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Synthesis of Mesoporous γ-Al2O3 with Spongy Structure: In-Situ Conversion of Metal-Organic Frameworks and Improved Performance as Catalyst Support in Hydrodesulfurization

机译:海绵结构介孔γ-Al2O3的合成:金属有机骨架的原位转化和作为加氢脱硫催化剂载体的改进性能

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摘要

Over the past decades, extensive efforts have been devoted to modulating the textural properties, morphology and microstructure of γ-Al2O3, since the physiochemical properties of γ-Al2O3 have close correlations with the performance of hydrotreating catalysts. In this work, a spongy mesoporous γ-alumina (γ-Al2O3) was synthesized using Al-based metal-organic frameworks (Al-MOFs) as precursor by two-step pyrolysis, and this Al-MOF-derived γ-Al2O3 was used as hydrodesulfurization (HDS) catalyst support, to explore the effect of support on the HDS performance. Compared with industrial γ-Al2O3, the spongy alumina displayed well-developed porosity with relatively high surface area, large pore volume, and abundant weak Lewis acid sites. Based on catalyst characterization and performance evaluation, sulfurized molybdenum and cobalt molecules were able to incorporate and highly disperse into channels of the spongy mesoporous alumina, increasing the dispersion of active catalytic species. The spongy γ-Al2O3 was also able to enhance the diffusion efficiency and mass transfer of reactant molecules due to its improved texture properties. Therefore, the corresponding catalyst presented higher activities toward HDS of dibenzothiophene (DBT) than that from industrial alumina. The spongy mesoporous γ-alumina synthesized by Al-MOFs provides a new alternative to further develop novel γ-alumina materials with different texture and various nanoporous structures, considering the diversity of MOFs with different compositions, topological structures, and morphology.
机译:在过去的几十年中,由于γ-Al2O3的物理化学性质与加氢处理催化剂的性能密切相关,因此人们已经在调节γ-Al2O3的质地,形态和微观结构方面进行了广泛的努力。在这项工作中,以铝基金属有机骨架(Al-MOFs)为前体,通过两步热解合成了海绵状介孔γ-氧化铝(γ-Al2O3),并使用了这种由Al-MOF衍生的γ-Al2O3作为加氢脱硫(HDS)催化剂的载体,以探讨载体对HDS性能的影响。与工业γ-Al2O3相比,海绵状氧化铝显示出良好的孔隙率,具有相对较高的表面积,较大的孔体积和丰富的弱路易斯酸位。基于催化剂的表征和性能评估,硫化的钼和钴分子能够并入并高度分散在海绵状中孔氧化铝的通道中,从而增加了活性催化物质的分散性。海绵状的γ-Al2O3由于其改善的织构特性,还能够提高反应物分子的扩散效率和传质。因此,与工业氧化铝相比,相应的催化剂对二苯并噻吩(DBT)的HDS活性更高。 Al-MOFs合成的海绵状介孔γ-氧化铝为进一步开发具有不同质地和纳米多孔结构的新型γ-氧化铝材料提供了新的选择,考虑到不同成分,拓扑结构和形态的MOF的多样性。

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