Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-08-21 , DOI: 10.1016/j.apcatb.2020.119459 André L.A. Marinho , Fabio S. Toniolo , Fabio B. Noronha , Florence Epron , Daniel Duprez , Nicolas Bion
Ni-based mesoporous mixed CeO2-Al2O3 oxide catalysts prepared by one pot Evaporation Induced Self Assembly (EISA) were tested in dry reforming of methane. The textural, structural and physicochemical properties of the catalysts were studied by N2 adsorption-desorption, TEM-EDS, XRD and elemental analysis. The mobility of oxygen in the structure and the redox properties were investigated by OSCC measurements, TPR and in situ DRIFTS. Finally, the post-reaction samples were analyzed by TGA, RAMAN and TEM. The calcined catalysts prepared by EISA method present mesoporous structures with highly dispersed Ni in the form of NiAl2O4 spinel clusters. After reduction, small size metallic Ni particles are observed (< 5 nm). The presence of Ce in the structure interacting strongly with Al2O3 promotes the oxygen mobility and acts as sites for CO2 adsorption, increasing the activity of the catalyst and promoting the carbon removal mechanism. In absence of Ce in the mesoporous alumina support, the activity for carbon gasification is limited and C filaments accumulate inside the reactor. The same behavior occurs with CeO2-Al2O3 oxide prepared by EISA method when Ni is post-impregnated because of the presence of isolated larger Ni particles which promotes the decomposition of CH4. Therefore, Ni-based CeO2-Al2O3 catalysts prepared by one pot EISA method exhibited high activity and stability for the dry reforming of methane thanks to both properties which are the confinement of Ni particles and the inhibition of carbon deposition.
中文翻译:
高活性和稳定的Ni分散在介孔CeO 2 -Al 2 O 3催化剂上,用于通过甲烷的干重整生产合成气
通过一锅蒸发诱导自组装(EISA)制得的镍基介孔混合CeO 2 -Al 2 O 3氧化物催化剂在甲烷的干重整中进行了测试。通过N 2吸附-脱附,TEM-EDS,XRD和元素分析研究了催化剂的结构,结构和理化性质。通过OSCC测量,TPR和原位DRIFTS研究了结构中氧的迁移率和氧化还原特性。最后,通过TGA,RAMAN和TEM分析反应后样品。通过EISA方法制备的煅烧催化剂呈现出具有NiAl 2 O 4形式的高度分散的Ni的介孔结构尖晶石簇。还原后,观察到小尺寸的金属Ni颗粒(<5 nm)。Ce在与Al 2 O 3强烈相互作用的结构中的存在促进了氧迁移率并充当了CO 2吸附的位点,从而增加了催化剂的活性并促进了除碳机理。在介孔氧化铝载体中不存在Ce的情况下,碳气化的活性受到限制,并且C丝堆积在反应器内部。当镍被后浸渍时,通过EISA方法制备的CeO 2 -Al 2 O 3氧化物会发生相同的行为,因为存在孤立的较大的Ni颗粒,该颗粒会促进CH 4的分解。。因此,通过一锅法EISA方法制备的Ni基CeO 2 -Al 2 O 3催化剂由于具有限制Ni颗粒的性质和抑制碳沉积的两种性能而对甲烷的干重整表现出高活性和稳定性。