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Effect of isomorphic substitution of zirconium on mesoporous silica as support for Cobalt Fischer-Tropsch synthesis catalysts

机译:介孔二氧化硅上锆的同晶取代对费-托合成钴催化剂的影响

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Isomorphic substituted mesoporous SBA-15 with zirconium at Zr/Si atomic ratios of1/100, 1/50, 1/20, 1/8 and 1/3 have been successfully synthesized. It was demonstrated thatthe Zr4+ ions were introduced into the framework of SBA-15 with the hexagonal array ofuniform tubular channel configuration intact until Zr/Si ratio of 1/20. Another sample ofzirconium incipient wetness impregnated SBA-15 with Zr/Si ratio of 1/20 was prepared forcomparison. These mesoporous materials were loaded with 10 wt % cobalt by incipientwetness impregnation and characterized by XRD, TEM, N2 absorption–desorption,UV-visible, H2-TPR, H2-TPD, O2 titration as well as XPS. It was shown that introductionof zirconium increased the density of surface cobalt, improved the cobalt reducibility andgenerated more available active sites with low zirconium content (Zr/Si atomic ratio <1/20). At high zirconium content, strong interaction between the cobalt species and thesurface of the support was formed, to decrease cobalt reducibility detected by XPS andH2-TPR. The catalytic performances of catalysts for FTS were tested in a fixed bed reactor,and the isomorphic substituted mesoporous SBA-15 with zirconium at Zr/Si ratio of 1/20supported cobalt catalyst showed the best performance.
机译:Zr / Si原子比为Zr的同晶取代的介孔SBA-15 1 / 100、1 / 50、1 / 20、1 / 8和1/3已成功合成。事实证明, Zr4 +离子被引入SBA-15骨架中,其六边形排列为 均匀的管状通道结构保持完整,直到Zr / Si比为1/20。的另一个样本 制备Zr / Si比为1/20的锆初湿浸渍SBA-15 比较。这些中孔材料在初始时就装载了10 wt%的钴 湿润浸渍,并通过XRD,TEM,N2吸收-解吸, 紫外可见光,H2-TPR,H2-TPD,O2滴定以及XPS。被证明介绍 锆增加了表面钴的密度,提高了钴的还原能力, 生成更多可用的低锆含量的活性位点(Zr / Si原子比< 1/20)。锆含量高时,钴物种与金属间的强相互作用 形成了载体的表面,以降低XPS和 H2-TPR。在固定床反应器中测试了FTS催化剂的催化性能, Zr / Si比为1/20的锆同晶取代的介孔SBA-15 负载型钴催化剂表现出最好的性能。

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