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Effects of calcination temperature and water-washing treatment on n-hexane hydroisomerization behavior of Pt-promoted sulfated zirconia based catalysts

机译:煅烧温度和水洗处理对Pt促进硫酸锆基催化剂正己烷氢代异构化行为的影响

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摘要

Synthesis of Pt-promoted sulfated zirconia catalyst Pt/SO4~(2-)/ZrO2 (designated as PSZ), Pt/SO4~(2-)/ZrO2-Al2O3 (designated as PSZA), and Pt/SO4~(2-)/ZrO2-Al2O3-Y2O3 (designated as PSZAY) was reported. These catalysts were characterized by N2 adsorption-desorption, thermal gravimetric (TG) analysis, NH3-temperature programmed desorption (NH3-TPD), and H2-temperature programmed reduction (H2-TPR) techniques. Effects of calcination temperature of the catalysts on the n-hexane hydroisomerization behavior were investigated in details. The experiment results revealed that the addition of Al and Y or Al promoter alone could improve the thermal stability of the catalysts. PSZA and PSZAY exhibited higher isomerization activity than unmodified PSZ as the calcination temperature of sulfated Zr(OH)4 was relatively high, for example, between 650 °C and 750 °C For the first time, it was found that water-washing treatment of PSZA and PSZAY at different preparation stages had considerably different impacts on their catalytic activity. Water-washing after calcination of the sulfated Zr(OH)4, the catalytic activity of PSZA and PSZAY was high, as indicated by approximately 80% of n-hexane conversion. However, water-washing before calcination of sulfated Zr(OH)4 led to a significant decrease in the catalytic activity of PSZA and PSZAY, that is, the n-hexane conversion diminished to around 35%. It was proposed that the presence of excessive sulfur species over sample was favorable for keeping the active sulfur species in the catalyst surface.
机译:合成PT促进的硫酸锆催化剂Pt / SO4〜(2 - )/ ZrO2(称为PSZ),Pt / SO4〜(2 - )/ ZrO2-Al2O3(称为PSZA),PT / SO4〜(2-报道/ ZrO2-Al2O3-Y2O3(指定为Pszay)。这些催化剂的特征在于N 2吸附 - 解吸,热重度(Tg)分析,NH3温度编程解吸(NH3-TPD)和H2温度编程(H2-TPR)技术。详细研究了催化剂对正己烷氢代异构化行为的煅烧温度的影响。实验结果表明,单独添加Al和Y或Al启动子可以改善催化剂的热稳定性。 PSZA和PSZAY表现出比未修饰的PSZ具有更高的异构化活性,因为硫酸化Zr(OH)4的煅烧温度是相对较高的,例如,首次在650℃和750℃之间,发现水洗涤处理不同制剂阶段的PSZA和PSZAY对其催化活性产生了相当不同的影响。煅烧硫酸化Zr(OH)4后的水洗,PSZA和Pszay的催化活性高,如大约80%的正己烷转化率所示。然而,硫酸化Zr(OH)4煅烧前的水洗导致Psza和Pszay的催化活性的显着降低,即,正己烷转化率降低至约35%。提出,在样品上存在过量的硫种类是有利于保持催化剂表面中的活性硫物质。

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