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Theoretical study on the reaction mechanism of carbon dioxide reforming of methane on La and La2O3 modified Ni(1 1 1) surface
Journal of Catalysis ( IF 7.3 ) Pub Date : 2018-06-13 , DOI: 10.1016/j.jcat.2018.05.026
Kai Li , Feng He , Hongmei Yu , Ying Wang , Zhijian Wu

The carbon dioxide (dry) reforming of methane (DRM) (CH4 + CO2 → 2CO + 2H2) on La and La2O3 modified Ni(1 1 1) has been investigated theoretically. As promoters, La and La2O3 strengthen the adsorption of the intermediates compared with pure Ni(1 1 1). The strong adsorption of CO2 on La2O3 modified Ni(1 1 1) deforms La2O3, and the complex intermediate CO2(La2O2-O) is formed. The CO2(La2O2-O) participates in the DRM reaction and reduces the carbon deposition on the catalyst surface. For La and La2O3 modified Ni(1 1 1), the reactions of CH4 + CO2 → CH + 3H + CO + O → CHO + 3H + CO → 2CO + 2H2 and CH4 + CO2 + La2O3 → CH + CO2(La2O2-O) + 3H → CHO + CO2(La2O2) + 3H → 2CO + 2H2 + La2O3 are the most favorable pathways for DRM, respectively. Both the density functional study and microkinetic analysis support that compared with pure Ni(1 1 1), La and La2O3 modified Ni(1 1 1) improve the reaction both thermodynamically and kinetically. The carbon deposition is suppressed on La2O3 modified Ni(1 1 1) due to the lower rate in the reaction CH → C + H, compared with La modified Ni(1 1 1).



中文翻译:

La和La 2 O 3修饰的Ni(1 1 1)表面甲烷二氧化碳重整反应机理的理论研究

理论上研究了La和La 2 O 3改性Ni(1 1 1)上甲烷(DRM)的二氧化碳(干式)重整(CH 4  + CO 2  →2CO + 2H 2)。与纯Ni(1 1 1)相比,La和La 2 O 3作为促进剂可增强中间体的吸附。CO 2在La 2 O 3修饰的Ni(1 1 1)上的强吸附使La 2 O 3变形,并形成复杂的中间CO 2(La 2 O 2 -O)。CO 2(La 2 O 2-O)参与DRM反应并减少碳在催化剂表面上的沉积。对于La和La 2 O 3修饰的Ni(1 1 1),CH 4  + CO 2  →CH + 3H + CO + O→CHO + 3H + CO→2CO + 2H 2和CH 4  + CO 2  + La的反应2 O 3  →CH + CO 2(La 2 O 2 -O)+ 3H→CHO + CO 2(La 2 O 2)+ 3H→2CO + 2H 2  + La 2 O 3分别是DRM的最有利途径。与纯Ni(1 1 1),La和La 2 O 3修饰的Ni(1 1 1)相比,密度泛函研究和微动力学分析均支持该反应在热力学和动力学上均改善了反应。与La修饰的Ni(1 1 1)相比,由于反应CH→C + H的速率较低,因此在La 2 O 3修饰的Ni(1 1 1)上抑制了碳沉积。

更新日期:2018-06-13
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