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Highly active and stable Ni/SBA-15 catalysts prepared by a 'two solvents' method for dry reforming of methane

机译:通过“两种溶剂”方法制备的高活性和稳定的Ni / SBA-15催化剂,用于甲烷的重整

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摘要

Two series of Ni (2.5-7.5 wt%) and Ce (6 wt%) containing SBA-15 catalysts were prepared and tested in dry reforming of methane, a promising route for the production of syngas. Both Ni and Ce species were introduced in the organized mesoporous silica support in the form of nitrate salts using the "two solvents" procedure that is known to favor metal dispersion inside the porosity. Samples characterizations by N-2 sorption, SAXS, XRD, SEM and TEM indicate good preservation of the porosities after Ni deposition and calcination as well as formation of NiO nanoparticles entrapped in the porous channels. In the cerium-enriched samples, the CeO2 nanoparticles are also highly dispersed. After reduction, all the catalysts show high activity and selectivity towards H-2 and CO at atmospheric pressure with full CH4 conversion below 650 degrees C. In these conditions, there is no significant promotional effect by ceria. Moreover, prolonged tests performed at 500 degrees C for 12 h reveal a high stability of the catalysts. The absence of deactivation throughout the catalytic run at this temperature agrees with the low carbon amount detected after test and with the limited sintering of the Ni nanoparticles in the used catalysts. The positive effect of the SBA-15 mesoporous channels towards stabilization of the supported particles is discussed. (C) 2015 Elsevier Inc. All rights reserved.
机译:制备了两个系列的含Ni(2.5-7.5 wt%)和Ce(6 wt%)的SBA-15催化剂,并在甲烷的干重整中进行了测试,这是生产合成气的有希望的途径。使用已知有助于金属在孔隙内分散的“两种溶剂”方法,将Ni和Ce物种均以硝酸盐的形式引入到有组织的介孔二氧化硅载体中。通过N-2吸附,SAXS,XRD,SEM和TEM表征的样品特性表明,在Ni沉积和煅烧以及形成多孔通道中截留的​​NiO纳米颗粒后,孔隙率得到了很好的保留。在富铈样品中,CeO2纳米颗粒也高度分散。还原后,所有催化剂在大气压下均表现出对H-2和CO的高活性和选择性,并且在650摄氏度以下具有完全CH4转化率。在这些条件下,二氧化铈没有明显的促进作用。此外,在500摄氏度下进行的长时间测试12小时显示出催化剂的高稳定性。在此温度下整个催化过程中没有失活,这与测试后检测到的低碳量以及所用催化剂中Ni纳米粒子的有限烧结相一致。讨论了SBA-15中孔通道对稳定负载颗粒的积极作用。 (C)2015 Elsevier Inc.保留所有权利。

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