物理化学学报 >> 2001, Vol. 17 >> Issue (07): 655-658.doi: 10.3866/PKU.WHXB20010717

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Cu/Zn、Cu/Zn/Ni催化剂甲醇部分氧化制氢

席靖宇;吕功煊;王志飞   

  1. 中国科学院兰州化学物理研究所 羰基合成与选择氧化国家重点实验室，兰州　730000
  • 收稿日期:2000-11-14 修回日期:2001-02-27 发布日期:2001-07-15
  • 通讯作者: 吕功煊 E-mail:gxlu@ns.lzb.ac.cn

Partial Oxidation of Methanol to Hydrogen over Cu/Zn and Cu/Zn/Ni Catalysts

Xi Jing-Yu;Lv Gong-Xuan;Wang Zhi-Fei   

  1. State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Instit ute of Chemical Physics, Chinese Academy of Sciences, Lanzhou　730000
  • Received:2000-11-14 Revised:2001-02-27 Published:2001-07-15
  • Contact: Lv Gong-Xuan E-mail:gxlu@ns.lzb.ac.cn

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摘要： 研究了甲醇在Cu/Zn及Cu/Zn/Ni催化剂上部分氧化热耦合裂解制氢的反应，系 统地考察了不同O2/CH3OH比及反应温度下催化剂性能.当O2/CH3OH=0.2时，催化剂的性能最 佳.在同样条件下， Cu/Zn催化剂对CO的选择性较Cu/Zn/Ni催化剂低，更具优势. Cu/Zn催化 剂用于甲醇部分氧化反应时，甲醇转化率在150 h寿命实验中基本保持在90％左右. XRD谱图 表明Cu/Zn合金的生成是导致Cu/Zn系催化剂在甲醇裂解反应中快速失活的主要原因，而在部 分氧化反应中， O2的存在可抑制Cu/Zn合金的生成，使Cu/Zn催化剂表现出高度的稳定性.

关键词: 甲醇, 氢气, 直接裂解, 部分氧化, Cu/Zn催化剂, Cu/Zn/Ni催化剂

Abstract: Catalytic generation of hydrogen by the coupling of decomposition and partial oxidation of methanol over Cu/Zn and Cu/Zn/Ni catalysts have been studie d. These Cu-Zn based catalysts show high activity and stability for the partial oxidation of methanol. The catalytic activity and selectivity are affected by t he ratio of O2/CH3OH. The optimum reaction conditions for Cu-Zn catalyst are O2 /CH3OH=0.2, T=523 K. The formation of CuZn alloy was observed in the deactivated Cu/Zn catalysts after methanol decomposition at 523 K for 20 h. On the contrary , no CuZn alloy was found in the used Cu/Zn catalyst after partial oxidation of methanol for 150 h at 523 K. The presented results seem to indicate that the for mation of CuZn alloy is one of the main reasons for the deactivation of Cu-Zn b ased catalysts in methanol decomposition.

Key words: Methanol, Hydrogen, Decomposition, Partial oxidation, Cu/Zn catal yst, 　Cu/Zn/Ni catalyst