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Amine-free synthesis of high-silica ZSM-5 assisted with calcined silicalite-1 and ethanol with the investigation of mechanism.
- Source :
-
Microporous & Mesoporous Materials . Jul2024, Vol. 375, pN.PAG-N.PAG. 1p. - Publication Year :
- 2024
-
Abstract
- Amine-free synthesis of high silica ZSM-5 with high crystallinity and well-defined morphology was challenging. In this work, ZSM-5 with the fed silica-alumina ratio (SAR) of 100 was rapidly synthesized with the assistance of the calcined silicalite-1 seed and ethanol, and their crystal structures, morphology and microporous properties were characterized by XRD, SEM, FT-IR, ICP and N 2 adsorption-desorption and so on. Firstly, the crystallization temperature was optimized between 140 and 180 °C at a certain alkalinity and ethanol content, and 160 °C was selected to not only provide high crystallization rate but also ensure the stability of high-silica skeleton. Secondly, the influences of the EtOH/SiO 2 ratio, Na 2 O/SiO 2 ratio and crystallization time on the crystallization of high-silica ZSM-5 were investigated at 160 °C. The results showed well-crystalline high-silica ZSM-5 could be synthesized within a wide range of the EtOH/SiO 2 ratios (0.5–2.0) and the increase of ethanol content slightly inhibited the growth of ZSM-5 along b-axial of hexagonal prisms due to the preferential adsorption of excess ethanol on the {010} crystal plane and the formation of Si–O–C 2 H 5 ; high alkalinity was favorable for the preparation of a small-sized and well-crystalline ZSM-5 due to the rapid depolymerization of calcined seed and the contribution of mass nucleation sites; meanwhile, excellent micropore characteristic of high-silica ZSM-5 further proved that the synthetic strategy of seed + ethanol was feasible. Finally, the synergistic action mechanism of calcined seed and ethanol for the synthesis of high-silica ZSM-5 was revealed that silicalite-1 with MFI structure unit combined with Na+(H 2 O/EtOH) with larger radius were very important for rapidly assembly of a large number of silica species into MFI framework. [Display omitted] • Complete amine-free synthesis of high-silica ZSM-5 was achieved via calcined silicalite-1 as seed. • High alkalinity can promote the depolymerization of silicalite-1 to obtain smaller-sized ZSM-5. • Silicalite-1+ethanol route could effectively inhibit magadiite and obtain high-crystalline ZSM-5. • Synergistic assembly mechanism of silicalite-1 and Na+(H 2 O/EtOH) with a large radius was put forward. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 13871811
- Volume :
- 375
- Database :
- Academic Search Index
- Journal :
- Microporous & Mesoporous Materials
- Publication Type :
- Academic Journal
- Accession number :
- 177484628
- Full Text :
- https://doi.org/10.1016/j.micromeso.2024.113160