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Synthesis and Characterisation of Hierarchically Structured Titanium Silicalite-1 Zeolites with Large Intracrystalline Macropores

Weissenberger, Tobias ; Leonhardt, Rainer ; Zubiri, Benjamin Apeleo ; Pitínová-Štekrová, Martina ; Sheppard, Thomas L. ; Reiprich, Bastian ; Bauer, Jürgen ; Dotzel, Ralf ; Kahnt, Maik LU orcid and Schropp, Andreas , et al. (2019) In Chemistry - A European Journal
Abstract

The successful synthesis of hierarchically structured titanium silicalite-1 (TS-1) with large intracrystalline macropores by steam-assisted crystallisation of mesoporous silica particles is reported. The macropore topology was imaged in 3D by using electron tomography and synchrotron radiation-based ptychographic X-ray computed tomography, revealing interconnected macropores within the crystals accounting for about 30 % of the particle volume. The study of the macropore formation mechanism revealed that the mesoporous silica particles act as a sacrificial macropore template during the synthesis. Silicon-to-titanium ratio of the macroporous TS-1 samples was successfully tuned from 100 to 44. The hierarchically structured TS-1 exhibited... (More)

The successful synthesis of hierarchically structured titanium silicalite-1 (TS-1) with large intracrystalline macropores by steam-assisted crystallisation of mesoporous silica particles is reported. The macropore topology was imaged in 3D by using electron tomography and synchrotron radiation-based ptychographic X-ray computed tomography, revealing interconnected macropores within the crystals accounting for about 30 % of the particle volume. The study of the macropore formation mechanism revealed that the mesoporous silica particles act as a sacrificial macropore template during the synthesis. Silicon-to-titanium ratio of the macroporous TS-1 samples was successfully tuned from 100 to 44. The hierarchically structured TS-1 exhibited high activity in the liquid phase epoxidation of 2-octene with hydrogen peroxide. The hierarchically structured TS-1 surpassed a conventional nano-sized TS-1 sample in terms of alkene conversion and showed comparable selectivity to the epoxide. The flexible synthesis route described here can be used to prepare hierarchical zeolites with improved mass transport properties for other selective oxidation reactions.

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publishing date
type
Contribution to journal
publication status
published
keywords
catalysis, crystallization, epoxidation, nanostructures, zeolites
in
Chemistry - A European Journal
publisher
Wiley-Blackwell
external identifiers
  • pmid:31478582
  • scopus:85074102156
ISSN
0947-6539
DOI
10.1002/chem.201903287
language
English
LU publication?
no
id
6f1447c0-41f2-4e0e-a03b-7d8ca6e080a5
date added to LUP
2019-11-02 13:10:27
date last changed
2024-05-01 00:01:55
@article{6f1447c0-41f2-4e0e-a03b-7d8ca6e080a5,
  abstract     = {{<p>The successful synthesis of hierarchically structured titanium silicalite-1 (TS-1) with large intracrystalline macropores by steam-assisted crystallisation of mesoporous silica particles is reported. The macropore topology was imaged in 3D by using electron tomography and synchrotron radiation-based ptychographic X-ray computed tomography, revealing interconnected macropores within the crystals accounting for about 30 % of the particle volume. The study of the macropore formation mechanism revealed that the mesoporous silica particles act as a sacrificial macropore template during the synthesis. Silicon-to-titanium ratio of the macroporous TS-1 samples was successfully tuned from 100 to 44. The hierarchically structured TS-1 exhibited high activity in the liquid phase epoxidation of 2-octene with hydrogen peroxide. The hierarchically structured TS-1 surpassed a conventional nano-sized TS-1 sample in terms of alkene conversion and showed comparable selectivity to the epoxide. The flexible synthesis route described here can be used to prepare hierarchical zeolites with improved mass transport properties for other selective oxidation reactions.</p>}},
  author       = {{Weissenberger, Tobias and Leonhardt, Rainer and Zubiri, Benjamin Apeleo and Pitínová-Štekrová, Martina and Sheppard, Thomas L. and Reiprich, Bastian and Bauer, Jürgen and Dotzel, Ralf and Kahnt, Maik and Schropp, Andreas and Schroer, Christian G. and Grunwaldt, Jan Dierk and Casci, John L. and Čejka, Jiří and Spiecker, Erdmann and Schwieger, Wilhelm}},
  issn         = {{0947-6539}},
  keywords     = {{catalysis; crystallization; epoxidation; nanostructures; zeolites}},
  language     = {{eng}},
  month        = {{01}},
  publisher    = {{Wiley-Blackwell}},
  series       = {{Chemistry - A European Journal}},
  title        = {{Synthesis and Characterisation of Hierarchically Structured Titanium Silicalite-1 Zeolites with Large Intracrystalline Macropores}},
  url          = {{http://dx.doi.org/10.1002/chem.201903287}},
  doi          = {{10.1002/chem.201903287}},
  year         = {{2019}},
}