuO-ZnO-ZrO2, respectively, adsorbed formate decomposes into CO2 and H2,and conversely,CO,CO2 and H2 are products of formate decomposition.

Key words: CuO-ZnO-ZrO2 catalyst, Steam reforming of methanol (SRM), 　Methanol, Reaction mechanism, Intermediate