能源化学(英文版)

能源化学(英文) ›› 2005, Vol. 14 ›› Issue (2): 107-114.

• Articles • 上一篇    下一篇

Influence of Aging Time on the Properties of Precursors of CuO/ZnO Catalysts for Methanol Synthesis

Deren Fang, Zhongmin Liu, Shuanghe Meng, Ligang Wang, Lei Xu, Hua Wang   

  1. 1. Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China; 2. Institute of Applied Catalysis, Yantai University, Yantai 264005, China
  • 出版日期:2005-06-30 发布日期:2005-06-30

Influence of Aging Time on the Properties of Precursors of CuO/ZnO Catalysts for Methanol Synthesis

Deren Fang, Zhongmin Liu, Shuanghe Meng, Ligang Wang, Lei Xu, Hua Wang   

  • Online:2005-06-30 Published:2005-06-30

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摘要： The aging process of pure copper precursors and copper-zinc binary precursors were studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnO were tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cu species were characterized with N2 adsorption and N2O passivation method, respectively. For the Cu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80 ‰, the initial phase was a mixture of copper nitrate hydroxide Cu2(NO3)(OH)3, georgeite and hydrozincite Zn5(CO3)2(OH)6. By increasing the duration of its aging time, the phase of Cu2(NO3)(OH)2 first transited to georgeite, and then interdiffused into Zn5(CO3)2(OH)6 and resulted in two new phases: rosasite (Cu,Zn)2CO3(OH)2 and aurichalcite (Zn,Cu)5(CO3)2(OH)6. The former phase was much easier to be formed than the latter one, while the latter phase was more responsible for the activity of methanol synthesis than the former one. It is found that the composition and structure of the precursors altered obviously after the colour transition point. The experimental results showed that methanol synthesis is a structure-sensitive catalytic reaction.

关键词: Cu/Zn oxide, methanol synthesis, precursor, aging time, colour transition, structure-sensitive reaction

Abstract: The aging process of pure copper precursors and copper-zinc binary precursors were studied by XRD, TG-DTG and TPR techniques. The catalytic activity and stability of CuO/ZnO were tested using fixed-bed flow reactor, and the physical properties of the catalysts and Cu species were characterized with N2 adsorption and N2O passivation method, respectively. For the Cu-Zn binary system prepared at the precipitating condition of pH=8.0 and temperature=80 ‰, the initial phase was a mixture of copper nitrate hydroxide Cu2(NO3)(OH)3, georgeite and hydrozincite Zn5(CO3)2(OH)6. By increasing the duration of its aging time, the phase of Cu2(NO3)(OH)2 first transited to georgeite, and then interdiffused into Zn5(CO3)2(OH)6 and resulted in two new phases: rosasite (Cu,Zn)2CO3(OH)2 and aurichalcite (Zn,Cu)5(CO3)2(OH)6. The former phase was much easier to be formed than the latter one, while the latter phase was more responsible for the activity of methanol synthesis than the former one. It is found that the composition and structure of the precursors altered obviously after the colour transition point. The experimental results showed that methanol synthesis is a structure-sensitive catalytic reaction.

Key words: Cu/Zn oxide, methanol synthesis, precursor, aging time, colour transition, structure-sensitive reaction