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蒸汽处理和 SiO₂ 表面钝化对 SSZ-13 沸石在乙烯丙烯反应中的影响。

Effects of Steaming and SiO₂ Surface Passivation on SSZ-13 Zeolites in the Ethylene to Propylene Reaction.

机构信息

Carbon Resources Institute, Korea Research Institute of Chemical Technology, 141 Gajeong-ro, Yusong, Daejeon 34114, Republic of Korea.

Center for Convergent Chemical Process, Korea Research Institute of Chemical Technology, 141 Gajeong-ro, Yusong, Daejeon 34114, Republic of Korea.

出版信息

J Nanosci Nanotechnol. 2020 Sep 1;20(9):5783-5786. doi: 10.1166/jnn.2020.17644.

Abstract

SSZ-13 zeolite was modified by two kinds of post-treatment methods such as steaming and SiO₂ surface passivation (silylation) for ETP catalyst with high activity. The former steaming treatment was conducted in the range of 400-700 °C, whereas the latter surfaces passivation was applied to a chemical liquid deposition (CLD) technique that uses various silylation agents such as tetramethylorthosilicate (TMOS), tetraethylorthosilicate (TEOS), and tetrabuthylorthosilicate (TBOS). Catalysts were characterized by powder-XRD, ICP, Ar-phsisorption, solid-state Al MAS NMR, and NH₃-TPD, and their activities were tested in fixed bed reaction system. Regarding the effects of steaming temperature, the results show that a relatively higher selectivity is observed in SSZ-13 catalysts treated at proper steaming temperatures such as 450 and 500 °C compared to parent and other steam treated catalysts. For optimum surface passivation treatments for ETP reactions, one-step surface passivation using TEOS agents among various passivation agents led to enhanced propylene selectivity to 80% when compared with parent and other silylated SSZ-13 catalysts. However, a sequential passivation treatment with a TEOS agent was not highly affected by the reaction activity.

摘要

SSZ-13 沸石通过蒸汽处理和 SiO₂表面钝化(硅烷化)这两种后处理方法进行改性,以制备具有高活性的 ETP 催化剂。前者的蒸汽处理在 400-700°C 的范围内进行,而后者的表面钝化则采用化学液沉积(CLD)技术,使用各种硅烷化剂,如四甲基原硅酸酯(TMOS)、四乙氧基硅烷(TEOS)和四丁氧基硅烷(TBOS)。采用粉末 XRD、ICP、Ar 吸附、固态 Al MAS NMR 和 NH₃-TPD 对催化剂进行了表征,并在固定床反应系统中测试了它们的活性。关于蒸汽处理温度的影响,结果表明,与母体和其他蒸汽处理的催化剂相比,在适当的蒸汽处理温度(如 450 和 500°C)下处理的 SSZ-13 催化剂具有相对较高的选择性。对于 ETP 反应的最佳表面钝化处理,与母体和其他硅烷化 SSZ-13 催化剂相比,各种钝化剂中使用 TEOS 试剂进行一步表面钝化处理可将丙烯选择性提高到 80%。然而,使用 TEOS 试剂的顺序钝化处理对反应活性的影响不大。

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