物理化学学报 >> 2002, Vol. 18 >> Issue (05): 426-431.doi: 10.3866/PKU.WHXB20020509

研究论文 上一篇    下一篇

Ni-Fe催化剂乙醇部分氧化制氢的研究

王卫平;席靖宇;王志飞;吕功煊;赵普   

  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:2001-09-19 修回日期:2001-12-21 发布日期:2002-05-15
  • 通讯作者: 吕功煊 E-mail:gxlu@ns.lzb.ac.cn

Partial Oxidation of Ethanol to Hydrogen over Ni-Fe Catalysts

Wang Wei-Ping;Xi Jing-Yu;Wang Zhi-Fei;Lü Gong-Xuan;Zhao Pu   

  • Received:2001-09-19 Revised:2001-12-21 Published:2002-05-15
  • Contact: Lü Gong-Xuan E-mail:gxlu@ns.lzb.ac.cn

摘要: 研究了NiFe催化剂对乙醇部分氧化制氢反应,系统地考察了不同O2/C2H5OH摩尔比及反应温度下催化剂的性能.发现NiFe催化剂对乙醇部分氧化制氢具有较好的催化活性,其中组成为Ni50Fe50催化剂最好,最佳的反应条件是O2/C2H5OH=1.0,T=573 K.XRD谱图表明催化剂主要由尖晶石结构的铁酸盐和FeNi3合金相组成. XPS结果说明,催化剂体相以还原态FeNi3合金相为主,表面以氧化态的铁酸盐为主.稳定性考察的结果表明,催化剂经40 h反应后,对氢的选择性明显下降,此时对应的FeNi3物相衍射峰强度也明显降低,表明催化剂对H2选择性的下降与FeNi3物相的转变有关.

关键词: 乙醇, 部分氧化, Ni-Fe催化剂, 制氢

Abstract: Catalytic generation of hydrogen by partial oxidation of ethanol over a series of NiFe catalysts has been studied.The catalytic performances have been investigated over various O2/C2H5OH molar ratio at 473~573 K.These NiFe catalysts showed high performances for the partial oxidation of ethanol to hydrogen and Ni50Fe50 catalyst had the best activity when reaction temperature was between 548K and 573 K.The optimum reaction conditions for Ni50Fe50 catalyst are O2/C2H5OH =1.0、T=573 K.The fresh and used catalysts were characterized by XRD and XPS.The XRD patterns showed the main components of the active catalysts are the spinaltype structure of magnetite and FeNi3 alloy(see Fig.4).The decrease in the selectivity for hydrogen of the catalyst may be resulted from the conversion of FeNi3 alloy phase in the catalyst during long term reaction(see Fig.5).XPS results confirmed that the phase of the bulk catalyst is mainly FeNi3 alloy and that of the surface catalyst is mainly magnetite (see Fig 6).

Key words: Ethanol, Partial oxidation, Ni-Fe catalyst, Hydrogen generation