化工学报 ›› 2014, Vol. 65 ›› Issue (8): 2997-3003.DOI: 10.3969/j.issn.0438-1157.2014.08.021

• 催化、动力学与反应器 • 上一篇    下一篇

Ni-Mn/Al2O3催化剂在浆态床中CO甲烷化催化性能

孟凡会, 常慧蓉, 李忠   

  1. 太原理工大学煤科学与技术教育部和山西省重点实验室, 山西 太原 030024
  • 收稿日期:2014-01-28 修回日期:2014-04-28 出版日期:2014-08-05 发布日期:2014-08-05
  • 通讯作者: 李忠
  • 基金资助:

    国家重点基础研究发展计划项目(2012CB723105);山西省青年基金项目(2013021007-4);中国博士后科学基金项目(2013M541210);太原理工大学校青年基金项目(2012L040,2013T091)。

Catalytic performance of Ni-Mn/Al2O3 catalyst for CO methanation in slurry-bed reactor

MENG Fanhui, CHANG Huirong, LI Zhong   

  1. Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2014-01-28 Revised:2014-04-28 Online:2014-08-05 Published:2014-08-05
  • Supported by:

    supported by the National Basic Research Program of China (2012CB723105), the Youth Foundation of Shanxi Province (2013021007-4), China Postdoctoral Science Foundation (2013M541210) and the Youth Foundation of Taiyuan University of Technology (2012L040, 2013T091).

摘要: 采用共浸渍法制备了Ni-Mn/Al2O3催化剂,考察了助剂Mn的含量对催化剂结构及浆态床CO甲烷化性能的影响。采用XRD、H2-TPR、BET、TEM、H2-化学吸附等表征对催化剂进行了测试分析,结果表明,Mn助剂的引入能够促进Ni物种在载体表面的分散,减弱Ni物种与载体的相互作用,降低催化剂的还原温度,提高催化剂的比表面积,减小活性金属Ni的晶粒尺寸。随着Mn含量的增加,Ni-Mn/Al2O3催化剂的甲烷化性能先升后降,其中以Mn含量为4%(质量分数)时的催化甲烷化性能最佳,添加过量的Mn导致活性组分Ni被部分覆盖,催化甲烷化性能下降。通过对16Ni4Mn/Al2O3催化剂样品的浆态床反应温度及反应压力的研究发现,当反应温度为280℃、反应压力为1.5 MPa时,催化剂样品16Ni4Mn/Al2O3的CO转化率及CH4选择性分别达到96.2%和88.8%。

关键词: 浆态床反应器, 合成气, 甲烷化, 天然气, Ni-Mn/Al2O3催化剂, Mn助剂

Abstract: Ni-Mn/Al2O3 catalysts with different contents of Mn were prepared by co-impregnation method, and the catalytic performance for CO methanation in slurry-bed reactor was studied. The catalysts were characterized by XRD, H2-TPR, BET, TEM and H2-chemisorption. The addition of Mn promoted the dispersion of Ni species, weakened the interaction between Ni species and support, decreased the reduction temperature, increased the catalyst specific surface area and decreased the particle size of active metallic Ni. With the increase of Mn content, the catalytic performance of Ni-Mn/Al2O3 catalysts increased firstly and then decreased, and the catalyst Ni-Mn/Al2O3 with Mn content of 4% exhibited the best catalytic performance. Excess addition of Mn decreased catalytic performance, because the active component Ni was covered by Mn. The investigation on effects of reaction temperature and reaction pressure showed that under the reaction conditions of 280℃ and 1.5 MPa, conversion of CO and selectivity of CH4 for the catalyst sample 16Ni4Mn/Al2O3 reached 96.2% and 88.8%, respectively.

Key words: slurry-bed reactor, syngas, methanation, natural gas, Ni-Mn/Al2O3 catalyst, manganese promoter

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