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Kinetics and mechanistic studies of methane dry reforming over Ca promoted 1Co–1Ce/AC-N catalyst

Journal 2020 · IF 4.939 · 发表于 2020 年 10 月 19 日
作者: Yinghui Sun,Guojie Zhang,Haizhu Cheng,Jun Liu,Guoqiang Li
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摘要

The mechanism and kinetic features of dry reforming with methane (DRM) over Ca promoted 1Co–1Ce/AC-N catalyst was investigated. The mechanistic pathway studies have conducted by FTIR and XPS analysis, structure-activity correlations demonstrated the CH 4 and CO 2 could adsorb on catalyst active sites and generate intermediate CH x , OH and CH x O, continue to generate CO and H 2 and then desorbed from active sites. Moreover, CH 4 could also oxidized by Ce 4+ and CO 2 reduced by Ce 3+ , the same content of Ce 4+ and Ce 3+ on promoted catalyst greatly improved the reaction rate. The kinetic of dry reforming with methane was examined for temperature between 650 and 850 at 800 °C. The research was carried out by changing the CH 4 /CO 2 ratios between 0.3 and 3.0. The obtained experiment data were fitted by three typical kinetic models (Power Law, Eley-Rideal and Langmuir-Hinshelwood), the fitting results demonstrated that the best prediction of reforming rates can provided by Langmuir-Hinshelwood model for the reaction temperatures between 650 and 800 °C. Moreover, activation energies of methane and carbon dioxide consumption were −117 and −47 kJ/mol, indicating that much higher energy barrier is needed for methane activation compared to carbon dioxide.

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