化工学报 ›› 2018, Vol. 69 ›› Issue (5): 2063-2072.DOI: 10.11949/j.issn.0438-1157.20171098

• 催化、动力学与反应器 • 上一篇    下一篇

Ni-Mo双金属催化剂的甲烷化性能与耐硫稳定性

王昱涵1, 白思雨2, 崔丽杰1, 刘姣3, 余剑3, 许光文4   

  1. 1. 中国科学院大学, 北京 100049;
    2. 中国矿业大学研究生院, 江苏 徐州 221008;
    3. 中国科学院过程工程研究所, 北京 100190;
    4. 沈阳化工大学, 辽宁 沈阳 110142
  • 收稿日期:2017-08-14 修回日期:2017-12-15 出版日期:2018-05-05 发布日期:2018-05-05
  • 通讯作者: 刘姣
  • 基金资助:

    国家高技术研究发展计划项目(2015AA050502)。

Catalytic activity and sulfur-resistance stability of Ni-Mo-based catalysts for syngas methanation

WANG Yuhan1, BAI Siyu2, CUI Lijie1, LIU Jiao3, YU Jian3, XU Guangwen4   

  1. 1. University of Chinese Academy of Sciences, Beijing 100049, China;
    2. China University of Mining and Technology, Xuzhou 221008, Jiangsu, China;
    3. Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    4. Shenyang University of Chemical Technology, Shenyang 110142, Liaoning. China
  • Received:2017-08-14 Revised:2017-12-15 Online:2018-05-05 Published:2018-05-05
  • Supported by:

    supported by the National High Technology Research and Development Program of China (2015AA050502).

摘要:

采用沉淀-浸渍法合成一系列Ni-Mo基双金属催化剂,在固定床反应器中对其催化活性和耐硫性能进行评价,并辅以不同的表征手段阐释其作用机理。实验结果表明,以MCM-41分子筛为载体的催化剂活性和稳定性优于以NaY、γ-Al2O3和拟薄水铝石(PB)为载体的催化剂;反应前后催化剂的表征结果则说明Ni-Mo分子间适宜的相互作用是决定催化剂性能的关键。MCM-41载体催化剂中适宜的Ni-Mo分子间相互作用使得此催化剂中活性组分与载体间的相互作用适中,还原后的活性金属Ni能够均匀分散在载体表面,从而提高了催化剂的耐硫稳定性和抗积炭能力。不同Ni-Mo比同样会影响Ni-Mo分子间的相互作用,通过考察确定20Ni-10Mo/MCM-41的活性和稳定性最优。

关键词: 甲烷, 耐硫, 催化剂, MCM-41, 一氧化碳, 合成气

Abstract:

A series of Ni-Mo-based catalysts, prepared by precipitation-impregnation method, were studied for catalytic activity and sulfur resistance in a fixed bed reactor. Different characterization techniques were carried out to interpret their reaction mechanisms. Compared to catalysts with supports of NaY, γ-Al2O3 and pseudoboehmite (PB), catalyst with MCM-41 support showed superior activity and stability. Characterization on catalysts before and after reaction showed that Ni-Mo interaction plays critical role in catalyst performance. In the catalyst supported with MCM-41, Ni-Mo interaction resulted in appropriate interaction between active species and support. Reduced active Ni was homogeneously dispersed on support surface, which enhanced sulfur-resistance stability and anti-carbon deposition. Different Ni/Mo ratios also affected Ni-Mo interaction in catalysts. It was found that the 20Ni-10Mo/MCM-41 catalysts exhibited the best performance.

Key words: methane, sulfur-resistance, catalyst, MCM-41, carbon monoxide, syngas

中图分类号: