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The Reaction Mechanism and Its Kinetic Model of CO2 Reforming with CH4 over Ni-Mg15@HC Catalyst
Catalysis Letters ( IF 2.8 ) Pub Date : 2019-11-29 , DOI: 10.1007/s10562-019-03052-7
Jun Han , Yan Liang , Linbo Qin , Yu Wang , Huaqin Wang , Fei Yu , Bo Zhao

In this paper, the kinetic of CO2 dry reforming with CH4 (DRM) over the Ni-Mg15@HC catalyst was studied after excluding the influence of internal and external mass transfer at 700–850 °C. At the same time, the partial pressures of CH4 and CO2 were varied from 10 to 50 kPa. The experimental results demonstrated that the reaction rate was sharply increased with the increase of CH4 partial pressure, while the increase of CO2 partial pressure led to a relative increase of the reaction rate. Therefore, it could be said that CH4 dissociation was the rate determining step for DRM reaction. Moreover, the apparent activation energy of CH4 consumption (48.6 kJ/mol) during DRM reaction was higher than that of CO2 consumption (30.1 kJ/mol), which also confirmed the above assumption. On the basis of the reaction mechanism, a Langmuir–Hinshelwood kinetic rate model was developed, and the kinetic parameters were also estimated by the nonlinear least square regression method. The developed model could satisfactorily fit the experimental data, and R2 was as high as 0.965. The apparent activation energy of CH4 consumption during DRM reaction was higher than that of CO2, then the rate determining step was determined. A kinetic rate model was developed, which could well describe the experiment.

中文翻译:

Ni-Mg15@HC催化剂上CO2与CH4重整反应机理及其动力学模型

在本文中,在排除内部和外部传质影响后,在 700-850 °C 下研究了在 Ni-Mg15@HC 催化剂上用 CH4 (DRM) 进行 CO2 干重整的动力学。同时,CH4 和CO2 的分压在10 到50 kPa 之间变化。实验结果表明,随着CH4分压的增加,反应速率急剧增加,而CO2分压的增加导致反应速率相对增加。因此,可以说 CH4 解离是 DRM 反应的速率决定步骤。此外,DRM反应过程中CH4消耗的表观活化能(48.6 kJ/mol)高于CO2消耗的表观活化能(30.1 kJ/mol),这也证实了上述假设。根据反应机理,建立了 Langmuir-Hinshelwood 动力学速率模型,并且还通过非线性最小二乘回归方法估计了动力学参数。所开发的模型能够很好地拟合实验数据,R2高达0.965。DRM反应过程中CH4消耗的表观活化能高于CO2的表观活化能,确定速率决定步骤。建立了动力学速率模型,可以很好地描述实验。
更新日期:2019-11-29
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