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Enhancing the CO2 methanation activity of Ni/CeO2 via activation treatment-determined metal-support interaction
Journal of Energy Chemistry ( IF 13.1 ) Pub Date : 2020-11-19 , DOI: 10.1016/j.jechem.2020.11.011
Shuangxi Lin , Ziwen Hao , Jindong Shen , Xiao Chang , Shouying Huang , Maoshuai Li , Xinbin Ma

The metal-support interaction is of critical importance to enhance the catalytic activity and selectivity. However, it is still challenging to construct an appropriate interaction starting from the catalyst fabrication and/or activation. We herein established low-temperature treatment of Ni2+ ions impregnated on ceria in reductive atmosphere and reduction–oxidation cycles as effective approachs to regulate the metal-support interaction and raise the catalytic performance in the CO2 methanation. The proposed construction approach yielded Ni/CeO2 that displayed highly dispersed Ni nanoparticles in contact with CeO2 (111) and (100) facet, higher density of surface oxygen vacancies and larger amounts of weak basic sites relative to the reference samples, which increased the capacity for H2 and CO2 adsorption/activation. The interaction resulted in appreciably (2–3 fold) higher activity in the CO2 methanation with maintaining almost full selectivity to CH4 and high stability. Coverage of Ni surface by CeO2−x thin layer as a typical structure of strong metal-support interaction resulting from high-temperature reduction, can be alleviated via reduction–oxidation cycles. We also demonstrate the activation treatment-determined metal-support interaction effect can generally extend to (TiO2 and ZrO2) supported Ni catalysts.



中文翻译:

通过活化处理确定的金属-载体相互作用提高Ni / CeO 2的CO 2甲烷化活性

金属-载体相互作用对于增强催化活性和选择性至关重要。然而,从催化剂的制造和/或活化开始构建适当的相互作用仍然是挑战性的。我们在这里建立了在还原性气氛和还原-氧化循环中对浸渍在二氧化铈上的Ni 2+离子进行低温处理的方法,以此作为调节金属-载体相互作用并提高CO 2甲烷化催化性能的有效方法。拟议的构建方法产生了Ni / CeO 2,该Ni / CeO 2显示出与CeO 2接触的高度分散的Ni纳米颗粒(111)和(100)面,相对于参考样品,表面氧空位的密度更高,碱性位点的数量更多,这增加了H 2和CO 2吸附/活化的能力。这种相互作用在保持对CH 4几乎完全选择性和高稳定性的同时,使CO 2甲烷化的活性明显提高了(2-3倍)。CeO 2- x薄层覆盖镍表面是高温还原导致的强金属-载体相互作用的典型结构,可通过还原-氧化循环来缓解。我们还证明了活化处理确定的金属-载体相互作用效应通常可以扩展到(TiO 2和ZrO 2)负载的Ni催化剂。

更新日期:2020-12-23
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