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Synthesis, characterization and catalytic performances of Ce-SBA-15 supported nickel catalysts for methane dry reforming to hydrogen and syngas

机译:Ce-sBa-15负载镍催化剂的合成,表征及催化性能,用于甲烷干重整制氢和合成气

摘要

A series of Ce-incorporated SBA-15 mesoporous materials were synthesized through direct hydrothermal synthesis method and further impregnated with 12 wt.% Ni. The samples were characterized by ICP-AES, XRD, N-2 physisorption, XPS, TPR, H-2 chemisorption, TGA, temperature-programmed hydrogenation (TPH) and TEM measurements. The low-angle XRD and N-2 physisorption results showed the Ce successfully incorporated into the framework of SBA-15. The catalytic properties of these catalysts were investigated in methane reforming with CO2. The Ce/Si molar ratio had a significant influence on the catalytic performance. The highest catalytic activity and long-term stability were obtained over the Ni/Ce-SBA-15 (Ce/Si = 0.04) sample. The improved catalytic behavior could be attributed to the cerium impact in the framework of SBA-15, where cerium promoted the dispersion of nano-sized Ni species and inhibited the carbon formation. In comparison with the effect of CeO2 crystallites in SBA-15, cerium in the framework of SBA-15 promoted the formation of the nickel metallic particles with smaller size. The XRD and TGA results exhibited that carbon deposition was responsible for activity loss of Ni/SBA-15 and Ni/Ce-SBA-15 (Ce/Si = 0.06) catalysts. TEM results showed that the hexagonal mesopores of SBA-15 were still kept intact after reaction and the pore walls of SBA-15 prevented the aggregation of nickel. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
机译:通过直接水热合成法合成了一系列掺Ce的SBA-15介孔材料,并进一步浸渍了12 wt%的Ni。通过ICP-AES,XRD,N-2物理吸附,XPS,TPR,H-2化学吸附,TGA,程序升温氢化(TPH)和TEM测量来表征样品。低角度XRD和N-2的物理吸附结果表明Ce成功地掺入了SBA-15的骨架中。在用CO2进行甲烷重整中研究了这些催化剂的催化性能。 Ce / Si摩尔比对催化性能有重要影响。在Ni / Ce-SBA-15(Ce / Si = 0.04)样品上获得了最高的催化活性和长期稳定性。改善的催化性能可归因于SBA-15框架中的铈影响,其中铈促进了纳米尺寸Ni物种的分散并抑制了碳的形成。与CeO2微晶在SBA-15中的作用相比,铈在SBA-15的框架内促进了尺寸较小的镍金属颗粒的形成。 XRD和TGA结果表明,碳沉积是Ni / SBA-15和Ni / Ce-SBA-15(Ce / Si = 0.06)催化剂活性下降的原因。 TEM结果表明,SBA-15的六角形中孔在反应后仍保持完整,SBA-15的孔壁阻止了镍的聚集。 Hydrogen Energy Publications,LLC版权所有(C)2011。由Elsevier Ltd.出版。保留所有权利。

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