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Effect of Pd doping in (Fe/Ni)/CeO2 catalyst for the reaction path in CO2 oxidative ethane dehydrogenation/reforming

Journal 2021 · IF 7.147 · 发表于 2021 年 6 月 17 日
作者: Xiuquan Li,Zhongqing Yang,Li Zhang,Ziqiang He,Ruiming Fang,Ziqi Wang,Yunfei Yan,Jingyu Ran
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摘要

The catalytic reaction of C 2 H 6 with CO 2 provides an opportunity to use shale gas and the greenhouse gas as source materials to produce ethylene through oxidative dehydrogenation or produce syngas through dry reforming . In this work, the reaction characteristics of ethane with CO 2 on Fe/Co/Ni/Cu monometallic catalysts and Pd-doped bimetallic catalysts were studied through activity test, kinetic analysis , catalyst characterization and DFT calculation. It is found that Pd–Fe 6 /CeO 2 has a high and stable C 2 H 4 selectivity of 80.4%, which is suitable for oxidative dehydrogenation reaction, while Ni 6 /CeO 2 has a large ethane/CO 2 conversion and a high CO selectivity of 96.5%, which is suitable for dry reforming reaction. For Fe-based catalyst, the doping of Pd form double active component structure. It only reduces the energy barrier of ethylene formation and CO 2 direct activation to provide O∗, but also increases the energy barrier of ethylene deep dehydrogenation, thus increasing the conversion of reactants and selectivity of C 2 H 4 . For Ni-based catalysts, the doping of Pd forms the alloy structure, which reduces the energy barrier of O∗-assisted dehydrogenation reaction and increases the conversion of reactants, but increases the energy barrier of C–C bond cleavage and CO 2 activation reaction, which reduces the selectivity of reforming to syngas.

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