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Kinetic study of reactive sorption-enhanced reforming of coke oven gas for hydrogen production

机译:焦炉煤气反应吸附增强重整制氢的动力学研究

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The kinetic behavior of reactive sorption-enhanced reforming (ReSER) process of coke oven gas (COG) for hydrogen production was investigated. Experimental studies were performed on a laboratory-scale fixed-bed reactor with a Ni-nano-CaO/Al2O3 sorption complex catalyst. Based on hypothesis that the surface reaction of steam methane reforming in the ReSER-COG process is the rate-determining step, a reaction kinetic model of the reforming reaction of the ReSER-COG process was established. The kinetic data of the methane conversion were obtained under a reaction temperature from 560 degrees C to 680 degrees C, a residue time of 0.0417-0.0105 g min.mL(-1), a steam-to-methane molar ratio of 4, and a reaction pressure of 0.1 MPa. The mean relative deviation of the methane conversion between the data from the simulated model and those from the experiments was determined to be 4.58%, which illustrates a good fit of the established model with the experimental data and confirmed the rationality of the hypothesis that the surface reaction of methane reforming in ReSER-COG process is rate-determining step. The calculation results show that the reforming reaction activation energy in ReSER-COG process is 95 kJ mol(-1), nearly 145 kJ mol(-1) decreased compared with the steam methane reforming without sorption-enhancement. This explains the reason that higher methane conversion rate at a lower reaction temperature observed in the ReSER-COG process. (C) 2015 Elsevier B.V. All rights reserved.
机译:研究了用于生产氢气的焦炉煤气(COG)的反应吸附增强重整(ReSER)过程的动力学行为。实验研究是在具有Ni-nano-CaO / Al2O3吸附复合催化剂的实验室规模固定床反应器上进行的。基于ReSER-COG工艺中蒸汽甲烷重整的表面反应是速率决定步骤的假设,建立了ReSER-COG工艺重整反应的反应动力学模型。在560℃至680℃的反应温度下,残留时间为0.0417-0.0105 g min.mL(-1),水蒸气与甲烷的摩尔比为4,以及反应压力为0.1 MPa。确定的模拟模型数据与实验数据之间的甲烷转化率的平均相对偏差为4.58%,这说明所建立的模型与实验数据吻合良好,并证实了表面假说的合理性ReSER-COG工艺中甲烷重整反应是决定速率的步骤。计算结果表明,与不进行吸附增强的蒸汽甲烷重整相比,ReSER-COG工艺的重整反应活化能为95 kJ mol(-1),降低了近145 kJ mol(-1)。这解释了在ReSER-COG工艺中以较低的反应温度观察到较高的甲烷转化率的原因。 (C)2015 Elsevier B.V.保留所有权利。

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