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Synthesis and stability evaluation of hierarchical silicoaluminophosphates with different structural frameworks in the methanol to olefins process
Particuology ( IF 3.5 ) Pub Date : 2017-09-28 , DOI: 10.1016/j.partic.2017.06.004
Seyed Hesam Mousavi , Shohreh Fatemi , Marjan Razavian

Silicoaluminophosphates (SAPOs) with different pore structures were synthesized through the implementation of polyethylene glycol (PEG) as a mesopores impregnation agent. Using PEGs with different molecular weights (MWs) and concentrations in the synthesis precursor, several samples were synthesized and characterized. Applying a PEG capping agent to the precursors led to the formation of tuned mesopores within the microporous matrix of the SAPO. The effects of the PEG molecular weight and PEG/Al molar ratio were investigated to maximize the efficiency of the catalyst in the methanol-to-olefin (MTO) process. Using PEG with a MW of 6000 resulted in the formation of both Zeolite Rho and chabazite structural frameworks (i.e., DNL-6 and SAPO-34). Pure SAPO-34 samples were successfully prepared using PEG with a MW of 4000. Our results showed that the PEG concentrations affect the porosity and acidity of the synthesized materials. Furthermore, the SAPO-34 sample synthesized with PEG (MW of 4000) and a PEG/Al molar ratio of 0.0125 showed a superior catalytic stability in the MTO reaction owing to the tuned bi-modal porosity and tailored acidity pattern. Finally, through reactivation experiments, it was found that the catalyst is stable even after several regeneration cycles.



中文翻译:

甲醇制烯烃过程中具有不同结构骨架的分级硅铝磷酸盐的合成与稳定性评价

通过将聚乙二醇(PEG)用作中孔浸渍剂,合成了具有不同孔结构的硅铝磷酸盐(SAPO)。使用在合成前体中具有不同分子量(MWs)和浓度的PEG,合成并表征了几个样品。将PEG封端剂应用于前体导致在SAPO的微孔基质内形成调节的中孔。研究了PEG分子量和PEG / Al摩尔比的影响,以最大程度地提高甲醇制烯烃(MTO)工艺中催化剂的效率。使用分子量为6000的PEG导致形成了Zeolite Rho和菱沸石结构骨架(即DNL-6和SAPO-34)。使用分子量为4000的PEG成功制备了纯SAPO-34样品。我们的结果表明,PEG浓度会影响合成材料的孔隙率和酸度。此外,归因于双峰孔隙率和定制的酸度模式,用PEG(分子量为4000)和PEG / Al摩尔比为0.0125合成的SAPO-34样品在MTO反应中显示出优异的催化稳定性。最后,通过再活化实验,发现即使在几个再生循环后,催化剂也是稳定的。

更新日期:2017-09-28
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