SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2015, Vol. 23 ›› Issue (1): 86-92.DOI: 10.1016/j.cjche.2014.09.038

• 催化、动力学与反应工程 • 上一篇    下一篇

Performance characteristics of fluidized bed syngas methanation over Ni-Mg/Al2O3 catalyst

Jiao Liu1, Dianmiao Cui1,2, Jian Yu1, Fabing Su1, Guangwen Xu1   

  1. 1 State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    2 Graduate University of Chinese Academy of Sciences, Beijing 100864, China
  • 收稿日期:2012-12-27 修回日期:2013-10-31 出版日期:2015-01-28 发布日期:2015-01-24
  • 通讯作者: Guangwen Xu
  • 基金资助:

    Supported by the National Natural Science Foundation of China (21161140329), the International Science & Technology Cooperation Program of China (2013DFG60060), and the National Key Technology R&D Program (2010BAC66B01, 2012BAC03B05).

Performance characteristics of fluidized bed syngas methanation over Ni-Mg/Al2O3 catalyst

Jiao Liu1, Dianmiao Cui1,2, Jian Yu1, Fabing Su1, Guangwen Xu1   

  1. 1 State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    2 Graduate University of Chinese Academy of Sciences, Beijing 100864, China
  • Received:2012-12-27 Revised:2013-10-31 Online:2015-01-28 Published:2015-01-24
  • Contact: Guangwen Xu
  • Supported by:

    Supported by the National Natural Science Foundation of China (21161140329), the International Science & Technology Cooperation Program of China (2013DFG60060), and the National Key Technology R&D Program (2010BAC66B01, 2012BAC03B05).

摘要: The performance characteristics of isothermal fluidized bed syngas methanation for substitute natural gas are investigated over a self-made Ni-Mg/Al2O3 catalyst. Via atmospheric methanation in a laboratory fluidized bed reactor it was clarified that the CO conversion varied in 5% when changing the space velocity in 40-120 L·g-1·h-1 but the conversion increased obviously by raising the superficial gas velocity from 4 to 12.4 cm·s-1. The temperature at 823 K is suitable for syngas methanation while obvious deposition of uneasyoxidizing Cγ occurs on the catalyst at temperatures around 873 K. From a kinetic aspect, the lowest reaction temperature is suggested to be 750 K when the space velocity is 60 L·g-1·h-1. Raising the H2/CO ratio of the syngas increased proportionally the CO conversion and CH4 selectivity, showing that at enough highH2/CO ratios the active sites on the catalyst are sufficient for CO adsorption and in turn the reaction with H2 for forming CH4. Introducing CO2 into the syngas feed suppresses the water gas shift and Boudouard reactions and thus increased H2 consumption. The ratio of CO2/CO in syngas should be better below 0.52 because varying the ratio from 0.52 to 0.92 resulted in negligible increases in the H2 conversion and CH4 selectivity but decreased the CH4 yield. Introducing steam into the feed gas affected little the CO conversion but decreased the selectivity to CH4. The tested Ni-Mg/Al2O3 catalyst manifested good stability in structure and activity even in syngas containing water vapor.

关键词: Syngas methanation, Ni catalyst, Fluidized bed, Substitute natural gas, Performance

Abstract: The performance characteristics of isothermal fluidized bed syngas methanation for substitute natural gas are investigated over a self-made Ni-Mg/Al2O3 catalyst. Via atmospheric methanation in a laboratory fluidized bed reactor it was clarified that the CO conversion varied in 5% when changing the space velocity in 40-120 L·g-1·h-1 but the conversion increased obviously by raising the superficial gas velocity from 4 to 12.4 cm·s-1. The temperature at 823 K is suitable for syngas methanation while obvious deposition of uneasyoxidizing Cγ occurs on the catalyst at temperatures around 873 K. From a kinetic aspect, the lowest reaction temperature is suggested to be 750 K when the space velocity is 60 L·g-1·h-1. Raising the H2/CO ratio of the syngas increased proportionally the CO conversion and CH4 selectivity, showing that at enough highH2/CO ratios the active sites on the catalyst are sufficient for CO adsorption and in turn the reaction with H2 for forming CH4. Introducing CO2 into the syngas feed suppresses the water gas shift and Boudouard reactions and thus increased H2 consumption. The ratio of CO2/CO in syngas should be better below 0.52 because varying the ratio from 0.52 to 0.92 resulted in negligible increases in the H2 conversion and CH4 selectivity but decreased the CH4 yield. Introducing steam into the feed gas affected little the CO conversion but decreased the selectivity to CH4. The tested Ni-Mg/Al2O3 catalyst manifested good stability in structure and activity even in syngas containing water vapor.

Key words: Syngas methanation, Ni catalyst, Fluidized bed, Substitute natural gas, Performance