Ni-Mo双金属催化剂的甲烷化性能与耐硫稳定性

doi:10.11949/j.issn.0438-1157.20171098

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. 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. 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/Abstract

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:

TQ426.94

王昱涵, 白思雨, 崔丽杰, 刘姣, 余剑, 许光文. Ni-Mo双金属催化剂的甲烷化性能与耐硫稳定性[J]. 化工学报, 2018, 69(5): 2063-2072.

WANG Yuhan, BAI Siyu, CUI Lijie, LIU Jiao, YU Jian, XU Guangwen. Catalytic activity and sulfur-resistance stability of Ni-Mo-based catalysts for syngas methanation[J]. CIESC Journal, 2018, 69(5): 2063-2072.

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Ni-Mo双金属催化剂的甲烷化性能与耐硫稳定性

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

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