等离子体催化甲烷干重整实验研究

Experimental study on dry reforming of methane by a plasma catalytic hybrid system

本文利用等离子体耦合催化剂的方式进行CH_(4)干重整(Dry Reforming of Methane,DRM),重点考察了反应温度、CO_(2)/CH_(4)物质的量比、合成气主要气体组分浓度(N_(2)、H2、CO、H2O)对CH_(4)转化率及等离子体催化能量效率的影响。结果表明,以La-Ni/γ-Al_(2)O_(3)为催化剂,当反应温度450℃,CO_(2)/CH_(4)物质的量比为1.0时,CH_(4)转化率为41.57%;提高CO_(2)/CH_(4)物质的量比可提高CH_(4)转化率,当CO_(2)/CH_(4)物质的量比为5.0时,等离子体催化CH_(4)干重整过程的CH_(4)转化率可达92.82%。温度和CO_(2)/CH_(4)物质的量比对CH_(4)转化率影响显著,气体组分的变化改变了体系中的激发态粒子,不仅直接影响到CH_(4)转化率,还影响着催化剂表面积炭。向反应体系中添加N_(2)、H2O可提高CH_(4)转化率,并抑制积炭;而添加H2、CO后CH_(4)转化率显著降低。研究结果可望为生物质气化合成化工品的工艺开发提供基础数据和参考依据。

In this paper,the plasma coupled catalyst was used for the dry reforming of methane(DRM).The impacts of the reaction temperature,the molar ratio of CO_(2)/CH_(4),and the concentration of the main gas components(N_(2),H2,CO,H2O)on the conversion rate of CH_(4) and the energy efficiency of plasma catalysis were observed.The results shows that the conversion rate of CH_(4) is 41.57%,with La-Ni/γ-Al_(2)O_(3) as the catalyst,the reaction temperature being 450℃and the molar ratio of CO_(2)/CH_(4) being 1.0,and without other gases.The conversion rate of CH_(4) increases with the increase of the molar ratio of CO_(2)/CH_(4).The conversion rate of CH_(4) is 92.82%respectively during DRM by plasma catalysis,with the molar ratio of CO_(2)/CH_(4) being 5.0.The reaction temperature and the molar ratio of CO_(2)/CH_(4) have a significant effect on CH_(4) conversion.The excited particles in the system are influenced by the changes of gas composition,which affect not only CH_(4) conversion directly,but also the carbon deposition on the surface of catalyst.The addition of N_(2) and H2O in the reaction system not only improves conversion of CH_(4) but also inhibits carbon deposition.The addition of H2 and CO reduces the conversion of CH_(4) significantly.The results are expected to provide basic data and reference for the development of the synthetic process of chemicals through biomass gasification.