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聚合物衍生的SiOC作为镍基催化剂的载体材料:CO甲烷化性能及LaO对载体改性的影响

Polymer-derived SiOC as support material for Ni-based catalysts: CO methanation performance and effect of support modification with LaO.

作者信息

Szoldatits E, Essmeister J, Schachtner L, Konegger T, Föttinger K

机构信息

Institute of Materials Chemistry, TUWien, Vienna, Austria.

Institute of Chemical Technologies and Analytics, TUWien, Vienna, Austria.

出版信息

Front Chem. 2023 Mar 22;11:1163503. doi: 10.3389/fchem.2023.1163503. eCollection 2023.

Abstract

In this study, we investigated Ni supported on polymer-derived ceramics as a new class of catalyst materials. Catalysts have to withstand harsh reaction conditions requiring the use of a support with outstanding thermal and mechanical stability. Polymer-derived ceramics meet these requirements and bring the additional opportunity to realize complex porous structures. Ni-SiOC and La-modified Ni-SiOC catalysts were prepared by wet impregnation methods with target concentrations of 5 wt% for both metal and oxide content. Polymer-derived SiOC supports were produced using a photoactive methyl-silsesquioxane as preceramic polymer. Catalysts were characterized by N-adsorption-desorption, XRD, SEM, H-TPR, and DRIFTS. CO methanation was performed as a test reaction to evaluate the catalytic performance of these new materials at atmospheric pressure in the temperature range between 200°C and 400°C. XDR, H-TPR, and DRIFTS results indicate both improved dispersion and stability of Ni sites and increased adsorption capacities for CO in La-modified samples. Also, modified catalysts exhibited excellent performance in the CO methanation with CO conversions up to 88% and methane selectivity >99% at 300°C reaction temperature. Furthermore, the pyrolysis temperature of the support material affected the catalytic properties, the surface area, the stability of active sites, and the hydrophobicity of the surface. Overall, the materials show promising properties for catalytic applications.

摘要

在本研究中,我们研究了负载在聚合物衍生陶瓷上的镍作为一类新型催化剂材料。催化剂必须承受苛刻的反应条件,这需要使用具有出色热稳定性和机械稳定性的载体。聚合物衍生陶瓷满足这些要求,并为实现复杂的多孔结构带来了额外的机会。通过湿浸渍法制备了Ni-SiOC和La改性的Ni-SiOC催化剂,金属和氧化物含量的目标浓度均为5 wt%。使用光活性甲基倍半硅氧烷作为陶瓷前驱体聚合物制备聚合物衍生的SiOC载体。通过N吸附-脱附、XRD、SEM、H-TPR和DRIFTS对催化剂进行了表征。以CO甲烷化作为测试反应,在常压下于200°C至400°C的温度范围内评估这些新材料的催化性能。XDR、H-TPR和DRIFTS结果表明,La改性样品中Ni位点的分散性和稳定性得到改善,CO的吸附容量增加。此外,改性催化剂在CO甲烷化反应中表现出优异的性能,在300°C反应温度下CO转化率高达88%,甲烷选择性>99%。此外,载体材料的热解温度影响催化性能、表面积、活性位点的稳定性和表面疏水性。总体而言,这些材料在催化应用方面显示出有前景的性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f554/10073567/c66ff26d0a23/fchem-11-1163503-g001.jpg

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