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Interconnection between feed composition and Ni/Co ratio in (La-Ni-Co-O)-based perovskites and its effects on the stability of LPG steam reforming
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2017-11-20 , DOI: 10.1016/j.apcata.2017.11.011
Cícero N. Ávila-Neto , Kátia D. Oliveira , Kimberly F. Oliveira , Aline M.M. Arouca , Rondinele A.R. Ferreira , Carla E. Hori

Nickel-based perovskites (La-Ni-O) partially substituted with cobalt were tested for steam reforming of Liquefied Petroleum Gas (LPG), and analyzed by a series of in situ techniques. In situ X-ray diffraction (XRD) analyses showed that, depending on the fraction of substituted Ni, the perovskites go through one or two reduction stages before decomposing into Ni0/Co0 and La2O3. Extended X-ray absorption fine structure (EXAFS) data indicated that the nanoparticle’s surface are enriched with Co after reduction, but the Ni atoms migrate to the surface and overlay the former Co shell soon after feeding the LPG steam reforming mixture. In samples synthesized with a low Co/Ni ratio, the Ni surface layer oxidizes after a few hours under reaction conditions, showing signs of deactivation. The oxidation could be prevented by decreasing the water/LPG feed ratio, which reactivated the catalyst. The use of a proper water/LPG feed ratio coupled with the suitable Co/Ni ratio in the synthesis of perovskite precursors is essential to keep the catalysts active during LPG steam reform.



中文翻译:

(La-Ni-Co-O)基钙钛矿中进料组成与Ni / Co比的相互关系及其对LPG蒸汽重整稳定性的影响

对部分被钴取代的镍基钙钛矿(La-Ni-O)进行了液化石油气(LPG)蒸汽重整的测试,并通过一系列原位技术进行了分析。原位X射线衍射(XRD)分析表明,根据取代的Ni的比例,钙钛矿经历一到两个还原阶段,然后分解为Ni 0 / Co 0和La 2 O 3。。扩展的X射线吸收精细结构(EXAFS)数据表明,还原后,纳米颗粒的表面富含Co,但在喂入LPG蒸汽重整混合物后,Ni原子迁移到该表面并覆盖了原来的Co壳层。在以低Co / Ni比合成的样品中,在反应条件下几个小时后,Ni表面层会氧化,显示出失活的迹象。可以通过降低水/ LPG进料比来防止氧化,从而重新活化催化剂。在钙钛矿前体的合成中使用适当的水/ LPG进料比以及合适的Co / Ni比对于在LPG蒸汽重整过程中保持催化剂活性至关重要。

更新日期:2017-11-20
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