Methodology for Synthesizing Crystalline Metallosilicates with Expanded Pore Windows Through Molecular Alkoxysilylation of Zeolitic Lamellar Precursors
Abstract
Postalkoxysilylation with diethoxydimethylsilane has been carried out on the zeolitic lamellar precursors of various topologies such as MWW, FER, CDO and MCM-47 aiming to construct new crystalline structures with expanded pore apertures between the layers. The silylation process and the crystalline and pore structures of the resulting materials have been investigated with the techniques of XRD, IR, (13)C and (29)Si MAS NMR, ICP, SEM, HRTEM, elemental analyses, and N 2 adsorption. In contrast to forming known three-dimensional zeolite structures after direct calcination of the lamellar precursors, the silylation led to new crystalline structures with opener pores, as evidenced by the shift of layer-related diffractions to the lower-angle region in XRD patterns and the enlarged interlayer pores found by HRTEM images. After optimizing the treatment conditions, particularly the amount of silane agent, a maximum and homogeneous silylation was realized, which guaranteed the phase purity in interlayer expanded zeolites. The expanded structures were well preserved after calcination at 823 K or reflux in water for 1 to 2 weeks, indicating a high thermal stability and also a hydrothermal stability. The interlayer expanded zeolites prepared from the metallosilicate precursors of MWW topology exhibited higher catalytic activities in the redox and solid acid-catalyzed reactions of bulky molecules than that of their counterparts with conventional MWW topology.
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New zeolites can be obtained by topotactic transformation in which labile atoms are removed by mild secondary treatments followed by condensation or pillarization of remaining zeolitic layers, providing new fully ordered microporous materials.
“On the other hand, new zeolites can be obtained by topotactic transformation in which some labile atoms are removed by mild secondary treatments followed by condensation or pillarization of the remaining zeolitic layers, providing new fully ordered microporous materials.72,103,124−126”
From Zeolites in Adsorption Processes: State of the Art and Future Prospects (2022) · cites this paper as [125]
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- Authors
- Wu, P., Ruan, J., Wang, L., Wu, L., Wang, Y., Liu, Y., Fan, W., He, M., Terasaki, O., & Tatsumi, T.
- Affiliations
- Tokyo Institute of Technology (JP)
- ORCID
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2008-06-04
- Volume
- 130
- Issue
- 26
- Pages
- 8178-8187
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2088558444
- Cited by
- 235
- References
- 0
- Citations by year
- 2026: 8 · 2025: 6 · 2024: 9 · 2023: 5 · 2022: 13 · 2021: 11 · 2020: 18 · 2019: 10 · 2018: 14 · 2017: 14 · 2016: 13 · 2015: 24 · 2014: 23 · 2013: 20 · 2012: 12
- FWCI
- 7.08
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- Topics
- Physical Sciences › Chemistry › Inorganic Chemistry › Zeolite Catalysis and Synthesis
- Physical Sciences › Materials Science › Materials Chemistry › Mesoporous Materials and Catalysis
- Physical Sciences › Materials Science › Biomaterials › Clay minerals and soil interactions
- Keywords
- metallosilicates, diethoxydimethylsilane, calcination stability, hydrothermal stability, heterogeneous acid catalysis, redox catalysis
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
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