期刊
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
卷 -, 期 1, 页码 51-58出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.201800926
关键词
Zeolites; Mesoporous materials; Microporous materials; Acidity; Propylene selectivity
资金
- National Natural Science Foundation of China [U1510107, 21776297, 21403303]
- Shanghai Rising-Star Program [18QB1404500]
A series of hierarchically structured ZSM-5 zeolites (ZSM-5 HSZs) with a Si/Al ratio of about 200 have been successfully synthesized in the absence of additional mesoporous agents. XRD, N-2 sorption isotherms, SEM, TEM and NH3-TPD results showed that the obtained HSZs materials possess high crystallinity, interconnected micro/mesoporous structures and similar total acid amounts. Meanwhile, in the methanol-to-propylene (MTP) reaction, compared to the microporous counterpart, all synthesized ZSM-5 HSZs demonstrated superior performance benefitting from their hierarchical porous structures. Interestingly, Al-27 MAS NMR and Py-FTIR results confirmed the inter-transformation of framework and extra-framework Al species with the extension of materials crystallization duration and consequently the variation of materials surface acidity. As a result, the optimized catalyst achieved the highest initial propylene selectivity of 54.4 % and the longest catalyst lifetime (t(90)) of 175 h under the weight hourly space velocity (WHSV) of 1.0 g g(-1) h(-1). Moreover, a new in situ alkali etching-hydrothermal restoring mechanism has been proposed to elucidate the structural evolution of here reported high-silica ZSM-5 HSZs during the synthesis.
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