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Nickel supported on YSZ: The effect of Ni particle size on the catalytic activity for CO2 methanation
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2017-12-06 , DOI: 10.1016/j.jcou.2017.11.015
Jagadesh Kopula Kesavan , Igor Luisetto , Simonetta Tuti , Carlo Meneghini , Giovanna Iucci , Chiara Battocchio , Settimio Mobilio , Stefano Casciardi , Renata Sisto

The catalytic conversion of carbon dioxide to synthetic CH4 was studied on five Ni/YSZ samples, with the same nickel loading (10 wt%) but different Ni particle size. The catalysts, prepared by different methods, were characterized combining morphological (BET, TEM), structural (XRD, in-operando XAS), electronic (XPS, in-operando XANES) analysis and H2-TPR experiments. The results showed that catalytic activity and CH4 selectivity depended on size and morphology of Ni particles, and that type and amount of deposited carbon strongly depended on Ni0 morphology. The kinetic measurements revealed that both H2 and CO2 reactants were activated on Ni sites, and that YSZ support was not directly involved in the reaction mechanism.

The most efficient catalyst was that prepared by wet impregnation with Ni(EDTA)2− complex due to the high Ni0 dispersion.This catalyst showed low amount of carbon and remarkable stability over time on stream. In-operando XAS showed that it did not undergo deactivation by Ni0 → Ni2+ oxidation using high CO2 concentration, thus it is applicable in dynamic conditions like those typical in the energy storage from renewable sources process.



中文翻译:

YSZ上负载的镍:Ni粒径对CO 2甲烷化催化活性的影响

在五个镍/ YSZ样品上研究了二氧化碳到合成CH 4的催化转化,其中镍负载量相同(10 wt%),但镍粒度不同。通过形态分析(BET,TEM),结构分析(XRD,操作数内XAS),电子分析(XPS,操作数内XANES)和H 2 -TPR实验,对用不同方法制备的催化剂进行了表征。结果表明,催化活性和CH 4选择性取决于Ni颗粒的大小和形态,而沉积碳的类型和数量则强烈取决于Ni 0形态。动力学测量表明,H 2和CO 2均 反应物在Ni位点上被激活,并且YSZ载体不直接参与反应机理。

最有效的催化剂是由于Ni 0的高分散性,通过用Ni(EDTA)2−络合物进行湿浸渍制备的催化剂,该催化剂显示出低的碳含量和长期的运行稳定性。In-operando XAS研究表明,它不会因使用高CO 2浓度的Ni 0  →Ni 2+氧化而失活,因此它适用于动态条件,例如可再生资源过程中的典型能量存储。

更新日期:2017-12-06
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