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Enhanced activity and stability of Ni/La2O2CO3 catalyst for CO2 methanation by metal-carbonate interaction
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-06-24 , DOI: 10.1016/j.apcatb.2020.119271
Yihu Dai , Min Xu , Qiaojuan Wang , Rui Huang , Yunyun Jin , Bo Bian , Chantsalmaa Tumurbaatar , Bolormaa Ishtsog , Tungalagtamir Bold , Yanhui Yang

The interaction between metal and support is critical for CO2 methanation reaction over supported Ni catalysts. This work provides a modification strategy using surface carbonate species for promoting the catalytic performances of lanthana-supported Ni catalyst. The carbonate-modified Ni/La2O2CO3 catalyst displays a superior catalytic activity, stability, and CO tolerance in CO2 methanation reactions in comparison with Ni/La2O3 catalyst. The structure of Ni-La2O2CO3 interfaces is verified to be stable against thermal decomposition and reduction reaction, determining catalytic roles through specific metal-carbonate interaction. The medium-strength surface basicity promotes the capability of CO2 chemisorption. The carbonate-modified interfaces facilitate the formation of monodentate and bidentate formates as the reaction intermediates. These species are highly reactive for further transformation into CH4 even in the presence of CO poison, which is benefited to both methanation activity and anti-CO ability.



中文翻译:

通过金属碳酸盐相互作用提高Ni / La 2 O 2 CO 3催化剂用于CO 2甲烷化的活性和稳定性

金属和载体之间的相互作用对于负载型Ni催化剂上的CO 2甲烷化反应至关重要。这项工作提供了一种使用表面碳酸盐种类的改性策略,以促进镧系负载的Ni催化剂的催化性能。与Ni / La 2 O 3催化剂相比,碳酸盐改性的Ni / La 2 O 2 CO 3催化剂在CO 2甲烷化反应中显示出优异的催化活性,稳定性和CO耐受性。Ni-La 2 O 2 CO 3的结构界面经验证对热分解和还原反应稳定,并通过特定的金属碳酸盐相互作用确定催化作用。中等强度的表面碱性提高了CO 2化学吸附能力。碳酸盐改性的界面促进了单齿和双齿甲酸酯作为反应中间体的形成。这些物种即使在存在CO毒物的情况下也具有很高的反应性,可以进一步转化为CH 4,这对甲烷化活性和抗CO能力均有利。

更新日期:2020-06-29
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