Direct Observation of Macrostructure Formation of Hierarchically Structured Meso-Macroporous Aluminosilicates with 3D Interconnectivity by Optical Microscope

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Abstract

Hierarchically structured spongy meso-macroporous aluminosilicates with high tetrahedral aluminum content were synthesized from a mixture of single molecular
alkoxide precursor, (sec-BuO)2-Al-O-Si(OEt)3, already containing Si-O-Al bonds, and a silica coreactant, tetramethoxysilane (TMOS). The spontaneous byproduct templated
macroporous structure formation has been directly visualized using in situ high-resolution optical microscopy (OM), allowing the crucial observation of amicrobubble dispersionwhich
is directly correlated to the macrostructure observed by electronic microscopies (SEM and TEM). This discovery leads to a comparative study with meso-macroporous pure metal
oxide and to a proposal of the formationmechanism of meso-macroporous aluminosilicates with 3D interconnectivity. The aluminosilicate phase/microbubbles emulsion is produced by
a phase separation process occurring between the aluminosilicate nanoparticles and the liquid hydrolysis-condensation reaction byproducts (water, methanol, ethanol, and butanol). The
use of alkoxysilane improves the heterocondensation rates between the highly reactive aluminum alkoxide part of the single precursor and added silica species but, above all, leads to
the spontaneous generation of an unusual meso-macroporosity in alkaline media. The particles obtained at pH = 13.0 featured regular micrometer-sized macrospheres separated by very thin mesoporous walls and connected by submicrometric openings, providing a 3D
interconnectivity. The slight increase in pHvalue to 13.5 induced significantmodifications in morphology and textural properties due to the slower gelification process of the aluminosilicate phase, resulting in the formation of an aluminosilicate material constituted of 1-2 μm large
independent hollow mesoporous spheres.
Original languageEnglish
Pages (from-to)3030-3043
Number of pages14
JournalLangmuir
Volume27
DOIs
Publication statusPublished - 2011

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Aluminosilicates
optical microscopes
Microscopes
silicon dioxide
aluminum
thin walls
alkoxides
emulsions
hydrolysis
proposals
micrometers
hollow
ethyl alcohol
methyl alcohol
condensation
microscopy
Aluminum
Silicon Dioxide
nanoparticles
transmission electron microscopy

Cite this

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title = "Direct Observation of Macrostructure Formation of Hierarchically Structured Meso-Macroporous Aluminosilicates with 3D Interconnectivity by Optical Microscope",
abstract = "Hierarchically structured spongy meso-macroporous aluminosilicates with high tetrahedral aluminum content were synthesized from a mixture of single molecularalkoxide precursor, (sec-BuO)2-Al-O-Si(OEt)3, already containing Si-O-Al bonds, and a silica coreactant, tetramethoxysilane (TMOS). The spontaneous byproduct templatedmacroporous structure formation has been directly visualized using in situ high-resolution optical microscopy (OM), allowing the crucial observation of amicrobubble dispersionwhichis directly correlated to the macrostructure observed by electronic microscopies (SEM and TEM). This discovery leads to a comparative study with meso-macroporous pure metaloxide and to a proposal of the formationmechanism of meso-macroporous aluminosilicates with 3D interconnectivity. The aluminosilicate phase/microbubbles emulsion is produced bya phase separation process occurring between the aluminosilicate nanoparticles and the liquid hydrolysis-condensation reaction byproducts (water, methanol, ethanol, and butanol). Theuse of alkoxysilane improves the heterocondensation rates between the highly reactive aluminum alkoxide part of the single precursor and added silica species but, above all, leads tothe spontaneous generation of an unusual meso-macroporosity in alkaline media. The particles obtained at pH = 13.0 featured regular micrometer-sized macrospheres separated by very thin mesoporous walls and connected by submicrometric openings, providing a 3Dinterconnectivity. The slight increase in pHvalue to 13.5 induced significantmodifications in morphology and textural properties due to the slower gelification process of the aluminosilicate phase, resulting in the formation of an aluminosilicate material constituted of 1-2 μm largeindependent hollow mesoporous spheres.",
author = "Arnaud Lemaire and Joanna Rooke and Lihua Chen and Bao-Lian Su",
year = "2011",
doi = "10.1021/la104679h",
language = "English",
volume = "27",
pages = "3030--3043",
journal = "Langmuir",
issn = "0743-7463",
publisher = "American Chemical Society",

}

TY - JOUR

T1 - Direct Observation of Macrostructure Formation of Hierarchically Structured Meso-Macroporous Aluminosilicates with 3D Interconnectivity by Optical Microscope

AU - Lemaire, Arnaud

AU - Rooke, Joanna

AU - Chen, Lihua

AU - Su, Bao-Lian

PY - 2011

Y1 - 2011

N2 - Hierarchically structured spongy meso-macroporous aluminosilicates with high tetrahedral aluminum content were synthesized from a mixture of single molecularalkoxide precursor, (sec-BuO)2-Al-O-Si(OEt)3, already containing Si-O-Al bonds, and a silica coreactant, tetramethoxysilane (TMOS). The spontaneous byproduct templatedmacroporous structure formation has been directly visualized using in situ high-resolution optical microscopy (OM), allowing the crucial observation of amicrobubble dispersionwhichis directly correlated to the macrostructure observed by electronic microscopies (SEM and TEM). This discovery leads to a comparative study with meso-macroporous pure metaloxide and to a proposal of the formationmechanism of meso-macroporous aluminosilicates with 3D interconnectivity. The aluminosilicate phase/microbubbles emulsion is produced bya phase separation process occurring between the aluminosilicate nanoparticles and the liquid hydrolysis-condensation reaction byproducts (water, methanol, ethanol, and butanol). Theuse of alkoxysilane improves the heterocondensation rates between the highly reactive aluminum alkoxide part of the single precursor and added silica species but, above all, leads tothe spontaneous generation of an unusual meso-macroporosity in alkaline media. The particles obtained at pH = 13.0 featured regular micrometer-sized macrospheres separated by very thin mesoporous walls and connected by submicrometric openings, providing a 3Dinterconnectivity. The slight increase in pHvalue to 13.5 induced significantmodifications in morphology and textural properties due to the slower gelification process of the aluminosilicate phase, resulting in the formation of an aluminosilicate material constituted of 1-2 μm largeindependent hollow mesoporous spheres.

AB - Hierarchically structured spongy meso-macroporous aluminosilicates with high tetrahedral aluminum content were synthesized from a mixture of single molecularalkoxide precursor, (sec-BuO)2-Al-O-Si(OEt)3, already containing Si-O-Al bonds, and a silica coreactant, tetramethoxysilane (TMOS). The spontaneous byproduct templatedmacroporous structure formation has been directly visualized using in situ high-resolution optical microscopy (OM), allowing the crucial observation of amicrobubble dispersionwhichis directly correlated to the macrostructure observed by electronic microscopies (SEM and TEM). This discovery leads to a comparative study with meso-macroporous pure metaloxide and to a proposal of the formationmechanism of meso-macroporous aluminosilicates with 3D interconnectivity. The aluminosilicate phase/microbubbles emulsion is produced bya phase separation process occurring between the aluminosilicate nanoparticles and the liquid hydrolysis-condensation reaction byproducts (water, methanol, ethanol, and butanol). Theuse of alkoxysilane improves the heterocondensation rates between the highly reactive aluminum alkoxide part of the single precursor and added silica species but, above all, leads tothe spontaneous generation of an unusual meso-macroporosity in alkaline media. The particles obtained at pH = 13.0 featured regular micrometer-sized macrospheres separated by very thin mesoporous walls and connected by submicrometric openings, providing a 3Dinterconnectivity. The slight increase in pHvalue to 13.5 induced significantmodifications in morphology and textural properties due to the slower gelification process of the aluminosilicate phase, resulting in the formation of an aluminosilicate material constituted of 1-2 μm largeindependent hollow mesoporous spheres.

U2 - 10.1021/la104679h

DO - 10.1021/la104679h

M3 - Article

VL - 27

SP - 3030

EP - 3043

JO - Langmuir

JF - Langmuir

SN - 0743-7463

ER -