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CO2 reforming of methane over supported LaNiO3 perovskite-type oxides
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2017-09-11 , DOI: 10.1016/j.apcatb.2017.09.022
R.C. Rabelo-Neto , H.B.E. Sales , C.V.M. Inocêncio , E. Varga , A. Oszko , A. Erdohelyi , F.B. Noronha , L.V. Mattos

This work investigated the performance of supported LaNiO3 perovskite-type oxides for the CO2 reforming of methane. The methane and CO2 conversion increased at the beginning of reaction for LaNiO3 and LaNiO3/Al2O3 catalysts. On the other hand, conversion remained quite constant for LaNiO3/CeSiO2. in situ XPS experiments under reaction conditions revealed that the metallic Ni particles were oxidized by CO2 from the feed for LaNiO3 and LaNiO3/Al2O3 catalysts. Ceria support was preferentially oxidized, limiting the oxidation of the metallic phase. Raman spectroscopy and thermogravimetric analysis showed that carbon was formed mainly over LaNiO3 and LaNiO3/Al2O3 catalysts. Supporting LaNiO3 over CeSiO2 almost completely suppressed carbon deposition. in situ XPS experiments showed a continuous change of ceria oxidation states between Ce4+ and Ce3+ under reaction conditions. This result in a high oxygen mobility of ceria support that reacts with carbon, inhibiting the formation of nickel carbide and consequently the nucleation and growth of carbon filaments.

中文翻译:

负载型LaNiO 3钙钛矿型氧化物上甲烷的CO 2重整

这项工作研究了负载的LaNiO 3钙钛矿型氧化物对甲烷CO 2重整的性能。对于LaNiO 3和LaNiO 3 / Al 2 O 3催化剂,在反应开始时甲烷和CO 2转化率增加。另一方面,LaNiO 3 / CeSiO 2的转化率保持相当恒定。反应条件下的原位XPS实验表明,金属Ni颗粒被LaNiO 3和LaNiO 3 / Al 2 O 3进料中的CO 2氧化催化剂。二氧化铈载体被优先氧化,限制了金属相的氧化。拉曼光谱和热重分析表明,碳主要在LaNiO 3和LaNiO 3 / Al 2 O 3催化剂上形成。在CeSiO 2上负载LaNiO 3几乎完全抑制了碳沉积。原位XPS实验表明Ce 4+和Ce 3+之间二氧化铈氧化态的连续变化在反应条件下。这导致二氧化铈载体的高氧迁移率,其与碳反应,抑制了碳化镍的形成,从而抑制了碳丝的成核和生长。
更新日期:2017-09-11
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