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Formation of Diverse Mesophases Templated by a Diprotic Anionic Surfactant
Stockholm University, Faculty of Science, Department of Physical, Inorganic and Structural Chemistry. (Osamu Terasaki)
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Inorganic and Structural Chemistry.
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK), Inorganic and Structural Chemistry.
2008 (English)In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 14, no 36, 11423-11428 p.Article in journal (Refereed) Published
Abstract [en]

The synthesis system for mesophase formation, using the diprotic anionic surfactant N-myristoyl-l-glutamic acid (C14GluA) as the structuredirecting agent (SDA) and N-trimethoxylsilylpropyl-N,N,N-trimethylammonium chloride (TMAPS) as the co-structure-directing agent (CSDA), has been investigated and a full-scaled synthesis-field diagram is presented. In this system we have obtained mesophases including three-dimensional (3D) micellar cubic Fm-3m, Pm-3n, Fd-3m, micellar tetragonal P42/mnm, two-dimensional (2D) hexagonal p6mm and bicontinuous cubic Pn-3m, by varying the C14GluA/NaOH/TMAPS composition ratios. From the diagram it can be concluded that the mesophase formation is affected to a high degree by the organic/inorganicinterface curvature and the mesocage–mesocage electrostatic interaction. Bicontinuous cubic and 2D-hexagonalphases were found in the low organic/inorganic-interface curvature zones, whereas micellar cubic and tetragonal mesophases were found in the high organic/inorganic-interface curvature zones. Formation of cubic Fm-3m and tetragonal P42/mnm was favoured in highly alkaline zones with strong mesocage–mesocage interactions, and formation of cubic Pm-3n and Fd-3m was favoured with moderate mesocage–mesocage interactions in the less alkaline zones of the diagram.

Place, publisher, year, edition, pages
Weinheim: Wiley-VCH Verlag GmbH&Co. KGaA , 2008. Vol. 14, no 36, 11423-11428 p.
Keyword [en]
formation mechanism, mesophases, mesoporous materials, surfactants, synthesis-field diagram
National Category
Chemical Sciences
Research subject
Materials Science
Identifiers
URN: urn:nbn:se:su:diva-29615DOI: 10.1002/chem.200800766ISI: 000262002900021OAI: oai:DiVA.org:su-29615DiVA: diva2:234475
Available from: 2009-09-09 Created: 2009-09-08 Last updated: 2017-12-13Bibliographically approved
In thesis
1. Formation mechanism of anionic-surfactant-templated mesoporous silica (AMS)
Open this publication in new window or tab >>Formation mechanism of anionic-surfactant-templated mesoporous silica (AMS)
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This dissertation is focused on synthesis, characterization and formation mechanism of anionic-surfactant-templated mesoporous silica (AMS).

Structural control mechanisms of AMS are investigated. First, different ionization degree of anionic surfactant affected by the acidity or alkalinity of the synthesis system gives rise to different charging density of micelles and therefore determines the organic/inorganic interface curvature, producing mesophases from cage-type to cylindrical, bicontinuous and lamellar. Second, mesocage/mesocage electrostatic repulsive interaction affects the formation of cage-type mesostructure, which is derived from a full-scaled synthesis-field diagram of AMS. The mesocage/mesocage interaction changes with charge density of mesocages and gives rise to their different packing manners. Third, the structural properties of AMS materials could be tuned by molecular features of surfactant and co-structure-directing agent (CSDA).

The pore size of AMS is found to be controlled by alkyl chain length, ionization degree of surfactant and the CSDA/surfactant ratio. Alkyl chain length of surfactant determines size of micelles and thus mesopores. Larger ionization degrees of anionic surfactant give rise to smaller pore sizes due to thermodynamic coiling of alkyl chains of surfactant. The hydrophobic interactions between the pendant organic groups of CSDA on the silica wall and the hydrophobic core of the micelles drive a contraction of the mesopores.

A mesoporous silica with novel bicontinuous cubic Pn-3m structure has been prepared using a diprotic anionic surfactant. 3d-reconstruction of the structure shows that it is bicontinuous composed of an enantiomeric pair of 3d mesoporous networks that are interwoven with each other, divided by a D surface. Inverse replication suggests the possible presence of ordered complimentary micropores in the material.

Place, publisher, year, edition, pages
Stockholm: Department of Physical, Inorganic and Structural Chemistry, Stockholm University, 2009. 75 p.
Keyword
mesoporous silica, anionic surfactant, formation mechanism, structural control
National Category
Other Basic Medicine
Research subject
Structural Chemistry
Identifiers
urn:nbn:se:su:diva-29628 (URN)978-91-7155-932-6 (ISBN)
Public defence
2009-10-06, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius vägen 16 B, Stockholm, 13:30 (English)
Opponent
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Available from: 2009-09-15 Created: 2009-09-08 Last updated: 2009-09-15Bibliographically approved

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