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

doi:10.11949/j.issn.0438-1157.20171098

Abstract

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

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

CLC Number:

TQ426.94

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.

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.

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