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Pt nanoparticles embedded in CeO2 and CeZrO2 catalysts for biogas upgrading: Investigation on carbon removal mechanism by oxygen isotopic exchange and DRIFTS
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2021-05-13 , DOI: 10.1016/j.jcou.2021.101572
André L.A. Marinho , Raimundo C. Rabelo-Neto , Florence Epron , Nicolas Bion , Fabio B. Noronha , Fabio Souza Toniolo

This work investigated the effect of Pt nanoparticles embedded into CeO2 (Pt@CeO2) and CeZrO2 (Pt@CeZrO2) on the carbon removal mechanism for the dry reforming of methane, in comparison to impregnated Pt/CeO2. Morphological and structural characterization by TEM and Raman spectroscopy showed that Pt sintering is suppressed on both structures and the doping with Zr led to the CeZrO2 solid solution formation. A combination of TPR, oxygen isotopic exchange and DRIFTS measurements demonstrated that embedded Pt nanoparticles interact more strongly with ceria than supported Pt, and as a consequence, reactive lattice oxygen becomes more abundant on the catalyst surface, promoting the mechanism of carbon gasification over Pt nanoparticle. The low availability of oxygen species on Pt/CeO2 resulted in higher carbon formation, as demonstrated by TPO analysis. Therefore, the Pt@CeO2 and Pt@CeZrO2 catalysts were more resistant to coke formation due to the higher presence of reactive oxygen species at the metal-support interface, promoting the balance between the rates of carbon formation and carbon gasification over Pt nanoparticle.



中文翻译:

嵌入CeO 2和CeZrO 2催化剂中的Pt纳米颗粒用于沼气提纯:通过氧同位素交换和DRIFTS进行碳去除机理的研究

与浸渍的Pt / CeO 2相比,这项工作研究了嵌入CeO 2(Pt @ CeO 2)和CeZrO 2(Pt @ CeZrO 2)中的Pt纳米颗粒对甲烷干重整的脱碳机理的影响。通过TEM和拉曼光谱的形态和结构表征表明,在两种结构上均抑制了Pt烧结,并且Zr的掺杂导致了CeZrO 2。固溶体的形成。TPR,氧同位素交换和DRIFTS测量的结合表明,包埋的Pt纳米粒子与二氧化铈的相互作用比负载的Pt更强,因此,反应性晶格氧在催化剂表面上变得更加丰富,从而促进了碳气化的机理超过了Pt纳米粒子。 。TPO分析表明,Pt / CeO 2上氧种类的低可用性导致较高的碳形成。因此,Pt @ CeO 2和Pt @ CeZrO 2催化剂对焦炭形成的抵抗力更高,因为在金属-载体界面上存在更高的活性氧种类,从而促进了碳形成速率与Pt纳米颗粒上的碳气化速率之间的平衡。 。

更新日期:2021-05-13
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