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pi-pi interaction of aromatic groups in amphiphilic molecules directing for single-crystalline mesostructured zeolite nanosheets
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Inorganic and Structural Chemistry.
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Number of Authors: 12
2014 (English)In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 5, 4262Article in journal (Refereed) Published
Abstract [en]

One of the challenges in material science has been to prepare macro-or mesoporous zeolite. Although examples of their synthesis exist, there is a need for a facile yet versatile approach to such hierarchical structures. Here we report a concept for designing a single quaternary ammonium head amphiphilic template with strong ordered self-assembling ability through pi-pi stacking in hydrophobic side, which stabilizes the mesostructure to form single-crystalline mesostructured zeolite nanosheets. The concept is demonstrated for the formation of a new type of MFI (zeolite framework code by International Zeolite Association) nanosheets joined with a 90 degrees rotational boundary, which results in a mesoporous zeolite with highly specific surface area even after calcination. Low binding energies for this self-assembling system are supported by a theoretical analysis. A geometrical matching between the arrangement of aromatic groups and the zeolitic framework is speculated for the formation of single-crystalline MFI nanosheets.

Place, publisher, year, edition, pages
2014. Vol. 5, 4262
National Category
Chemical Sciences
Research subject
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-106605DOI: 10.1038/ncomms5262ISI: 000338840800001OAI: oai:DiVA.org:su-106605DiVA: diva2:737635
Note

AuthorCount:12;

Available from: 2014-08-13 Created: 2014-08-12 Last updated: 2017-12-05Bibliographically approved
In thesis
1. Structural study of nano-structured materials: electron crystallography approaches
Open this publication in new window or tab >>Structural study of nano-structured materials: electron crystallography approaches
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The structural analysis serves as a bridge to link the structure of materials to their properties. Revealing the structure details allows a better understanding on the growth mechanisms and properties of materials, and a further designed synthesis of functional materials. The widely used methods based on X-ray diffraction have certain limitations for the structural analysis when crystals are small, poorly crystallized or contain many defects. As electrons interact strongly with matter and can be focused by electromagnetic lenses to form an image, electron crystallography (EC) approaches become prime candidates for the structural analysis of a wide range of materials that cannot be done using X-rays, particularly nanomaterials with poor crystallinity.

Three-dimensional electron diffraction tomography (3D EDT) is a recently developed method to automatically collect 3D electron diffraction data. By combining mechanical specimen tilt and electronic e-beam tilt, a large volume of reciprocal space can be swept at a fine step size to ensure the completeness and accuracy of the diffraction data with respect to both position and intensity. Effects of the dynamical scattering are enormously reduced as most of the patterns are collected at conditions off the zone axes. In this thesis, 3D EDT has been used for unit cell determination (COF-505), phase identifications and structure solutions (ZnO, Ba-Ta3N5, Zn-Sc, and V4O9), and the study of layer stacking faults (ETS-10 and SAPO-34 nanosheets).

High-resolution transmission electron microscope (HRTEM) imaging shows its particular advantages over diffraction by allowing observations of crystal structure projections and the 3D potential map reconstruction. HRTEM imaging has been used to visualize fine structures of different materials (hierarchical zeolites, ETS-10, and SAPO-34). Reconstructed 3D potential maps have been used to locate the positions of metal ions in a woven framework (COF-505) and elucidate the pore shape and connectivity in a silica mesoporous crystal.

The last part of this thesis explores the combination with X-ray crystallography to obtain more structure details.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm University, 2016. 101 p.
Keyword
structural analysis, electron crystallography, 3D EDT, HRTEM imaging, defects
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:su:diva-129233 (URN)978-91-7649-425-7 (ISBN)
Public defence
2016-06-08, Magnéli Hall, Arrhenius Laboratory, Svante arrhenius väg 16 B, Stockholm, 13:00 (English)
Opponent
Supervisors
Funder
Swedish Research Council, 1486801
Available from: 2016-05-16 Created: 2016-04-18 Last updated: 2017-02-23Bibliographically approved

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Ma, YanhangOleynikov, PeterTerasaki, Osamu
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